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Records |
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Author |
da Pieve, F.; Hogan, C.; Lamoen, D.; Verbeeck, J.; Vanmeert, F.; Radepont, M.; Cotte, M.; Janssens, K.; Gonze, X.; Van Tendeloo, G. |
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Title |
Casting light on the darkening of colors in historical paintings |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Physical review letters |
Abbreviated Journal |
Phys Rev Lett |
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Volume |
111 |
Issue |
20 |
Pages |
208302-208305 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The degradation of colors in historical paintings affects our cultural heritage in both museums and archeological sites. Despite intensive experimental studies, the origin of darkening of one of the most ancient pigments known to humankind, vermilion (α-HgS), remains unexplained. Here, by combining many-body theoretical spectroscopy and high-resolution microscopic x-ray diffraction, we clarify the composition of the damaged paint work and demonstrate possible physicochemical processes, induced by illumination and exposure to humidity and air, that cause photoactivation of the original pigment and the degradation of the secondary minerals. The results suggest a new path for the darkening process which was never considered by previous studies and prompt a critical examination of their findings. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
New York, N.Y. |
Editor |
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Language |
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Wos |
000327244500003 |
Publication Date |
2013-11-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0031-9007;1079-7114; |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.462 |
Times cited |
30 |
Open Access |
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Notes |
Vortex; ERC FP7; COUNTATOMS; ECASJO_; |
Approved |
Most recent IF: 8.462; 2013 IF: 7.728 |
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Call Number |
UA @ lucian @ c:irua:111396UA @ admin @ c:irua:111396 |
Serial |
287 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Miliani, C.; Brunetti, B.G.; Vagnini, M.; Vanmeert, F.; Falkenberg, G.; Abakumov, A.; Lu, Y.; Tian, H.; Verbeeck, J.; Radepont, M.; Cotte, M.; Hendriks, E.; Geldof, M.; van der Loeff, L.; Salvant, J.; Menu, M.; |
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Title |
Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of spectromicroscopic methods : 3 : synthesis, characterization, and detection of different crystal forms of the chrome yellow pigment |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
85 |
Issue |
2 |
Pages |
860-867 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The painter, Vincent van Gogh, and some of his contemporaries frequently made use of the pigment chrome yellow that is known to show a tendency toward darkening. This pigment may correspond to various chemical compounds such as PbCrO4 and PbCr1-xSxO4, that may each be present in various crystallographic forms with different tendencies toward degradation. Investigations by X-ray diffraction (XRD), mid-Fourier Transform infrared (FTIR), and Raman instruments (benchtop and portable) and synchrotron radiation-based micro-XRD and X-ray absorption near edge structure spectroscopy performed on oil-paint models, prepared with in-house synthesized PbCrO4 and PbCr1-xSxO4, permitted us to characterize the spectroscopic features of the various forms. On the basis of these results, an extended study has been carried out on historic paint tubes and on embedded paint microsamples taken from yellow-orange/pale yellow areas of 12 Van Gogh paintings, demonstrating that Van Gogh effectively made use of different chrome yellow types. This conclusion was also confirmed by in situ mid-FTIR investigations on Van Goghs Portrait of Gauguin (Van Gogh Museum, Amsterdam). |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000313668400031 |
Publication Date |
2012-10-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700;1520-6882; |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
79 |
Open Access |
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Notes |
Goa; Fwo |
Approved |
Most recent IF: 6.32; 2013 IF: 5.825 |
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Call Number |
UA @ lucian @ c:irua:108707UA @ admin @ c:irua:108707 |
Serial |
631 |
Permanent link to this record |
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Author |
Monico, L.; van der Snickt, G.; Janssens, K.; de Nolf, W.; Miliani, C.; Verbeeck, J.; Tian, H.; Tan, H.; Dik, J.; Radepont, M.; Cotte, M. |
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Title |
Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of synchrotron X-ray spectromicroscopy and related methods : 1 : artificially aged model samples |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
83 |
Issue |
4 |
Pages |
1214-1223 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
On several paintings by artists of the end of the 19th century and the beginning of the 20th Century a darkening of the original yellow areas, painted with the chrome yellow pigment (PbCrO4, PbCrO4·xPbSO4, or PbCrO4·xPbO) is observed. The most famous of these are the various Sunflowers paintings Vincent van Gogh made during his career. In the first part of this work, we attempt to elucidate the degradation process of chrome yellow by studying artificially aged model samples. In view of the very thin (1−3 μm) alteration layers that are formed, high lateral resolution spectroscopic methods such as microscopic X-ray absorption near edge (μ-XANES), X-ray fluorescence spectrometry (μ-XRF), and electron energy loss spectrometry (EELS) were employed. Some of these use synchrotron radiation (SR). Additionally, microscopic SR X-ray diffraction (SR μ-XRD), μ-Raman, and mid-FTIR spectroscopy were employed to completely characterize the samples. The formation of Cr(III) compounds at the surface of the chrome yellow paint layers is particularly observed in one aged model sample taken from a historic paint tube (ca. 1914). About two-thirds of the chromium that is present at the surface has reduced from the hexavalent to the trivalent state. The EELS and μ-XANES spectra are consistent with the presence of Cr2O3·2H2O (viridian). Moreover, as demonstrated by μ-XANES, the presence of another Cr(III) compound, such as either Cr2(SO4)3·H2O or (CH3CO2)7Cr3(OH)2 [chromium(III) acetate hydroxide], is likely. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000287176900011 |
Publication Date |
2011-02-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700;1520-6882; |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
113 |
Open Access |
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Notes |
Iuap; Fwo |
Approved |
Most recent IF: 6.32; 2011 IF: 5.856 |
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Call Number |
UA @ lucian @ c:irua:88794UA @ admin @ c:irua:88794 |
Serial |
632 |
Permanent link to this record |
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Author |
Cotte, M.; Genty-Vincent, A.; Janssens, K.; Susini, J. |
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Title |
Applications of synchrotron X-ray nano-probes in the field of cultural heritage |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Comptes rendus : physique |
Abbreviated Journal |
Cr Phys |
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Volume |
19 |
Issue |
7 |
Pages |
575-588 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Synchrotron-based techniques are increasingly used in the field of cultural heritage, and this review focuses notably on the application of nano-beams to access high-spatial-resolution information on fragments sampled in historical or model artworks. Depending on the targeted information, various nano-analytical techniques can be applied, providing both identification and localization of the various components. More precisely, nano-X-ray fluorescence probes elements, nano-X-ray diffraction identify crystalline phases, and nano X-ray absorption spectroscopy is sensitive to speciation. Furthermore, computed tomography-based techniques can provide useful information about the morphology and in particular the porosity of materials. (C) 2018 Academie des sciences. Published by Elsevier Masson SAS. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000451631400006 |
Publication Date |
2018-08-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1631-0705; 1878-1535 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.048 |
Times cited |
3 |
Open Access |
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Notes |
; ; |
Approved |
Most recent IF: 2.048 |
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Call Number |
UA @ admin @ c:irua:156320 |
Serial |
5476 |
Permanent link to this record |
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Author |
van der Snickt, G.; Dik, J.; Cotte, M.; Janssens, K.; Jaroszewicz, J.; de Nolf, W.; Groenewegen, J.; van der Loeff, L. |
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Title |
Characterization of a degraded cadmium yellow (CdS) pigment in an oil painting by means of synchrotron radiation based X-ray techniques |
Type |
A1 Journal article |
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Year |
2009 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
81 |
Issue |
7 |
Pages |
2600-2610 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
On several paintings of James Ensor (1860−1949), a gradual fading of originally bright yellow areas, painted with the pigment cadmium yellow (CdS), is observed. Additionally, in some areas exposed to light, the formation of small white-colored globules on top of the original paint surface is observed. In this paper the chemical transformation leading to the color change and to the formation of the globules is elucidated. Microscopic X-ray absorption near-edge spectroscopy (ì-XANES) experiments show that sulfur, originally present in sulfidic form (S2−), is oxidized during the transformation to the sulfate form (S6+). Upon formation (at or immediately below the surface), the highly soluble cadmium sulfate is assumed to be transported to the surface in solution and reprecipitates there, forming the whitish globules. The presence of cadmium sulfate (CdSO4·2H2O) and ammonium cadmium sulfate [(NH4)2Cd(SO4)2] at the surface is confirmed by microscopic X-ray diffraction measurements, where the latter salt is suspected to result from a secondary reaction of cadmium sulfate with ammonia. Measurements performed on cross sections reveal that the oxidation front has penetrated into the yellow paint down to ca. 1−2 ìm. The morphology and elemental distribution of the paint and degradation product were examined by means of scanning electron microscopy equipped with an energy-dispersive spectrometer (SEM-EDS) and synchrotron radiation based micro-X-ray fluorescence spectrometry (SR ì-XRF). In addition, ultraviolet-induced visible fluorescence photography (UIVFP) revealed itself to be a straightforward technique for documenting the occurrence of this specific kind of degradation on a macroscale by painting conservators. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000264759400025 |
Publication Date |
2009-03-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
91 |
Open Access |
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Notes |
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Approved |
Most recent IF: 6.32; 2009 IF: 5.214 |
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Call Number |
UA @ admin @ c:irua:76415 |
Serial |
5501 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Cotte, M.; Sorace, L.; Vanmeert, F.; Brunetti, B.G.; Miliani, C. |
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Title |
Chromium speciation methods and infrared spectroscopy for studying the chemical reactivity of lead chromate-based pigments in oil medium |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
Microchemical journal
T2 – TECHNART Conference, APR 27-30, 2015, Catania, ITALY |
Abbreviated Journal |
Microchem J |
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Volume |
