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Author |
Bottari, F.; Daems, E.; de Vries, A.-M.; Van Wielendaele, P.; Trashin, S.; Blust, R.; Sobott, F.; Madder, A.; Martins, J.C.; De Wael, K. |
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Title |
Do aptamers always bind? The need for a multifaceted analytical approach when demonstrating binding affinity between aptamer and low molecular weight compounds |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Journal Of The American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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| |
Volume |
142 |
Issue |
46 |
Pages |
jacs.0c08691-19630 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Medical Biochemistry |
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Abstract |
In this manuscript, we compare different analytical methodologies to validate or disprove the binding capabilities of aptamer sequences. This was prompted by the lack of a universally accepted and robust quality control protocol for the characterization of aptamer performances coupled with the observation of independent yet inconsistent data sets in the literature. As an example, we chose three aptamers with a reported affinity in the nanomolar range for ampicillin, a β-lactam antibiotic, used as biorecognition elements in several detection strategies described in the literature. Application of a well-known colorimetric assay based on aggregation of gold nanoparticles (AuNPs) yielded conflicting results with respect to the original report. Therefore, ampicillin binding was evaluated in solution using isothermal titration calorimetry (ITC), native nano-electrospray ionization mass spectrometry (native nESI-MS), and 1H-nuclear magnetic resonance spectroscopy (1H NMR). By coupling the thermodynamic data obtained with ITC with the structural information on the binding event given by native nESI-MS and 1H NMR we could verify that none of the ampicillin aptamers show any specific binding with their intended target. The effect of AuNPs on the binding event was studied by both ITC and 1H NMR, again without providing positive evidence of ampicillin binding. To validate the performance of our analytical approach, we investigated two well-characterized aptamers for cocaine/quinine (MN4), chosen for its nanomolar range affinity, and l-argininamide (1OLD) to show the versatility of our approach. The results clearly indicate the need for a multifaceted analytical approach, to unequivocally establish the actual detection potential and performance of aptamers aimed at small organic molecules. |
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Wos |
000592911000024 |
Publication Date |
2020-11-09 |
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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 |
0002-7863 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor  |
15 |
Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: 15; 2020 IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:173136 |
Serial |
6488 |
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Author |
Marchetti, A.; Beltran, V.; Nuyts, G.; Borondics, F.; De Meyer, S.; Van Bos, M.; Jaroszewicz, J.; Otten, E.; Debulpaep, M.; De Wael, K. |
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Title |
Novel optical photothermal infrared (O-PTIR) spectroscopy for the noninvasive characterization of heritage glass-metal objects |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Science Advances |
Abbreviated Journal |
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Volume |
8 |
Issue |
9 |
Pages |
eabl6769-9 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab); Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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Abstract |
Optical photothermal infrared (O-PTIR) is a recently developed molecular spectroscopy technique that allows to noninvasively obtain chemical information on organic and inorganic samples at a submicrometric scale. The high spatial resolution (approximate to 450 nm), lack of sample preparation, and comparability of the spectral results to traditional Fourier transform infrared spectroscopy make it a promising candidate for the analysis of cultural heritage. In this work, the potential of O-PTIR for the noninvasive characterization of small heritage objects (few cubic centimeters) is demonstrated on a series of degraded 16th century brass and glass decorative elements. These small and challenging samples, typically encountering limitations with existing noninvasive methods such as macroscopic x-ray powder diffraction and mu Raman, were successfully characterized by O-PTIR, ultimately identifying the markers of glass-induced metal corrosion processes. The results clearly demonstrate how O-PTIR can be easily implemented in a noninvasive multianalytical strategy for the study of heritage materials, making it a fundamental tool for cultural heritage analyses. |
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Wos |
000790020300013 |
Publication Date |
2022-03-04 |
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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 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 13.6 |
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Call Number |
UA @ admin @ c:irua:188642 |
Serial |
7184 |
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Author |
Cánovas, R.; Daems, E.; Langley, A.R.; De Wael, K. |
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Title |