124 |
Issue |
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Pages |
272-282 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Environmental factors, such as light, humidity and temperature are triggering agents for the alteration of organic and/or inorganic constituents of oil paintings. The oxidation of the organic material is favored by increasing of relative humidity and temperature, whereas processes involving changes of the oxidation states of a number of inorganic pigments (e.g., vermilion, cadmium yellows, zinc yellows, chrome yellows) are mainly activated by light-exposure. In view of the optimization of the long-term conservation and restoration strategies of paintings it is of relevant interest to establish the consequences of thermal parameters (temperature and relative humidity) on the chemical/photochemical-reactivity and the nature of the alteration products of light sensitive-pigments in oil medium. To this aim here we propose a multi-method analytical approach based on the combination of diffuse reflectance UV-Vis, FTIR, synchrotron radiation (SR)-based micro X-ray fluorescence (mu-XRF)/micro-X-ray absorption neat edge structure ()CANES) and electron paramagnetic resonance (EPR) spectroscopies for studying the effects of different relative humidity conditions before and after light exposure on the reactivity of a series of lead chromate-based pigments [such as PbCrO4 center dot PbO (monoclinic), PbCrO4 (monoclinic) and PbCr0.2S0.8O4 (orthorhombic)] in an oil medium. The investigation of paint models was also compared to that of a late 19th century historical orthorhombic PbCr0.4S0.6O4 oil paint. Diffuse reflectance UV-Vis and FTIR spectroscopies were used to obtain information associated with chromatic changes and the formation of organo-metal degradation products at the paint surface. SR-based Cr K-edge mu-XANES/mu-XRF mapping analysis and EPR spectroscopy were employed in a complementary fashion to determine the amount, nature and distribution of Cr(III) and Cr(V)-based alteration compounds within the paints with micrometric spatial resolution. Under the employed thermal aging conditions, lead(II)-carboxylates and reduced Cr-compounds (in abundance of up to about 35% at the surface) have been identified in the lead chromate-based paints. The tendency of chromates to become reduced increased with increasing moisture levels and was favored for the orthorhombic PbCr0.2S0.8O4 compounds. The redox process gave rise to the formation of Cr(V)-species in relative amount much higher than that was formed in the equivalent paint which was exposed only to light. After light-exposure of the thermally aged paints, compounds ascribable to the oxidation of the organic binder were detected for all the types of pigments. Nevertheless, the previous thermal treatment increased the tendency toward photo-reduction of only the PbCr0.2S0.8O4 pigment. For this light-sensitive compound, the thickness variation of the reduced Cr-rich (ca. 70%) photo-alteration layer with moisture levels could be ascribed to a surface passivation phenomenon that had already occurred before photochemical aging. (C) 2015 Elsevier B.V. All rights reserved. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000367755600042 |
Publication Date |
2015-09-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0026-265x; 0026-265x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.034 |
Times cited |
23 |
Open Access |
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Notes |
; ; |
Approved |
Most recent IF: 3.034 |
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Call Number |
UA @ admin @ c:irua:131099 |
Serial |
5519 |
Permanent link to this record |
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Author |
van der Snickt, G.; Janssens, K.; Dik, J.; de Nolf, W.; Vanmeert, F.; Jaroszewicz, J.; Cotte, M.; Falkenberg, G.; Van der Loeff, L. |
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Title |
Combined use of synchrotron radiation based micro-X-ray fluorescence, micro-X-ray diffraction, micro-X-ray absorption near-edge, and micro-fourier transform infrared spectroscopies for revealing an alternative degradation pathway of the pigment cadmium yellow in a painting by Van Gogh |
Type |
A1 Journal article |
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Year |
2012 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
84 |
Issue |
23 |
Pages |
10221-10228 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Over the past years a number of studies have described the instability of the pigment cadmium yellow (CdS). In a previous paper we have shown how cadmium sulfide on paintings by James Ensor oxidizes to CdSO4 center dot H2O. The degradation process gives rise to the fading of the bright yellow color and the formation of disfiguring white crystals that are present on the paint surface in approximately 50 mu m sized globular agglomerations. Here, we study cadmium yellow in the painting “Flowers in a blue vase” by Vincent van Gogh. This painting differs from the Ensor case in the fact that (a) a varnish was superimposed onto the degraded paint surface and (b) the CdS paint area is entirely covered with an opaque crust. The latter obscures the yellow color completely and thus presents a seemingly more advanced state of degradation. Analysis of a cross-sectioned and a crushed sample by combining scanning microscopic X-ray diffraction (mu-XRD), microscopic X-ray absorption near-edge spectroscopy (mu-XANES), microscopic X-ray fluorescence (mu-XRF) based chemical state mapping and scanning microscopic Fourier transform infrared (mu-FT-IR) spectrometry allowed unravelling the complex alteration pathway. Although no crystalline CdSO4 compounds were identified on the Van Gogh paint samples, we conclude that the observed degradation was initially caused by oxidation of the original CdS pigment, similar as for the previous Ensor case. However, due to the presence of an overlying varnish containing lead-based driers and oxalate ions, secondary reactions took place. In particular, it appears that upon the photoinduced oxidation of its sulfidic counterion, the Cd2+ ions reprecipitated at the paint/varnish interface after having formed a complex with oxalate ions that themselves are considered to be degradation products of the resin and/or oil in the varnish. The SO42- anions, for their part, found a suitable reaction partner in Pb2+ ions stemming from a dissolved lead-based siccative that was added to the varnish to promote its drying. The resulting opaque anglesite compound in the varnish, in combination with the underlying CdC2O4 layer at the paint/varnish interface, account for the orange-gray crust that is disfiguring the painting on a macroscopic level. In this way, the results presented in this paper demonstrate how, through a judicious combined use of several microanalytical methods with speciation capabilities, many new insights can be obtained from two minute, but highly complex and heterogeneous paint samples. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000311815300013 |
Publication Date |
2012-08-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
59 |
Open Access |
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Notes |
; This research was supported by BELSPO via the Interuniversity Attraction Poles Programme (IUAP VI/16) and the S2-ART project (SD/RI/04A) and funded by Grants from the ESRF (EC-442) and PETRA-III (I-20120312 EC). The text also presents results of GOA “XANES meets ELNES” (Research Fund University of Antwerp, Belgium) and from FWO (Brussels, Belgium) project nos. G.0103.04, G.0689.06, and G.0704.08. The staff of the Kroller-Muller Museum and painting conservators Margje Leeuwestein and Esther Van Duijn are acknowledged for this pleasant cooperation and the authorization for the publication of the images in this article. ; |
Approved |
Most recent IF: 6.32; 2012 IF: 5.695 |
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Call Number |
UA @ admin @ c:irua:105971 |
Serial |
5526 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Miliani, C.; van der Snickt, G.; Brunetti, B.G.; Guidi, M.C.; Radepont, M.; Cotte, M. |
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Title |
Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of spectromicroscopic methods : 4 : artificial aging of model samples of co-precipitates of lead chromate and lead sulfate |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
85 |
Issue |
2 |
Pages |
860-867 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Previous investigations about the darkening of chrome yellow pigments revealed that this form of alteration is attributable to a reduction of the original Cr(VI) to Cr(III), and that the presence of sulfur-containing compounds, most often sulfates, plays a key role during this process. We recently demonstrated that different crystal forms of chrome yellow pigments (PbCrO4 and PbCr1xSxO4) are present in paintings by Vincent van Gogh. In the present work, we show how both the chemical composition and the crystalline structure of lead chromate-based pigments influence their stability. For this purpose, oil model samples made with in-house synthesized powders of PbCrO4 and PbCr1xSxO4 were artificially aged and characterized. We observed a profound darkening only for those paint models made with PbCr1xSxO4, rich in SO42 (x ≥ 0.4), and orthorhombic phases (>30 wt %). Cr and S K-edge micro X-ray absorption near edge structure investigations revealed in an unequivocal manner the formation of up to about 60% of Cr(III)-species in the outer layer of the most altered samples; conversely, independent of the paint models chemical composition, no change in the S-oxidation state was observed. Analyses employing UVvisible diffuse reflectance and Fourier transform infrared spectroscopy were performed on unaged and aged model samples in order to obtain additional information on the physicochemical changes induced by the aging treatment. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000313668400032 |
Publication Date |
2012-10-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
49 |
Open Access |
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Notes |
; This research was supported by grants from ESRF (experiment EC-799), the Interuniversity Attraction Poles Programme-Belgian Science Policy (IUAP VI/16), and the BELSPO-SDD S2-ART (SD/RI/04) project. The text also presents results from GOA “XANES meets ELNES” (Research Fund University of Antwerp, Belgium) and FWO (Brussels, Belgium) projects G.0704.08 and G.01769.09. The EU FP7 programme CHARISMA (Grant Agreement 228330) and MIUR (PRIN08, Materiali e sistemi innovativi per la conservazione dell'arte contemporanea 2008 FFXXN9) are also acknowledged. ; |
Approved |
Most recent IF: 6.32; 2013 IF: 5.825 |
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Call Number |
UA @ admin @ c:irua:110471 |
Serial |
5569 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Vanmeert, F.; Cotte, M.; Brunetti, B.G.; van der Snickt, G.; Leeuwestein, M.; Plisson, J.S.; Menu, M.; Miliani, C. |
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Title |
Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of spectromicroscopic methods : part 5 : effects of nonoriginal surface coatings into the nature and distribution of chromium and sulfur species in chrome yellow paints |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
86 |
Issue |
21 |
Pages |
10804-10811 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The darkening of lead chromate yellow pigments, caused by a reduction of the chromate ions to Cr(III) compounds, is known to affect the appearance of several paintings by Vincent van Gogh. In previous papers of this series, we demonstrated that the darkening is activated by light and depends on the chemical composition and crystalline structure of the pigments. In this work, the results of Part 2 are extended and complemented with a new study aimed at deepening the knowledge of the nature and distribution of Cr and S species at the interface between the chrome yellow paint and the nonoriginal coating layer. For this purpose, three microsamples from two varnished paintings by Van Gogh and a waxed low relief by Gauguin (all originally uncoated) have been examined. Because nonoriginal coatings are often present in artwork by Van Gogh and contemporaries, the understanding of whether or not their application has influenced the morphological and/or physicochemical properties of the chrome yellow paint underneath is relevant in view of the conservation of these masterpieces. In all the samples studied, microscopic X-ray fluorescence (mu-XRF) and X-ray absorption near edge structure (mu-XANES) investigations showed that Cr(III)-based alteration products are present in the form of grains inside the coating (generally enriched of S species) and also homogeneously widespread at the paint surface. The distribution of Cr(III) species may be explained by the mechanical friction caused by the coating application by brush that picked up and redistributed the superficial Cr compounds, likely already present in the reduced state as result of the photodegradation process. The analysis of the XANES profiles allowed us to obtain new insights into the nature of the Cr(III) alteration products, that were identified as sulfate-, oxide-, organo-metal-, and chloride-based compounds. Building upon the knowledge acquired through the examination of original paint samples and from the investigation of aged model paints in the last Part 4 paper, in this study we aim to characterize a possible relation between the chemical composition of the coating and the chrome yellow degradation pathways by studying photochemically aged model samples covered with a dammar varnish contaminated with sulfide and sulfate salts. Cr speciation results did not show any evidence of the active role of the varnish and added S species on the reduction process of chrome yellows. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000344510200043 |
Publication Date |
2014-10-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
25 |
Open Access |
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|
Notes |
; This research was supported by the Italian projects PRIN (SICH) and PON (ITACHA). The text also presents results from Interuniversity Attraction Poles Programme Belgian Science Policy (S2-ART project S4DA), GOA “XANES meets ELNES” (Research Fund University of Antwerp, Belgium) and FWO (Brussels, Belgium) projects no. G.0704.08 and G.01769.09. ESRF is acknowledged for the grants received (experiments EC-799 and EC-1051). L.M. acknowledges the CNR for the financial support received in the framework of the Short Term Mobility Programme 2013. Thanks are expressed to Ella Hendriks (Van Gogh Museum, Amsterdam) and Muriel Geldof (Cultural Heritage Agency of The Netherlands) for selecting and sharing the information on the cross-section taken from Bank of the Seine. All the staff of the Van Gogh Museum, the Kroller-Muller Museum, and the Musee d'Orsay are acknowledged for the agreeable cooperation. ; |
Approved |
Most recent IF: 6.32; 2014 IF: 5.636 |
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Call Number |
UA @ admin @ c:irua:122100 |
Serial |
5570 |
Permanent link to this record |
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Author |
Monico, L.; van der Snickt, G.; Janssens, K.; de Nolf, W.; Miliani, C.; Dik, J.; Radepont, M.; Hendriks, E.; Geldof, M.; Cotte, M. |
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Title |
Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of synchrotron X-ray spectromicroscopy and related methods : 2 : original paint layer samples |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
83 |
Issue |
4 |
Pages |
1224-1231 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The darkening of the original yellow areas painted with the chrome yellow pigment (PbCrO4, PbCrO4·xPbSO4, or PbCrO4·xPbO) is a phenomenon widely observed on several paintings by Vincent van Gogh, such as the famous different versions of Sunflowers. During our previous investigations on artificially aged model samples of lead chromate, we established for the first time that darkening of chrome yellow is caused by reduction of PbCrO4 to Cr2O3·2H2O (viridian green), likely accompanied by the presence of another Cr(III) compound, such as either Cr2(SO4)3·H2O or (CH3CO2)7Cr3(OH)2 [chromium(III) acetate hydroxide]. In the second part of this work, in order to demonstrate that this reduction phenomenon effectively takes place in real paintings, we study original paint samples from two paintings of V. van Gogh. As with the model samples, in view of the thin superficial alteration layers that are present, high lateral resolution spectroscopic methods that make use of synchrotron radiation (SR), such as microscopic X-ray absorption near edge (μ-XANES) and X-ray fluorescence spectrometry (μ-XRF) were employed. Additionally, μ-Raman and mid-FTIR analyses were carried out to completely characterize the samples. On both paint microsamples, the local presence of reduced Cr was demonstrated by means of μ-XANES point measurements. The presence of Cr(III) was revealed in specific areas, in some cases correlated to the presence of Ba(sulfate) and/or to that of aluminum silicate compounds. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000287176900012 |
Publication Date |
2011-02-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.32 |
Times cited |
84 |
Open Access |
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|
Notes |
; This research was funded by grants from ESRF (experiment EC-504) and by HASYLAB (experiments 11-20080130 EC and 11-20070157 EC) and was supported by the Interuniversity Attraction Poles Programme-Belgian Science Policy (IUAP VI/16). The text also presents results of GOA “XANES meets ELNES” (Research Fund University of Antwerp, Belgium) and from FWO (Brussels, Belgium) project nos. G.0103.04, G.0689.06, and G.0704.08. The staff of the Van Gogh Museum, Amsterdam, is acknowledged for their agreeable cooperation and for the authorization to publish the images of the paintings in this article. L.M. was financially supported by the Erasmus Placement in the framework of Lifelong Learning Programme (A.Y. 2009-2010). The EU Community's FP7 Research Infrastructures program under the CHARISMA Project (Grant Agreement 228330) is also acknowledged. ; |
Approved |
Most recent IF: 6.32; 2011 IF: 5.856 |
|
Call Number |
UA @ admin @ c:irua:88795 |
Serial |
5571 |
Permanent link to this record |
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Author |
Monico, L.; Sorace, L.; Cotte, M.; de Nolf, W.; Janssens, K.; Romani, A.; Miliani, C. |
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Title |
Disclosing the binding medium effects and the pigment solubility in the (photo)reduction process of chrome yellows (PbCrO4/PbCr1-xSxO4) |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS Omega |
Abbreviated Journal |
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Volume |
4 |
Issue |
4 |
Pages |
6607-6619 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The darkening due to chemical alteration of chrome yellows (PbCrO4/PbCr1-xSxO4) is a phenomenon threatening a large number of 19th-20th century paintings, including the Amsterdam Sunflowers by Vincent van Gogh. Our earlier studies have proven that the alteration is due to a Cr(VI) -> Cr(III) reduction with Cr(V)-species that are formed as long-lived intermediates and that bCr(1-x)S(x)O(4) (0 < x <= 0.8) types undergo reduction more readily than monoclinic, S-free, PbCrO4. In this context, there is still lack of knowledge about the effects of the chemical properties of the binding medium (i.e., chemical composition and drying process) and the solubility of chrome yellows on the overall reduction pathways. Here, we study a series of naturally and photochemically aged mock-up paints prepared by mixing chrome yellow powders (PbCrO4/PbCr0.2S0.8O4) with either linseed oil or a water-based acrylic emulsion as the binding medium. Equivalent paints made up of the highly soluble K2CrO4 were also investigated and used as benchmarks to provide a more in-depth understanding of the influence of the solubility on the chromate reduction pathways in the two different binders. A combination of synchrotron radiation-based Cr K-edge X-ray absorption near edge structure (XANES), electron paramagnetic resonance (EPR), and UV-Visible spectroscopy measurements shows that: (1) the Cr(VI) reduction results from the interaction between the pigment and the binder; (2) the process is more significant in oil, giving rise to Cr(V)- and Cr(III)-species as well as oxidized organic compounds; (3) the lightfastness of the chrome yellow pigment is enhanced in the acrylic binder; and (4) the tendency toward chromium reduction increases with increasing solubility of the pigment. Based on our findings, we propose a scheme for the mechanism of the (photo)reduction process of chrome yellows in the oil and acrylic binder. Overall, our results provide new insights into the factors driving the degradation of lead chromate-based paints in artworks and contribute to the development of strategies for preserving them over time. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000466552500057 |
Publication Date |
2019-04-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2470-1343 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
4 |
Open Access |
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Notes |
; The research was financially supported by the European research project IPERION-CH, funded by the European Commission, H2020-INFRAIA-2014-2015 (grant agreement n. 654028), and by the project AMIS, within the program Dipartimenti di Eccellenza 2018-2022, funded by MIUR and University of Perugia. The University of Perugia is also acknowledged for financial support under the program “Ricerca di Base 2017”. L.S. acknowledges the financial support of Ente CRF. For the beamtime grants received, we thank the ESRF (experiment no. HG64 and in-house beamtimes). ; |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:160416 |
Serial |
5577 |
Permanent link to this record |
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Author |
Cagno, S.; Nuyts, G.; Bugani, S.; De Vis, K.; Schalm, O.; Caen, J.; Helfen, L.; Cotte, M.; Reischig, P.; Janssens, K. |
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Title |
Evaluation of manganese-bodies removal in historical stained glass windows via SR-\mu-XANES/XRF and SR-\mu-CT |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
26 |
Issue |
12 |
Pages |
2442-2451 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The speed and effectiveness of a conservation treatment used for stained glass windows have been investigated. Dark-coloured Mn-rich stains can be found in the alteration layer of ancient glass artefacts and cause the surface to turn brown/black: this phenomenon is known as Mn-browning or Mn-staining. While in glass manganese is present in the +II or +III oxidation states, in the Mn-rich bodies, manganese is in a higher oxidation state (+IV). In restoration practice, mildly reducing solutions are employed to eliminate the dark colour and restore the clear appearance of the glass. In this paper the effectiveness and side effects of the use of hydroxylamine hydrochloride for this purpose are assessed. Archaeological fragments of stained glass windows, dated to the 14th century and originating from Sidney Sussex College, Cambridge (UK), were examined by means of synchrotron radiation (SR) based microscopic X-ray Absorption Near-Edge Spectroscopy (μ-XANES) and microscopic X-Ray Fluorescence (μ-XRF) and with high resolution computed absorption tomography (μ-CT) before, during and after the treatment. The monitoring of the glass fragments during the treatment allows us to better understand the manner in which the process unfolds and its kinetics. The results obtained reveal that the hydroxylamine hydrochloride treatment is effective, but also that it has a number of unwanted side effects. These findings are useful for optimizing the time and other modalities of the Mn-reducing treatment as well as minimizing its unwanted results. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000297030400009 |
Publication Date |
2011-10-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.379 |
Times cited |
17 |
Open Access |