Are aptamer-based biosensing approaches a good choice for female fertility monitoring? A comprehensive review |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Biosensors and bioelectronics |
Abbreviated Journal |
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Volume |
220 |
Issue |
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Pages |
114881-18 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
The WHO estimates that 8–10% of couples are facing fertility problems, often due to inaccuracy in predicting the female's ovulation period controlled by four key hormones. The quantification and monitoring of such key hormones are crucial for the early identification of infertility, but also in improving therapeutic management associated with hormonal imbalance. In this review, we extensively summarize and discuss: i) drawbacks of laboratory methods for fertility testing (costly, invasive, complex) and commercially available point-of-care tests (measuring only one/two of the four key hormones), ii) the understanding of different biosensors for fertility monitoring, and iii) an in-depth classification and overview of aptamer-based sensing of the hormones of interest. This review provides insights on hormone detection strategies for fertility, with a focus on the classification of the current ‘aptasensing’ strategies, aiming to assist as a basic guide for the development of accurate fertility window monitoring tools based on aptamers. |
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Wos |
000890547600004 |
Publication Date |
2022-11-07 |
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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 |
0956-5663 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 12.6; 2023 IF: 7.78 |
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Call Number |
UA @ admin @ c:irua:191711 |
Serial |
8833 |
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Author |
Meysman, F.J.R.; Cornelissen, R.; Trashin, S.; Bonne, R.; Hidalgo-Martinez, S.; van der Veen, J.; Blom, C.J.; Karman, C.; Hou, J.-L.; Eachambadi, R.T.; Geelhoed, J.S.; De Wael, K.; Beaumont, H.J.E.; Cleuren, B.; Valcke, R.; van der Zant, H.S.J.; Boschker, H.T.S.; Manca, J.V. |
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Title |
A highly conductive fibre network enables centimetre-scale electron transport in multicellular cable bacteria |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
10 |
Issue |
10 |
Pages |
4120 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Biological electron transport is classically thought to occur over nanometre distances, yet recent studies suggest that electrical currents can run along centimetre-long cable bacteria. The phenomenon remains elusive, however, as currents have not been directly measured, nor have the conductive structures been identified. Here we demonstrate that cable bacteria conduct electrons over centimetre distances via highly conductive fibres embedded in the cell envelope. Direct electrode measurements reveal nanoampere currents in intact filaments up to 10.1 mm long (>2000 adjacent cells). A network of parallel periplasmic fibres displays a high conductivity (up to 79 S cm(-1)), explaining currents measured through intact filaments. Conductance rapidly declines upon exposure to air, but remains stable under vacuum, demonstrating that charge transfer is electronic rather than ionic. Our finding of a biological structure that efficiently guides electrical currents over long distances greatly expands the paradigm of biological charge transport and could enable new bio-electronic applications. |
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Wos |
000485216900006 |
Publication Date |
2019-09-11 |
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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 |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
10 |
Open Access |
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Notes |
; This research was financially supported by the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013) through ERC Grant 306933 (F.J.R.M.), the Research Foundation Flanders (FWO project grant G031416N), and the Netherlands Organisation for Scientific Research (VICI grant 016.VICI.170.072 to F.J.R.M.). H.J.E.B., C.J.B. and H.S.J.Z. were supported by the Netherlands Organisation for Scientific Research (NWO/OCW), as part of the Frontiers of Nanoscience program. R.B. is supported by an 'aspirant' grant from Research Foundation Flanders (FWO). We thank Laurine Burdorf (UAntwerpen) for help with Thiothrix cultivation, Marlies Nijemeisland (Faculty of Aerospace, TU Delft) for assistance with Raman microscopy, and Jan D'Haen (UHasselt) and Renaat Dasseville (UGent) for help with EM imaging. ; |
Approved |
Most recent IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:162795 |
Serial |
5451 |
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Author |
De Henau, S.; Tilleman, L.; Vangheel, M.; Luyckx, E.; Trashin, S.; Pauwels, M.; Germani, F.; Vlaeminck, C.; Vanfleteren, J.R.; Bert, W.; Pesce, A.; Nardini, M.; Bolognesi, M.; De Wael, K.; Moens, L.; Dewilde, S.; Braeckman, B.P. |
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Title |
A redox signalling globin is essential for reproduction in Caenorhabditis elegans |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
6 |
Issue |
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Pages |