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Notes |
; This research was supported by the Interuniversity Attraction Poles Programme-Belgian Science Policy (IUAP VI/16). The text also presents results of GOA “XANES meets ELNES” (Research Fund University of Antwerp, Belgium) and from FWO (Brussels, Belgium) projects no. G.0704.08 and G.01769.09. Special thanks to Ms Leonie Seliger, head of the stained-glass conservation studio (The Cathedral Studios-The Chapter of Canterbury Cathedral) for the supply of the archaeological samples. The authors gratefully acknowledge ESRF for granting beamtime (proposal EC-602). ; |
Approved |
Most recent IF: 3.379; 2011 IF: 3.220 |
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Call Number |
UA @ admin @ c:irua:93848 |
Serial |
5613 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Hendriks, E.; Vanmeert, F.; van der Snickt, G.; Cotte, M.; Falkenberg, G.; Brunetti, B.G.; Miliani, C. |
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Title |
Evidence for degradation of the chrome yellows in Van Gogh's sunflowers : a study using noninvasive in situ methods and synchrotron-radiation-based x-ray techniques |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
54 |
Issue |
47 |
Pages |
13923-13927 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
This paper presents firm evidence for the chemical alteration of chrome yellow pigments in Van Gogh's Sunflowers (Van Gogh Museum, Amsterdam). Noninvasive in situ spectroscopic analysis at several spots on the painting, combined with synchrotron-radiation-based X-ray investigations of two microsamples, revealed the presence of different types of chrome yellow used by Van Gogh, including the lightfast PbCrO4 and the sulfur-rich PbCr1-xSxO4 (x approximate to 0.5) variety that is known for its high propensity to undergo photoinduced reduction. The products of this degradation process, i.e., Cr-III compounds, were found at the interface between the paint and the varnish. Selected locations of the painting with the highest risk of color modification by chemical deterioration of chrome yellow are identified, thus calling for careful monitoring in the future. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000367722500009 |
Publication Date |
2015-10-20 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.994 |
Times cited |
24 |
Open Access |
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Notes |
; We acknowledge financial support from the Italian MIUR project SICH-PRIN (2010329WPF_001) and BELSPO (Brussels) Project S2-ART (SD04A), GOA “SOLARPAINT” (Research Fund Antwerp University, BOF-2015), and FWO (Brussels) projects G.0C12.13, G.0704.08, G.01769.09. We thank ESRF (EC-1051, HG-26) and DESY (I-20120312 EC) for beamtime grants received. Noninvasive analysis of Sunflowers were supported by the EU FP7 programme CHARISMA (Grant 228330) and the Fund Inbev-Baillet Latour (Brussels). L.M. acknowledges financial support from the CNR Short Term Mobility Programme-2013. We thank Muriel Geldof, Luc Megens, Suzan de Groot (The Netherlands Cultural Heritage Agency, RCE), Chiara Grazia, David Buti (CNR-ISTM and SMAArt Centre), and the staff of the Van Gogh Museum for their collaboration. ; |
Approved |
Most recent IF: 11.994; 2015 IF: 11.261 |
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Call Number |
UA @ admin @ c:irua:131110 |
Serial |
5617 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Alfeld, M.; Cotte, M.; Vanmeert, F.; Ryan, C.G.; Falkenberg, G.; Howard, D.L.; Brunetti, B.G.; Miliani, C. |
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Title |
Full spectral XANES imaging using the Maia detector array as a new tool for the study of the alteration process of chrome yellow pigments in paintings by Vincent van Gogh |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
30 |
Issue |
3 |
Pages |
613-626 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
A combination of synchrotron radiation (SR) micro X-ray fluorescence (m-XRF) and XRF mode X-ray absorption near edge structure (XANES) measurements at the Cr K-edge already allowed us to establish that the photo-reduction of chromates to Cr(III) compounds is the cause of darkening of chrome yellow pigments (PbCr1-xSxO4, 0 <= x <= 0.8) in a number of paintings by Vincent van Gogh and in corresponding artificially aged paint models. A silicon drift detector (SDD) was employed to record the Cr-K XRF radiation in these X-ray micro beam-based measurements. However, in view of the limited count rate capabilities and collection solid angle of a single device, m-XRF and m-XANES employing single element SDDs (or similar) are primarily suited for collection of spectral data from individual points. Additionally, collection of XRF maps via point-by-point scanning with relatively long dwell times per point is possible but is usually confined to small areas. The development of the 384 silicon-diode array Maia XRF detector has provided valuable solutions in terms of data acquisition rate, allowing for full spectral (FS) XANES imaging in XRF mode, i.e., where spectroscopic information is available at each pixel in the scanned map. In this paper, the possibilities of SR Cr K-edge FS-XANES imaging in XRF mode using the Maia detector are examined as a new data collection strategy to study the speciation and distribution of alteration products of lead chromate-based pigments in painting materials. The results collected from two micro-samples taken from two Van Gogh paintings and an aged paint model show the possibility to perform FS-XANES imaging in practical time frames (from several minutes to a few hours) by scanning regions of sample sizes of the same order (more than 500 mm). The sensitivity and capabilities of FS-XANES imaging in providing representative chemical speciation information at the microscale (spatial resolution from similar to 2 to 0.6 mm) over the entire scanned area are demonstrated by the identification of Cr(OH) 3, Cr(III) sulfates and/or Cr(III) organometallic compounds in the corresponding phase maps, as alteration products. Comparable Cr-speciation results were obtained by performing equivalent higher spatial resolution SR m-XRF/single-point m-XANES analysis using a more conventional SDD from smaller regions of interest of each sample. Thus, large-area XRF mode FS-XANES imaging (Maia detector) is here proposed as a valuable and complementary data collection strategy in relation to “ zoomed-in” high-resolution m-XRF mapping and single-point m-XANES analysis (SDD). |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000350650800006 |
Publication Date |
2014-12-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.379 |
Times cited |
28 |
Open Access |
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Notes |
; This research was supported by the Interuniversity Attraction Poles Programme – Belgian Science Policy (S2-ART project S4DA), GOA “SOLARPAINT” (Research Fund University of Antwerp, Belgium) and FWO (Brussels, Belgium) project no. G.0C12.13, G.0704.08 and G.01769.09. Support from the Italian projects PRIN (SICH Sustainability in Cultural Heritage: from diagnosis to the development of innovative system for consolidation, cleaning and protection) and PON (ITACHA Italian advanced technologies for cultural heritage applications) is also acknowledged. For the grants received thanks are expressed to ESRF (experiments EC-799, EC-1051) and DESY (experiment H-20000043). Part of this research was undertaken at the XFM beamline at the Australian Synchrotron, Victoria, Australia (experiment M4604). LM acknowledges the CNR for the financial support received in the framework of the Short Term Mobility Programme 2013. Thanks are expressed to Ella Hendriks (Van Gogh Museum, Amsterdam), Muriel Geldof (Cultural Heritage Agency of The Netherlands) and Margje Leeuwestein (Kroller-Muller Museum, Otterlo) for selecting and sharing the information on the cross-section taken from the paintings The Bedroom and Falling Leaves (Les Alyscamps). All the staff of the Van Gogh Museum and the Kroller-Muller Museum are acknowledged for their agreeable cooperation. ; |
Approved |
Most recent IF: 3.379; 2015 IF: 3.466 |
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Call Number |
UA @ admin @ c:irua:125475 |
Serial |
5628 |
Permanent link to this record |
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Author |
Cotte, M.; Checroun, E.; De Nolf, W.; Taniguchi, Y.; De Viguerie, L.; Burghammer, M.; Walter, P.; Rivard, C.; Salome, M.; Janssens, K.; Susini, J. |
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Title |
Lead soaps in paintings : friends or foes? |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Studies in conservation |
Abbreviated Journal |
Stud Conserv |
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Volume |
62 |
Issue |
1 |
Pages |
2-23 |
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Keywords |
A1 Journal article; Art; History; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The origin(s) and role(s) of metal soaps in paints are a worldwide concern today. These hybrid compounds, containing both fatty acid chains and metals associated with a carboxylate function, are increasingly identified in paints. As reviewed in the first part of this work, the presence of metal soaps in paints is differently interpreted in scientific publications: metal soaps are sometimes considered to play a positive role as anchor points, during paint drying processes; they can also be considered as responsible for many degradation processes (protrusions, efflorescences, darkening, etc.). Their origins are also interpreted in various ways. In some paintings (in particular from the twentieth century), they have sometimes introduced on purpose, as additives, to modify the physical properties of the painting materials. In older paintings, metal soaps are usually thought to result from an uncontrolled reaction of oil with lead-based pigments, in particular lead white, red lead, and lead tin yellow. In the second part of this work, the review of historical recipes of lead-based paint shows an important number of recipes based on controlled mixing of oil with lead driers. In the third part, the experimental reproduction of such traditional recipes using walnut oil and litharge (PbO) shows that lead soaps can be formed, both in about one hour at approximate to 100 degrees C, or in about one month at room temperature. It shows as well that after a few years, litharge is no longer detected in the paint medium, while different lead carbonates are. Finally, the micro-infrared spectroscopy and micro-X-ray diffraction re-analysis of protrusions from a nine-year model painting shows together with lead soaps, the presence of Pb-5(CO3)(3)(OH)(2)O ('synthetic plumbonacrite'), an unusual phase recently observed in a protrusion from a painting by Vincent Van Gogh. This work highlights (i) the multiple origins and roles of metal soaps in paints and (ii) the importance of combining the analysis of fragments from historical paintings with the analysis and reproduction of historical recipes. In particular, we show that the components detected today in historical paintings may severely differ from those originally used or prepared by the painter, complicating the assessment of the painter's intentions. More than the presence of metal soaps, the key questions to be tackled should be about their origins and (re)mobilization. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000393691200002 |
Publication Date |
2016-10-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0039-3630; 2047-0584 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
0.578 |
Times cited |
26 |
Open Access |
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|
Notes |
; This work was supported by the European Synchrotron Radiation Facility. ; |
Approved |
Most recent IF: 0.578 |
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Call Number |
UA @ admin @ c:irua:141976 |
Serial |
5690 |
Permanent link to this record |
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Author |
Janssens, K.; Dik, J.; Cotte, M.; Susini, J. |
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Title |