8782 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Moderate levels of reactive oxygen species (ROS) are now recognized as redox signalling molecules. However, thus far, only mitochondria and NADPH oxidases have been identified as cellular sources of ROS in signalling. Here we identify a globin (GLB-12) that produces superoxide, a type of ROS, which serves as an essential signal for reproduction in C. elegans. We find that GLB-12 has an important role in the regulation of multiple aspects in germline development, including germ cell apoptosis. We further describe how GLB-12 displays specific molecular, biochemical and structural properties that allow this globin to act as a superoxide generator. In addition, both an intra- and extracellular superoxide dismutase act as key partners of GLB-12 to create a transmembrane redox signal. Our results show that a globin can function as a driving factor in redox signalling, and how this signal is regulated at the subcellular level by multiple control layers. |
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Corporate Author |
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Wos |
000367577100002 |
Publication Date |
2015-12-01 |
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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 |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
20 |
Open Access |
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Notes |
; We thank Dr K. Matsumoto and Dr T. Mizuno for kindly providing the mek-1(ks54) sek-1(km4) double mutant, the antibody anti-PMK-1 and technical advice on antibody use; Dr D. Kim for kindly providing the pDK177 RNAi strain; Dr M. Ubbink and Dr Q. Bashir for providing CCP; Dr K. Oegema and the OD lab for sharing technical expertise; M. Couvreur for assistance in generating transgenic lines; and Dr T. Dansen for the final support. Some strains were provided by the CGC, which is funded by the NIH Office of Research Infrastructure Programs (P40 OD010440). S.D.H. and F.G. are PhD fellows of the Fund for Scientific Research (FWO). Financial support to S.D. and L.M. was provided by the University of Antwerp (BOF UA TOP 2006), to K.D.W., S.D. and S.T. by the University of Antwerp (BOF-GOA) and to S.D., L.M., B.P.B., by FWO project G.0247.09. ; |
Approved |
Most recent IF: 12.124; 2015 IF: 11.470 |
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Call Number |
UA @ admin @ c:irua:129310 |
Serial |
5809 |
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Author |
Trashin, S.; Rahemi, V.; Ramji, K.; Neven, L.; Gorun, S.M.; De Wael, K. |
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Title |
Singlet oxygen-based electrosensing by molecular photosensitizers |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
8 |
Issue |
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Pages |
16108 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Enzyme-based electrochemical biosensors are an inspiration for the development of (bio)analytical techniques. However, the instability and reproducibility of the reactivity of enzymes, combined with the need for chemical reagents for sensing remain challenges for the construction of useful devices. Here we present a sensing strategy inspired by the advantages of enzymes and photoelectrochemical sensing, namely the integration of aerobic photocatalysis and electrochemical analysis. The photosensitizer, a bioinspired perfluorinated Zn phthalocyanine, generates singlet-oxygen from air under visible light illumination and oxidizes analytes, yielding electrochemically-detectable products while resisting the oxidizing species it produces. Compared with enzymatic detection methods, the proposed strategy uses air instead of internally added reactive reagents, features intrinsic baseline correction via on/off light switching and shows C-F bonds-type enhanced stability. It also affords selectivity imparted by the catalytic process and nano-level detection, such as 20 nM amoxicillin in μl sample volumes. |
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Place of Publication |
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Language |
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Wos |
000405466200002 |
Publication Date |
2017-07-14 |
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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 |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
26 |
Open Access |
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Notes |
; Evonik is thanked for providing samples of silicon and titanium oxides. Support from the National Science Foundation (SMG) for a portion of this work is gratefully acknowledged. FWO and UAntwerpen (BOF) are acknowledged for financial support. ; |
Approved |
Most recent IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:144538 |
Serial |
5833 |
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Author |
Parrilla, M.; De Wael, K. |
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Title |
Wearable self‐powered electrochemical devices for continuous health management |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Advanced Functional Materials |
Abbreviated Journal |
Adv Funct Mater |
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Volume |
31 |
Issue |
50 |
Pages |
2107042 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