Photon-based techniques for nondestructive subsurface analysis of painted cultural heritage artifacts |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Accounts of chemical research |
Abbreviated Journal |
Accounts Chem Res |
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Volume |
43 |
Issue |
6 |
Pages |
814-825 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Often, just micrometers below a paintings surface lies a wealth of information, both with Old Masters such as Peter Paul Rubens and Rembrandt van Rijn and with more recent artists of great renown such as Vincent Van Gogh and James Ensor. Subsurface layers may include underdrawing, underpainting, and alterations, and in a growing number of cases conservators have discovered abandoned compositions on paintings, illustrating artists practice of reusing a canvas or panel. The standard methods for studying the inner structure of cultural heritage (CH) artifacts are infrared reflectography and X-ray radiography, techniques that are optionally complemented with the microscopic analysis of cross-sectioned samples. These methods have limitations, but recently, a number of fundamentally new approaches for fully imaging the buildup of hidden paint layers and other complex three-dimensional (3D) substructures have been put into practice. In this Account, we discuss these developments and their recent practical application with CH artifacts. We begin with a tabular summary of 14 IR- and X-ray-based imaging methods and then continue with a discussion of each technique, illustrating CH applications with specific case studies. X-ray-based tomographic and laminographic techniques can be used to generate 3D renditions of artifacts of varying dimensions. These methods are proving invaluable for exploring inner structures, identifying the conservation state, and postulating the original manufacturing technology of metallic and other sculptures. In the analysis of paint layers, terahertz time-domain spectroscopy (THz-TDS) can highlight interfaces between layers in a stratigraphic buildup, whereas macrosopic scanning X-ray fluorescence (MA-XRF) has been employed to measure the distribution of pigments within these layers. This combination of innovative methods provides topographic and color information about the micrometer depth scale, allowing us to look into paintings in an entirely new manner. Over the past five years, several new variants of traditional IR- and X-ray-based imaging methods have been implemented by conservators and museums, and the first reports have begun to emerge in the primary research literature. Applying these state-of-the-art techniques in a complementary fashion affords a more comprehensive view of paintings and other artworks. |
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Place of Publication |
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Editor |
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Wos |
000278842500013 |
Publication Date |
2010-05-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0001-4842 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
20.268 |
Times cited |
78 |
Open Access |
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|
Notes |
; This research was supported by the Interuniversity Attraction Poles Programme-Belgian Science Policy (IUAP VI/16). The text also presents results of FWO (Brussels, Belgium) projects nr. G.0704.08 and G.0179.09 and from the UA-BOF GOA programme. ; |
Approved |
Most recent IF: 20.268; 2010 IF: 21.852 |
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Call Number |
UA @ admin @ c:irua:83983 |
Serial |
5772 |
Permanent link to this record |
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Author |
Monico, L.; Chieli, A.; De Meyer, S.; Cotte, M.; de Nolf, W.; Falkenberg, G.; Janssens, K.; Romani, A.; Miliani, C. |
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Title |
Role of the relative humidity and the Cd/Zn stoichiometry in the photooxidation process of cadmium yellows (CdS/Cd1-xZnxS) in oil paintings |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemistry: a European journal |
Abbreviated Journal |
Chem-Eur J |
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Volume |
24 |
Issue |
45 |
Pages |
11584-11593 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Cadmium yellows (CdYs) refer to a family of cadmium sulfide pigments, which have been widely used by artists since the late 19th century. Despite being considered stable, they are suffering from discoloration in iconic paintings, such as Joy of Life by Matisse, Flowers in a blue vase by Van Gogh, and The Scream by Munch, most likely due to the formation of CdSO4 center dot nH(2)O. The driving factors of the CdYs degradation and how these affect the overall process are still unknown. Here, we study a series of oil mock-up paints made of CdYs of different stoichiometry (CdS/Cd0.76Zn0.24S) and crystalline structure (hexagonal/ cubic) before and after aging at variable relative humidity under exposure to light and in darkness. Synchrotron radiation-based X-ray methods combined with UV-Vis and FTIR spectroscopy show that: 1) Cd0.76Zn0.24S is more susceptible to photooxidation than CdS; both compounds can act as photocatalysts for the oil oxidation. 2) The photooxidation of CdS/Cd0.76Zn0.24S to CdSO4 center dot nH(2)O is triggered by moisture. 3) The nature of alteration products depends on the aging conditions and the Cd/Zn stoichiometry. Based on our findings, we propose a scheme for the mechanism of the photocorrosion process and the photocatalytic activity of CdY pigments in the oil binder. Overall, our results form a reliable basis for understanding the degradation of CdS-based paints in artworks and contribute towards developing better ways of preserving them for future generations. |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000441126900012 |
Publication Date |
2018-06-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0947-6539 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.317 |
Times cited |
5 |
Open Access |
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Notes |
; The research was financially supported by the European research project IPERION-CH, funded by the European Commission, H2020-INFRAIA-2014-2015 (Grant agreement n. 654028) and by the BOF-GOA Project SOLARPaint (University of Antwerp Research Council). For the beamtime grants received, we thank the ESRF (experiments n. HG64, HG95 and in-house beamtimes) and PETRA III-DESY (experiments: I-20130221 EC, I-20160126 EC). We are also grateful to Dr. Jan Garrevoet for his contribution to set up the P06-beamline at PETRA III-DESY. ; |
Approved |
Most recent IF: 5.317 |
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Call Number |
UA @ admin @ c:irua:153733 |
Serial |
5821 |
Permanent link to this record |
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Author |
Nuyts, G.; Cagno, S.; Hellemans, K.; Veronesi, G.; Cotte, M.; Janssens, K. |
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Title |
Study of the early stages of Mn intrusion in corroded glass by means of combined SR FTIR/\muXRF imaging and XANES spectroscopy |
Type |
P1 Proceeding |
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Year |
2013 |
Publication |
Procedia Chemistry
T2 – Youth in Conservation of Cultural Heritage Conference (YOCOCU), June 18-20, 2012, University of Antwerp, Antwerp, Belgium |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
239-247 |
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Keywords |
P1 Proceeding; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Historical glass, especially medieval glass, can undergo weathering under the influence of time and environmental conditions. The aim of this investigation was to better understand the processes involved in this natural degradation process by studying artificially altered glass samples prepared for the use of evaluation of conservation methods. Non-durable glass sensors produced by the Fraunhofer Institute (type M1.0) were used as a starting material for artificial alteration. These were immersed in acidic (pH = 0, 2, 4) and neutral solutions (1 h – 8 h). In a second stage the glass samples were immersed in a 0.5 M MnCl2 solution (24 h, 48 h and 72 h), allowing intrusion of Mn from the solution into the gel layer. The samples were characterized at different stages with reflectance FTIR spectroscopy, mu XRF mapping and mu XANES. All measurements were carried out at ESRF, beamline ID21. Reflectance FTIR spectroscopy measurements were performed in the 800 4000 cm(-1) range. Cluster analysis of the resulting maps evidenced the rapid growth of the gel layer in strong acidic conditions. The average spectra for each cluster feature show for the original glass a strong Si-O- stretching band between 900 and 1000 cm(-1), whereas the gel layer could be identified by the increasing Si-O-Si bands around 1100 and 1250 cm(-1). mu XRF maps were recorded at different stages of the experiment at energies around the Mn-K edge (6.539 keV) and with a step size of 2 by 2 m. These confirm the leaching of K+ and Ca+2 from the glass and the intrusion of Mn from the solution. Mn was found throughout the entire gel layer, but with a concentration gradient peaking at the surface. XANES point measurements were recorded at various points where Mn was present. No spatial variation was found, but linear combination fitting of the spectra with various Mn reference compounds indicated that Mn2+Mn23+O4 is the main Mn compound in the gel layer, as was hypothesised by Watkinson et al. The standard corroded glass samples studied here can be used for the evaluation of conservation treatments in follow-up experiments. (C) 2013 The Authors. Published by Elsevier B.V. Selection and peer-review under responsibility of the IA-CS (Italian Association of Conservation Scientists) and University of Antwerp |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000321673900030 |
Publication Date |
2013-04-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
8 |
Series Issue |
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Edition |
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ISSN |
1876-6196 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
4 |
Open Access |
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Notes |
; This research was supported by the Interuniversity Attraction Poles Programme – Belgian Science Policy (IUAP VI/16). The text also presents results of GOA XANES “meets ELNES” (Research Fund University of Antwerp, Belgium) and from FWO (Brussels, Belgium) projects no. G.0704.08 and G.01769.09. We gratefully acknowledge ESRF for granting beamtime (experiment EC873). ; |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:109871 |
Serial |
5851 |
Permanent link to this record |
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Author |
Cotte, M.; Susini, J.; Dik, J.; Janssens, K. |
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Title |
Synchrotron-based X-ray absorption spectroscopy for art conservation: looking back and looking forward |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Accounts of chemical research |
Abbreviated Journal |
Accounts Chem Res |
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Volume |
43 |
Issue |
6 |
Pages |
705-714 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
A variety of analytical techniques augmented by the use of synchrotron radiation (SR), such as X-ray fluorescence (SR-XRF) and X-ray diffraction (SR-XRD), are now readily available, and they differ little, conceptually, from their common laboratory counterparts. Because of numerous advantages afforded by SR-based techniques over benchtop versions, however, SR methods have become popular with archaeologists, art historians, curators, and other researchers in the field of cultural heritage (CH). Although the CH community now commonly uses both SR-XRF and SR-XRD, the use of synchrotron-based X-ray absorption spectroscopy (SR-XAS) techniques remains marginal, mostly because CH specialists rarely interact with SR physicists. In this Account, we examine the basic principles and capabilities of XAS techniques in art preservation. XAS techniques offer a combination of features particularly well-suited for the chemical analysis of works of art. The methods are noninvasive, have low detection limits, afford high lateral resolution, and provide exceptional chemical sensitivity. These characteristics are highly desirable for the chemical characterization of precious, heterogeneous, and complex materials. In particular, the chemical mapping capability, with high spatial resolution that provides information about local composition and chemical states, even for trace elements, is a unique asset. The chemistry involved in both the objects history (that is, during fabrication) and future (that is, during preservation and restoration treatments) can be addressed by XAS. On the one hand, many studies seek to explain optical effects occurring in historical glasses or ceramics by probing the molecular environment of relevant chromophores. Hence, XAS can provide insight into craft skills that were mastered years, decades, or centuries ago but were lost over the course of time. On the other hand, XAS can also be used to characterize unwanted reactions, which are then considered alteration phenomena and can dramatically alter the objects original visual properties. In such cases, the bulk elemental composition is usually unchanged. Hence, monitoring oxidation state (or, more generally, other chemical modifications) can be of great importance. Recent applications of XAS in art conservation are reviewed and new trends are discussed, highlighting the value (and future possibilities) of XAS, which remains, given its potential, underutilized in the CH community. |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000278842500003 |
Publication Date |
2010-01-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0001-4842 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
20.268 |
Times cited |
74 |
Open Access |
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Notes |
; ; |
Approved |
Most recent IF: 20.268; 2010 IF: 21.852 |
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Call Number |
UA @ admin @ c:irua:83982 |
Serial |
5861 |
Permanent link to this record |
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Author |
Monico, L.; Janssens, K.; Cotte, M.; Romani, A.; Sorace, L.; Grazia, C.; Brunetti, B.G.; Miliani, C. |
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Title |
Synchrotron-based X-ray spectromicroscopy and electron paramagnetic resonance spectroscopy to investigate the redox properties of lead chromate pigments under the effect of visible light |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
30 |
Issue |
7 |
Pages |
1500-1510 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Light-induced redox processes have been established as the cause of the chromatic alterations of a number of artists' pigments used from the 15th to the 20th century. Despite the fact that a general comprehension of the mechanisms has been provided through the characterization of photo-degraded compounds, both exhaustive information on the wavelength-dependence of the alteration process of the pigments and experimental evidence in how visible light may influence the formation pathways of specific secondary compounds are still lacking. Establishing an analytical protocol for the study of wavelength-dependence of pigments on photo-redox pathways is relevant for the safe illumination of paintings, especially in view of the possible use of spectrally tunable light sources such as white light emitting diodes (WLEDs). In this work, we propose an integrated approach based on a combination of diffuse reflectance UV-visible, synchrotron radiation (SR)-based micro X-ray fluorescence (m-XRF)/X-ray absorption near edge structure (m-XANES) and electron paramagnetic resonance (EPR) spectroscopies to study the photo-redox process of Cr(VI) -> Cr(III) for lead chromate yellows (PbCr1-xSxO4, 0 <= x <= 0.8) under exposure to different monochromatic light. In view of the thin (3-5 mm) alteration layer that is formed at the paint surface after light exposure, SR-based Cr K-edge mu-XANES/mu-XRF analysis was employed to obtain information on the abundance, nature and distribution of the alteration of Cr(III)-compounds at the micrometricscale level. On the other hand, EPR spectroscopy was used as a complementary tool to the SR-based X-ray methods due to its sensitivity for revealing species containing one or more unpaired electrons and for distinguishing different coordination geometries of paramagnetic centers, such as Cr(V)-species. Semi-quantitative indications about the darkening of the paint surface were obtained by UV-Vis spectroscopy. An abundance of reduced Cr down to around 50% was detected at the aged surface of chrome yellow paints. The reduction process was favored not only by wavelengths shorter than 460 nm (i.e., where the pigment shows its maximum absorption) but also by light in the 490-530 nm range. The first evidence of the presence of Cr(V)-intermediates in the Cr(VI) -> Cr(III) reduction reaction allowed the risks of inducing photo-degradation of the 490-530 nm wavelength range to be explained. |
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Place of Publication |
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Editor |
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Wos |
000356971900004 |
Publication Date |
2015-04-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.379 |
Times cited |
17 |
Open Access |
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Notes |
; This research was supported by the Italian projects PRIN-(SICH) and PON- (ITACHA) and by Belgian Science Policy project S2-ART (BELSPO S4DA), the GOA “SOLARPAINT” (Research Fund Antwerp University, Belgium) and FWO (Brussels, Belgium) projects no. G.0C12.13, G.0704.08 and G.01769.09. ESRF is acknowledged for the grants received (experiments HG18 and HG26). L.S. and L.M. acknowledge the financial support of Ente-CRF and CNR-Short Term Mobility Programme 2013, respectively. ; |
Approved |
Most recent IF: 3.379; 2015 IF: 3.466 |
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Call Number |
UA @ admin @ c:irua:127059 |
Serial |
5862 |
Permanent link to this record |
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Author |
Cotte, M.; Pouyet, E.; Salome, M.; Rivard, C.; De Nolf, W.; Castillo-Michel, H.; Fabris, T.; Monico, L.; Janssens, K.; Wang, T.; Sciau, P.; Verger, L.; Cormier, L.; Dargaud, O.; Brun, E.; Bugnazet, D.; Fayard, B.; Hesse, B.; del Real, A.E.P.; Veronesi, G.; Langlois, J.; Balcar, N.; Vandenberghe, Y.; Sole, V.A.; Kieffer, J.; Barrett, R.; Cohen, C.; Cornu, C.; Baker, R.; Gagliardini, E.; Papillon, E.; Susini, J. |
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Title |
The ID21 X-ray and infrared microscopy beamline at the ESRF: status and recent applications to artistic materials |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
32 |
Issue |
3 |
Pages |
477-493 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The ID21 beamline (European Synchrotron Radiation facility, France) is a multi micro-analytical platform combining X-ray and infrared micro-probes, for characterization of elements, species, molecular groups and crystalline structures in complex materials. Applications are mainly in the fields of cultural heritage, life science, environmental and earth sciences, materials sciences. Here, we first present the status of instruments: (i) the scanning micro-spectroscopy end-station, operating from 2.0 to 9.2 keV, under vacuum and offering cryo conditions, for the acquisition of 2D micro X-ray fluorescence (mu XRF) maps, single point micro X-ray Absorption Near Edge Structure (mu XANES) spectra and speciation maps with sub-micrometric resolution; (ii) the XANES full-field end-station, operating in the same vacuum and energy conditions, for the acquisition of hyper-spectral radiographs of thin concentrated samples, resulting in speciation maps with micrometric resolution and millimetric field of view; (iii) the scanning micro-X-ray diffraction (mu XRD)/mu XRF end-station, operating at 8.5 keV, in air, for the acquisition of 2D crystalline phase maps, with micrometric resolution; and (iv) the scanning infrared microscope, operating in the mid-infrared range for the acquisition of molecular maps and some structural maps with micrometric resolution. Recent hardware and software developments are presented, as well as new protocols for improved sample preparation of thin sections. Secondly, a review of recent applications for the study of cultural heritage is presented, illustrated by various examples: determination of the origin of the color in blue Chinese porcelains and in brown Sevres porcelains; detection of lead in ink on Herculaneum papyri; identification and degradation of modeling materials used by Auguste Rodin and of chrome yellow pigments used by Vincent van Gogh. Cryo capabilities are illustrated by the analysis of plants exposed to chromate solutions. These examples show the variety of materials analyzed, of questions tackled, and particularly the multiple advantages of the ID21 analytical platform for the analysis of ancient and artistic materials. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000396286900002 |
Publication Date |
2016-12-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.379 |
Times cited |
39 |
Open Access |
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Notes |
; ; |
Approved |
Most recent IF: 3.379 |
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Call Number |
UA @ admin @ c:irua:142493 |
Serial |
5874 |
Permanent link to this record |
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Author |
Radepont, M.; Coquinot, Y.; Janssens, K.; Ezrati, J.-J.; de Nolf, W.; Cotte, M. |
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Title |
Thermodynamic and experimental study of the degradation of the red pigment mercury sulfide |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
30 |
Issue |
3 |
Pages |
599-612 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The red pigment mercury sulfide, called cinnabar or vermilion, is well known to suffer from an alteration giving rise to a grey, grey-white or black color at the surface of degraded works of art. This phenomenon can dramatically affect the esthetical value of artworks. This work aims at assessing the factors (light, halides) influencing the instability of red mercury sulfide and understanding (by combining thermodynamic and experimental approaches) the chemical equilibria governing the formation and evolution of the different degradation compounds. From the thermodynamic study of the Hg-S-Cl-H2O system, it was concluded that Hg(0), Hg3S2Cl2, and Hg2Cl2 can be formed from the reaction of alpha-HgS with ClO(g). In the second part, the artificial ageing experiments presented were carried out on model samples following the conditions assessed in the first part, in order to reproduce natural ageing observed on red mercury sulfide. Similarly to degradation compounds detected on original works of art, mercury chlorine compounds such as calomel (Hg2Cl2) and corderoite (alpha-Hg3S2Cl2) were identified on the surface of alpha-HgS model samples, when exposed to light and a sodium hypochlorite solution. Sulfates were detected as well, and more particularly gypsum (CaSO4 center dot 2H(2)O) when Ca was originally present in the model sample. The relationship between color and composition is discussed as well. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000350650800005 |
Publication Date |
2015-01-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
3.379 |
Times cited |
26 |
Open Access |
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Notes |
; The authors gratefully acknowledge the ESRF for granting beamtime under proposal no. EC720. Michel Dubus is thanked for providing precious advices concerning ageing protocols. This research was supported by Belgian Science Policy project S2-ART (BELSPO S4DA), the GOA “SOLARPAINT” (Research Fund University of Antwerp, Belgium) and FWO (Brussels, Belgium) projects no. G.0C12.13, G.0704.08 and G.01769.09. ; |
Approved |
Most recent IF: 3.379; 2015 IF: 3.466 |
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Call Number |
UA @ admin @ c:irua:125474 |
Serial |
5877 |
Permanent link to this record |
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Author |