The wearable revolution is already present in society through numerous gadgets. However, the contest remains in fully deployable wearable (bio)chemical sensing. Its use is constrained by the energy consumption which is provided by miniaturized batteries, limiting the autonomy of the device. Hence, the combination of materials and engineering efforts to develop sustainable energy management is paramount in the next generation of wearable self-powered electrochemical devices (WeSPEDs). In this direction, this review highlights for the first time the incorporation of innovative energy harvesting technologies with top-notch wearable self-powered sensors and low-powered electrochemical sensors toward battery-free and self-sustainable devices for health and wellbeing management. First, current elements such as wearable designs, electrochemical sensors, energy harvesters and storage, and user interfaces that conform WeSPEDs are depicted. Importantly, the bottlenecks in the development of WeSPEDs from an analytical perspective, product side, and power needs are carefully addressed. Subsequently, energy harvesting opportunities to power wearable electrochemical sensors are discussed. Finally, key findings that will enable the next generation of wearable devices are proposed. Overall, this review aims to bring new strategies for an energy-balanced deployment of WeSPEDs for successful monitoring of (bio)chemical parameters of the body toward personalized, predictive, and importantly, preventive healthcare. |
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Place of Publication |
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Wos |
000694642500001 |
Publication Date |
2021-09-09 |
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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 |
1616-301x |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:181306 |
Serial |
8750 |
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Author |
Anaf, W.; Janssens, K.; De Wael, K. |
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Title |
Formation of metallic mercury during photodegradation/photodarkening of \alpha-HgS : electrochemical evidence |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
52 |
Issue |
48 |
Pages |
12568-12571 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Das rote Pigment α-HgS neigt in Gegenwart von Licht und Chloridionen zur Schwärzung. Als Grund für die Zersetzung und Entfärbung werden die Bildung von (schwarzem) β-HgS oder Quecksilbermetall vermutet, doch diese Substanzen wurden noch nicht auf natürlich oder künstlich zersetzter HgS-Farbe nachgewiesen. Elektrochemische Experimente belegen nun die Bildung von Quecksilbermetall in Gegenwart von Licht und Chloridionen. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000327582900015 |
Publication Date |
2013-10-04 |
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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 |
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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 |
19 |
Open Access |
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Notes |
; The authors acknowledge L. Klaassen for valuable discussions and providing samples. We acknowledge financial support from the SDD programme (S2-ART project) of the Belgian Federal Goverment. ; |
Approved |
Most recent IF: 11.994; 2013 IF: 11.336 |
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Call Number |
UA @ admin @ c:irua:111265 |
Serial |
5626 |
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Author |
Beltran, V.; Marchetti, A.; Nuyts, G.; Leeuwestein, M.; Sandt, C.; Borondics, F.; De Wael, K. |
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Title |
Nanoscale analysis of historical paintings by means of O‐PTIR spectroscopy : the identification of the organic particles in L’Arlésienne (portrait of Madame Ginoux) by Van Gogh |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
60 |
Issue |
42 |
Pages |
22753-22760 |
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Keywords |
A1 Journal article; Art; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Optical-photothermal infrared (O-PTIR) spectroscopy is a recently developed technique that provides spectra comparable to traditional transmission FTIR spectroscopy with nanometric spatial resolution. Hence, O-PTIR is a promising candidate for the analysis of historical paintings, as well as other cultural heritage objects, but its potential has not yet been evaluated. |
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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 |
000694015700001 |
Publication Date |
2021-06-24 |
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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 |
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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 |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 11.994 |
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Call Number |
UA @ admin @ c:irua:179989 |
Serial |
8291 |
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Author |
Geerlings, N.M.J.; Karman, C.; Trashin, S.; As, K.S.; Kienhuis, M.V.M.; Hidalgo-Martinez, S.; Vasquez-Cardenas, D.; Boschker, H.T.S.; De Wael, K.; Middelburg, J.J.; Polerecky, L.; Meysman, F.J.R. |
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Title |
Division of labor and growth during electrical cooperation in multicellular cable bacteria |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Proceedings Of The National Academy Of Sciences Of The United States Of America |
Abbreviated Journal |
P Natl Acad Sci Usa |
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Volume |
117 |
Issue |
10 |
Pages |
5478-5485 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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| |
Abstract |