Radepont, M.; de Nolf, W.; Janssens, K.; van der Snickt, G.; Coquinot, Y.; Klaassen, L.; Cotte, M. |
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Title |
The use of microscopic X-ray diffraction for the study of HgS and its degradation products corderoite (\alpha-Hg3S2Cl2), kenhsuite (\gamma-Hg3S2Cl2) and calomel (Hg2Cl2) in historical paintings |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
26 |
Issue |
5 |
Pages |
959-968 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Since antiquity, the red pigment mercury sulfide (α-HgS), called cinnabar in its natural form or vermilion red when synthetic, was very often used in frescoes and paintings, even if it was known to suffer occasionally from degradation. The paint hereby acquires a black or silver-grey aspect. The chemical characterization of these alteration products is rather challenging mainly because of the micrometric size and heterogeneity of the surface layers that develop and that are responsible for the color change. Methods such as electron microscopy, synchrotron-based microscopic X-ray fluorescence, microscopic X-ray absorption near edge spectroscopy, Raman microscopy and secondary ion microscopy have been previously employed to identify the (Hg- and S-) compounds present and to study their co-localization. Next to these, also microscopic X-ray diffraction (XRD) (either by making use of laboratory X-ray sources or when used at a synchrotron facility) allows the identification of the crystal phases that are present in degraded HgS paint layers. In this paper we employ these various forms of micro-XRD to analyze degraded red paint in different paintings and compare the results with other X-ray based methods. Whereas the elemental analyses of the degradation products revealed, next to mercury and sulfur, the presence of chlorine, X-ray diffraction allowed the identification, next to α-HgS, of the Hg and S-containing compound calomel (Hg2Cl2) but also of the Hg, S and Cl-containing minerals corderoite (α-Hg3S2Cl2) and kenhsuite (γ-Hg3S2Cl2). These observations are consistent with X-ray absorption spectroscopy measurements performed at the S- and Cl-edges. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000289731900011 |
Publication Date |
2011-03-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
3.379 |
Times cited |
40 |
Open Access |
|
|
Notes |
; The authors gratefully acknowledge GOA programme “XANES meets EELS'' (University of Antwerp Research Council), the IUAP VI/P16 programme ”Nacho'' (BELSPO, Brussels, Belgium) and FWO (Brussels, Belgium) projects no. G.0689.06, G.0704.08 and G017909N for financial support, the ESRF for granting beamtime under proposals no. EC442 and EC720, and Gema Martinez-Criado for practical help on ID18F. The KMSKA staff is also gratefully acknowledged for their help and interest. Javier Chillida is thanked for providing us with the Pedralbes samples. The authors are also indebted to the CHARISMA project (grant agreement 228330) for financial support. ; |
Approved |
Most recent IF: 3.379; 2011 IF: 3.220 |
|
Call Number |
UA @ admin @ c:irua:89927 |
Serial |
5896 |
Permanent link to this record |
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|
|
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Author |
Dik, J.; Janssens, K.; van der Snickt, G.; van der Loeff, L.; Rickers, K.; Cotte, M. |
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Title |
Visualization of a lost painting by Vincent van Gogh using synchrotron radiation based X-ray fluorescence elemental mapping |
Type |
A1 Journal article |
|
Year |
2008 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
|
Volume |
80 |
Issue |
16 |
Pages |
6436-6442 |
|
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
Abstract |
Vincent van Gogh (1853−1890), one of the founding fathers of modern painting, is best known for his vivid colors, his vibrant painting style, and his short but highly productive career. His productivity is even higher than generally realized, as many of his known paintings cover a previous composition. This is thought to be the case in one-third of his early period paintings. Van Gogh would often reuse the canvas of an abandoned painting and paint a new or modified composition on top. These hidden paintings offer a unique and intimate insight into the genesis of his works. Yet, current museum-based imaging tools are unable to properly visualize many of these hidden images. We present the first-time use of synchrotron radiation based X-ray fluorescence mapping, applied to visualize a womans head hidden under the work Patch of Grass by Van Gogh. We recorded decimeter-scale, X-ray fluorescence intensity maps, reflecting the distribution of specific elements in the paint layers. In doing so we succeeded in visualizing the hidden face with unprecedented detail. In particular, the distribution of Hg and Sb in the red and light tones, respectively, enabled an approximate color reconstruction of the flesh tones. This reconstruction proved to be the missing link for the comparison of the hidden face with Van Goghs known paintings. Our approach literally opens up new vistas in the nondestructive study of hidden paint layers, which applies to the oeuvre of Van Gogh in particular and to old master paintings in general. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000258448100039 |
Publication Date |
2008-07-29 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
|
ISSN |
0003-2700; 5206-882x |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
6.32 |
Times cited |
178 |
Open Access |
|
|
Notes |
|
Approved |
Most recent IF: 6.32; 2008 IF: 5.712 |
|
Call Number |
UA @ admin @ c:irua:74466 |
Serial |
5906 |
Permanent link to this record |
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|
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Author |
Gonzalez, V.; Cotte, M.; Vanmeert, F.; de Nolf, W.; Janssens, K. |
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Title |
X-ray diffraction mapping for cultural heritage science : a review of experimental configurations and applications |
Type |
A1 Journal article |
|
Year |
2019 |
Publication |
Chemistry: a European journal |
Abbreviated Journal |
Chem-Eur J |
|
Volume |
26 |
Issue |
26 |
Pages |
1703-1719 |
|
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
Abstract |
X-ray diffraction (XRD) mapping consists in the acquisition of XRD patterns at each pixel (or voxel) of an area (or volume). The spatial resolution ranges from the micrometer (mu XRD) to the millimeter (MA-XRD) scale, making the technique relevant for tiny samples up to large objects. Although XRD is primarily used for the identification of different materials in (complex) mixtures, additional information regarding the crystallite size, their orientation, and their in-depth distribution can also be obtained. Through mapping, these different types of information can be located on the studied sample/object. Cultural heritage objects are usually highly heterogeneous, and contain both original and later (degradation, conservation) materials. Their structural characterization is required both to determine ancient manufacturing processes and to evaluate their conservation state. Together with other mapping techniques, XRD mapping is increasingly used for these purposes. Here, the authors review applications as well as the various configurations for XRD mapping (synchrotron/laboratory X-ray source, poly-/monochromatic beam, micro/macro beam, 2D/3D, transmission/reflection mode). On-going hardware and software developments will further establish the technique as a key tool in heritage science. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000501927300001 |
Publication Date |
2019-10-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
ISSN |
0947-6539 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
5.317 |
Times cited |
|
Open Access |
|
|
Notes |
; M.C. thanks the KNAW for supporting her stays in the Netherlands through the Descartes Huygens price. V.G. and M.C. thank the Center of Research and Restoration of French Museums (C2RMF), Paris and in particular Myriam Eveno, for the collaboration on Rembrandt's impastos (Figure 7). M.C. is indebted to the Afghan government, NRICPT and in particular, Yoko Taniguchi for providing samples shown in Figure 5. K.J. and F.V. acknowledge the University of Antwerp Research Council for financial support via GOA project SolarPaint as well as InterReg project Smart*Light. FWO projects G057419N and G056619N are also acknowledged. The authors also wish to acknowledge the Van Gogh and Kroller-Muller museums, the Rijksmuseum, the Royal Museum of Fine Arts Antwerp and the Louvre museum for the constructive and inspiring collaborations in the past decade. Various beam lines and the staff at ESRF and DESY are thanked for providing beam time and support during experiments. ; |
Approved |
Most recent IF: 5.317 |
|
Call Number |
UA @ admin @ c:irua:165061 |
Serial |
5911 |
Permanent link to this record |
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|
|
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Author |
Pouyet, E.; Cotte, M.; Fayard, B.; Salome, M.; Meirer, F.; Mehta, A.; Uffelman, E.S.; Hull, A.; Vanmeert, F.; Kieffer, J.; Burghammer, M.; Janssens, K.; Sette, F.; Mass, J. |
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Title |
2D X-ray and FTIR micro-analysis of the degradation of cadmium yellow pigment in paintings of Henri Matisse |
Type |
A1 Journal article |
|
Year |
2015 |
Publication |
Applied physics A : materials science & processing |
Abbreviated Journal |
|
|
Volume |
121 |
Issue |
3 |
Pages |
967-980 |
|
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
Abstract |
The chemical and physical alterations of cadmium yellow (CdS) paints in Henri Matisse's The Joy of Life (1905-1906, The Barnes Foundation) have been recognized since 2006, when a survey by portable X-ray fluorescence identified this pigment in all altered regions of the monumental painting. This alteration is visible as fading, discoloration, chalking, flaking, and spalling of several regions of light to medium yellow paint. Since that time, synchrotron radiation-based techniques including elemental and spectroscopic imaging, as well as X-ray scattering have been employed to locate and identify the alteration products observed in this and related works by Henri Matisse. This information is necessary to formulate one or multiple mechanisms for degradation of Matisse's paints from this period, and thus ensure proper environmental conditions for the storage and the display of his works. This paper focuses on 2D full-field X-ray Near Edge Structure imaging, 2D micro-X-ray Diffraction, X-ray Fluorescence, and Fourier Transform Infra-red imaging of the altered paint layers to address one of the long-standing questions about cadmium yellow alteration-the roles of cadmium carbonates and cadmium sulphates found in the altered paint layers. These compounds have often been assumed to be photo-oxidation products, but could also be residual starting reagents from an indirect wet process synthesis of CdS. The data presented here allow identifying and mapping the location of cadmium carbonates, cadmium chlorides, cadmium oxalates, cadmium sulphates, and cadmium sulphides in thin sections of altered cadmium yellow paints from The Joy of Life and Matisse's Flower Piece (1906, The Barnes Foundation). Distribution of various cadmium compounds confirms that cadmium carbonates and sulphates are photo-degradation products in The Joy of Life, whereas in Flower Piece, cadmium carbonates appear to have been a [(partially) unreacted] starting reagent for the yellow paint, a role previously suggested in other altered yellow paints. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000364914100017 |
Publication Date |
2015-06-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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ISSN |
0947-8396; 1432-0630 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
|
|
Notes |
|
Approved |
no |
|
Call Number |
UA @ admin @ c:irua:130290 |
Serial |
7382 |
Permanent link to this record |
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Author |