Multicellularity is a key evolutionary innovation, leading to coordinated activity and resource sharing among cells, which generally occurs via the physical exchange of chemical compounds. However, filamentous cable bacteria display a unique metabolism in which redox transformations in distant cells are coupled via long-distance electron transport rather than an exchange of chemicals. This challenges our understanding of organismal functioning, as the link among electron transfer, metabolism, energy conservation, and filament growth in cable bacteria remains enigmatic. Here, we show that cells within individual filaments of cable bacteria display a remarkable dichotomy in biosynthesis that coincides with redox zonation. Nanoscale secondary ion mass spectrometry combined with 13 C (bicarbonate and propionate) and 15 N-ammonia isotope labeling reveals that cells performing sulfide oxidation in deeper anoxic horizons have a high assimilation rate, whereas cells performing oxygen reduction in the oxic zone show very little or no label uptake. Accordingly, oxygen reduction appears to merely function as a mechanism to quickly dispense of electrons with little to no energy conservation, while biosynthesis and growth are restricted to sulfide-respiring cells. Still, cells can immediately switch roles when redox conditions change, and show no differentiation, which suggests that the “community service” performed by the cells in the oxic zone is only temporary. Overall, our data reveal a division of labor and electrical cooperation among cells that has not been seen previously in multicellular organisms. |
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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 |
|
Wos |
000519530400054 |
Publication Date |
2020-02-25 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0027-8424; 1091-6490 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
11.1 |
Times cited |
6 |
Open Access |
|
|
| |
Notes |
; We thank Arnold van Dijk for helping with the GasBench isotope ratio mass spectrometry analysis. N.M.J.G. is the recipient of a Ph.D. scholarship for teachers from the Netherlands Organisation for Scientific Research (NWO) in the Netherlands (grant 023.005.049). K.S.A. received financial support from the Olaf Schuiling fund. F.J.R.M. was financially supported by the Research Foundation Flanders (FWO) via grant G043119N, and the Netherlands Organization for Scientific Research (VICI grant 016.VICI.170.072). J.J.M. was supported by the Ministry of Education via the Netherlands Earth System Science Centre. The NanoSIMS facility was partly supported by an NWO large infrastructure subsidy to J.J.M. (175.010.2009.011). ; |
Approved |
Most recent IF: 11.1; 2020 IF: 9.661 |
|
| |
Call Number |
UA @ admin @ c:irua:166452 |
Serial |
6487 |
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| Permanent link to this record |
| |
|
| |
|
Author |
Zhang, T.; Schilling, W.; Khan, S.U.; Ching, H.Y.V.; Lu, C.; Chen, J.; Jaworski, A.; Barcaro, G.; Monti, S.; De Wael, K.; Slabon, A.; Das, S. |
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| |
Title |
Atomic-level understanding for the enhanced generation of hydrogen peroxide by the introduction of an aryl amino group in polymeric carbon nitrides |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
11 |
Issue |
22 |
Pages |
14087-14101 |
|
| |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Organic synthesis (ORSY); Applied Electrochemistry & Catalysis (ELCAT); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
|
| |
Abstract |
Heterogeneous catalysts are often & ldquo;black boxes & rdquo; due to the insufficient understanding of the detailed mechanisms at the catalytic sites. An atomic-level elucidation of the processes taking place in those regions is, thus, mandatory to produce robust and selective heterogeneous catalysts. We have improved the description of the whole reactive scenario for polymeric carbon nitrides (PCN) by combining atomic-level characterizations with magic-angle spinning (MAS) solid-state nuclear magnetic resonance (NMR) spectroscopy, classical reactive molecular dynamics (RMD) simulations, and quantum chemistry (QC) calculations. We disclose the structure & minus;property relationships of an ad hoc modified PCN by inserting an aryl amino group that turned out to be very efficient for the production of H2O2. The main advancement of this work is the development of a difluoromethylene-substituted aryl amino PCN to generate H2O2 at a rate of 2.0 mM & middot;h & minus;1 under the irradiation of household blue LEDs and the identification of possible active catalytic sites with the aid of 15N and 19F MAS solid-state NMR without using any expensive labeling reagent. RMD simulations and QC calculations confirm and further extend the experimental descriptions by revealing the role and locations of the identified functionalities, namely, NH linkers, & minus;NH2 terminal groups, and difluoromethylene units, reactants, and products. <comment>Superscript/Subscript Available</comment |
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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 |
|
Wos |
000758012900020 |
Publication Date |
2021-11-05 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10.614 |
Times cited |
|
Open Access |
Not_Open_Access |
|
| |
Notes |
|
Approved |
Most recent IF: 10.614 |
|
| |
Call Number |
UA @ admin @ c:irua:187276 |
Serial |
7534 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Van Hal, M.; Campos, R.; Lenaerts, S.; De Wael, K.; Verbruggen, S.W. |
|
| |
Title |
Gas phase photofuel cell consisting of WO₃- and TiO₂-photoanodes and an air-exposed cathode for simultaneous air purification and electricity generation |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Applied Catalysis B-Environmental |
Abbreviated Journal |
Appl Catal B-Environ |
|
| |
Volume |
292 |
Issue |
|
Pages |