Monico, L.; Cartechini, L.; Rosi, F.; Chieli, A.; Grazia, C.; De Meyer, S.; Nuyts, G.; Vanmeert, F.; Janssens, K.; Cotte, M.; De Nolf, W.; Falkenberg, G.; Sandu, I.C.A.; Tveit, E.S.; Mass, J.; De Freitas, R.P.; Romani, A.; Miliani, C. |
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Title |
Probing the chemistry of CdS paints in The Scream by in situ noninvasive spectroscopies and synchrotron radiation x-ray techniques |
Type |
A1 Journal article |
|
Year |
2020 |
Publication |
Science Advances |
Abbreviated Journal |
|
|
Volume |
6 |
Issue |
20 |
Pages |
eaay3514 |
|
Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
Abstract |
The degradation of cadmium sulfide (CdS)-based oil paints is a phenomenon potentially threatening the iconic painting The Scream (ca. 1910) by Edvard Munch (Munch Museum, Oslo) that is still poorly understood. Here, we provide evidence for the presence of cadmium sulfate and sulfites as alteration products of the original CdS-based paint and explore the external circumstances and internal factors causing this transformation. Macroscale in situ noninvasive spectroscopy studies of the painting in combination with synchrotron-radiation x-ray microspectroscopy investigations of a microsample and artificially aged mock-ups show that moisture and mobile chlorine compounds are key factors for promoting the oxidation of CdS, while light (photodegradation) plays a less important role. Furthermore, under exposure to humidity, parallel/secondary reactions involving dissolution, migration through the paint, and recrystallization of water-soluble phases of the paint are associated with the formation of cadmium sulfates. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000533573300009 |
Publication Date |
2020-05-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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ISSN |
2375-2548 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
13.6 |
Times cited |
4 |
Open Access |
|
|
Notes |
; The research was financially supported by the European research project IPERION-CH, funded by the European Commission, H2020-INFRAIA-2014-2015 (grant agreement no. 654028); the project AMIS, within the program Dipartimenti di Eccellenza 2018-2022 (funded by MIUR and University of Perugia); and the program “Ricerca di Base 2017” (funded by University of Perugia). S.D.M. and K.J. acknowledge the GOA Project SolarPaint from the University of Antwerp Research Council and projects G056619N and G054719N from FWO (Brussels). F.V. and K.J. acknowledge support from Interreg Project Smart*Light and thank BELSPO (Brussels) for financial support via FED-tWIN mandate PRF055. L.M. acknowledges the Erasmus+ program (Staff Mobility for training, A. Y. 2018 to 2019) of the European Commission. In situ noninvasive analyses were performed using the European MOLAB platform, which is financially supported by the European project IPERION-CH. For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiment nos. HG32, HG64, and HG95), DESY-P06 beamline, a member of the Helmholtz Association HGF (experiment nos. I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. ; |
Approved |
Most recent IF: 13.6; 2020 IF: NA |
|
Call Number |
UA @ admin @ c:irua:169519 |
Serial |
6585 |
Permanent link to this record |
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|
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Author |
Monico, L.; Prati, S.; Sciutto, G.; Catelli, E.; Romani, A.; Balbas, D.Q.; Li, Z.; De Meyer, S.; Nuyts, G.; Janssens, K.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Tardillo Suarez, V.I.; Tucoulou, R.; Mazzeo, R. |
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Title |
Development of a multi-method analytical approach based on the combination of synchrotron radiation X-ray micro-analytical techniques and vibrational micro-spectroscopy methods to unveil the causes and mechanism of darkening of “fake-gilded” decorations in a Cimabue painting |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
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Volume |
37 |
Issue |
1 |
Pages |
114-129 |
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Keywords |
A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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Abstract |
Redox processes activated by environmental factors have been identified as the main cause of the chromatic alterations of a number of artists' pigments, including the yellow pigment orpiment (As2S3). Although a general comprehension of the mechanisms has been provided through characterization of degradation compounds of As2S3, experimental evidences to prove how other paint components and how different environmental agents influence the formation pathways of specific secondary compounds are still lacking. Thus, it becomes fundamental to develop a methodological strategy which enable achieving a discrimination among the causes affecting the chemical stability of more heterogenous As2S3-based paints and defining the mechanism through which the alteration establishes and evolves, with the ultimate goal of optimizing the preventive conservation measures of unique masterpieces. In this paper, we propose a comprehensive multi-material and multi-method approach based on the combination of synchrotron radiation X-ray micro-analytical techniques (i.e., X-ray diffraction, X-ray fluorescence and X-ray absorption near edge structure spectroscopy at S K-/Ag L-3-/As K-edges) and vibrational micro-spectroscopy methods to unveil the causes and mechanism of darkening of “fake-gilded” decorations in tempera paintings, originally consisting of an unusual mixture of As2S3 and metallic silver (Ag-0). Such degradation process is a not yet understood phenomenon threatening a series of Old Master paintings, including those by the Italian painters Cimabue and Pietro Lorenzetti. The high specificity, sensitivity and lateral resolution of the employed analytical methods allowed providing first-time evidence for the presence of black acanthite (alpha-Ag2S), mimetite [Pb-5(AsO4)(3)Cl] and syngenite [K2Ca(SO4)(2)center dot H2O] as degradation products of the “fake-gilded” decorations in the Maesta by Cimabue (Church of Santa Maria dei Servi, Bologna, Italy). Furthermore, the study of the painting combined with that of tempera paint mock-ups permitted to explore and define the environmental agents and internal factors causing the darkening, by proving that: (i) Ag-0 and moisture are key-factors for triggering the transformation of As2S3 to alpha-Ag2S and As-oxides; (ii) S2--ions arising from the degradation of As2S3 are the main responsible for the formation of alpha-Ag2S; (iii) light exposure strengthens the tendency of the paint components towards alteration. Based on our findings, we finally propose a degradation mechanism of As2S3/Ag-0-based tempera paints. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000722353400001 |
Publication Date |
2021-11-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
ISSN |
0267-9477 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
3.4 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
|
Approved |
Most recent IF: 3.4 |
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Call Number |
UA @ admin @ c:irua:184871 |
Serial |
7142 |
Permanent link to this record |
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Author |
Cotte, M.; Gonzalez, V.; Vanmeert, F.; Monico, L.; Dejoie, C.; Burghammer, M.; Huder, L.; de Nolf, W.; Fisher, S.; Fazlic, I.; Chauffeton, C.; Wallez, G.; Jimenez, N.; Albert-Tortosa, F.; Salvado, N.; Possenti, E.; Colombo, C.; Ghirardello, M.; Comelli, D.; Avranovich Clerici, E.; Vivani, R.; Romani, A.; Costantino, C.; Janssens, K.; Taniguchi, Y.; McCarthy, J.; Reichert, H.; Susini, J. |
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Title |
The “Historical Materials BAG” : a new facilitated access to synchrotron X-ray diffraction analyses for cultural heritage materials at the European Synchrotron Radiation Facility |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
Molecules: a journal of synthetic chemistry and natural product chemistry |
Abbreviated Journal |
Molecules |
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Volume |
27 |
Issue |
6 |
Pages |
1997-21 |
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Keywords |
A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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Abstract |
The European Synchrotron Radiation Facility (ESRF) has recently commissioned the new Extremely Brilliant Source (EBS). The gain in brightness as well as the continuous development of beamline instruments boosts the beamline performances, in particular in terms of accelerated data acquisition. This has motivated the development of new access modes as an alternative to standard proposals for access to beamtime, in particular via the “block allocation group” (BAG) mode. Here, we present the recently implemented “historical materials BAG”: a community proposal giving to 10 European institutes the opportunity for guaranteed beamtime at two X-ray powder diffraction (XRPD) beamlines-ID13, for 2D high lateral resolution XRPD mapping, and ID22 for high angular resolution XRPD bulk analyses-with a particular focus on applications to cultural heritage. The capabilities offered by these instruments, the specific hardware and software developments to facilitate and speed-up data acquisition and data processing are detailed, and the first results from this new access are illustrated with recent applications to pigments, paintings, ceramics and wood. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000776369800001 |
Publication Date |
2022-03-21 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
|
ISSN |
1420-3049 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
4.6 |
Times cited |
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Open Access |
OpenAccess |
|
Notes |
|
Approved |
Most recent IF: 4.6 |
|
Call Number |
UA @ admin @ c:irua:188053 |
Serial |
7218 |
Permanent link to this record |
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Author |
Gonzalez, V.; Fazlic, I.; Cotte, M.; Vanmeert, F.; Gestels, A.; De Meyer, S.; Broers, F.; Hermans, J.; van Loon, A.; Janssens, K.; Noble, P.; Keune, K. |
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Title |
Lead(II) formate in Rembrandt's Night Watch : detection and distribution from the macro- to the micro-scale |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
|
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Volume |
|
Issue |
|
Pages |
1-9 |
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Keywords |
A1 Journal article; Art; Antwerp X-ray Imaging and Spectroscopy (AXIS) |
|
Abstract |
The Night Watch, painted in 1642 and on view in the Rijksmuseum in Amsterdam, is considered Rembrandt's most famous work. X-ray powder diffraction (XRPD) mapping at multiple length scales revealed the unusual presence of lead(II) formate, Pb(HCOO)(2), in several areas of the painting. Until now, this compound was never reported in historical oil paints. In order to get insights into this phenomenon, one possible chemical pathway was explored thanks to the preparation and micro-analysis of model oil paint media prepared by heating linseed oil and lead(II) oxide (PbO) drier as described in 17(th) century recipes. Synchrotron radiation based micro-XRPD (SR-mu-XRPD) and infrared microscopy were combined to identify and map at the micro-scale various neo-formed lead-based compounds in these model samples. Both lead(II) formate and lead(II) formate hydroxide Pb(HCOO)(OH) were detected and mapped, providing new clues regarding the reactivity of lead driers in oil matrices in historical paintings. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000920584500001 |
Publication Date |
2023-01-02 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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ISSN |
1433-7851; 0570-0833 |
ISBN ![sorted by ISBN field, ascending order (up)](img/sort_asc.gif) |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
Impact Factor |
16.6 |
Times cited |
|
Open Access |
OpenAccess |
|
Notes |
|
Approved |
Most recent IF: 16.6; 2023 IF: 11.994 |
|
Call Number |
UA @ admin @ c:irua:194279 |
Serial |
7318 |
Permanent link to this record |