120204 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Sustainable Energy, Air and Water Technology (DuEL) |
|
| |
Abstract |
Research has shown the potential of photofuel cells (PFCs) for waste water treatment, enabling the (partial) recovery of the energy released from the degraded compounds as electricity. Literature on PFCs targeting air pollution on the other hand is extremely scarce. In this work an autonomously operating air purification device targeting sustainable electricity generation is presented. Knowledge on gas phase operation of PFCs was gathered by combining photocatalytic and photoelectrochemical measurements, both for TiO2 and WO3-based photocatalysts. While TiO2-based photocatalysts performed better in direct photocatalytic experiments, they were outperformed by WO3-based photoanodes in all-gas-phase PFC operation. Not only do WO3-based photocatalysts generate the highest steady state photocurrent, they also achieved the highest fuel-to-electricity conversion (>65 %). The discrepancies between gas phase photocatalytic and photoelectrochemical processes highlight the difference in driving material properties. This study serves as a proof-of-concept towards development of an autonomous, low-cost and widely applicable waste gas-to-electricity PFC device. |
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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 |
|
Wos |
000663216500001 |
Publication Date |
2021-04-06 |
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| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0926-3373 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.446 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 9.446 |
|
| |
Call Number |
UA @ admin @ c:irua:177075 |
Serial |
7989 |
|
| Permanent link to this record |
| |
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| |
|
Author |
Teymourian, H.; Parrilla, M.; Sempionatto, J.R.; Montiel, N.F.; Barfidokht, A.; Van Echelpoel, R.; De Wael, K.; Wang, J. |
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| |
Title |
Wearable Electrochemical Sensors for the Monitoring and Screening of Drugs |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Sensors |
Abbreviated Journal |
Acs Sensors |
|
| |
Volume |
5 |
Issue |
9 |
Pages |
2679-2700 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
| |
Abstract |
Wearable electrochemical sensors capable of noninvasive monitoring of chemical markers represent a rapidly emerging digital-health technology. Recent advances toward wearable continuous glucose monitoring (CGM) systems have ignited tremendous interest in expanding such sensor technology to other important fields. This article reviews for the first time wearable electrochemical sensors for monitoring therapeutic drugs and drugs of abuse. This rapidly emerging class of drug-sensing wearable devices addresses the growing demand for personalized medicine, toward improved therapeutic outcomes while minimizing the side effects of drugs and the related medical expenses. Continuous, noninvasive monitoring of therapeutic drugs within bodily fluids empowers clinicians and patients to correlate the pharmacokinetic properties with optimal outcomes by realizing patient-specific dose regulation and tracking dynamic changes in pharmacokinetics behavior while assuring the medication adherence of patients. Furthermore, wearable electrochemical drug monitoring devices can also serve as powerful screening tools in the hands of law enforcement agents to combat drug trafficking and support on-site forensic investigations. The review covers various wearable form factors developed for noninvasive monitoring of therapeutic drugs in different body fluids and toward on-site screening of drugs of abuse. The future prospects of such wearable drug monitoring devices are presented with the ultimate goals of introducing accurate real-time drug monitoring protocols and autonomous closed-loop platforms toward precise dose regulation and optimal therapeutic outcomes. Finally, current unmet challenges and existing gaps are discussed for motivating future technological innovations regarding personalized therapy. The current pace of developments and the tremendous market opportunities for such wearable drug monitoring platforms are expected to drive intense future research and
commercialization efforts. |
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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 |
000573560800003 |
Publication Date |
2020-09-25 |
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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 |
2379-3694 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
8.9 |
Times cited |
|
Open Access |
|
|
| |
Notes |
Horizon 2020 Framework Programme, 833787 ; Center of Wearable Sensors, University of California San Diego; |
Approved |
Most recent IF: 8.9; 2020 IF: NA |
|
| |
Call Number |
AXES @ axes @c:irua:170894 |
Serial |
6436 |
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| Permanent link to this record |
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Author |
Blidar, A.; Trashin, S.; Carrion, E.N.; Gorun, S.M.; Cristea, C.; De Wael, K. |
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| |
Title |
Enhanced photoelectrochemical detection of an analyte triggered by its concentration by a singlet oxygen-generating fluoro photosensitizer |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Sensors |
Abbreviated Journal |
Acs Sensors |
|
| |
Volume |
5 |
Issue |
11 |
Pages |
3501-3509 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
| |
Abstract |
The use of a photocatalyst (photosensitizer) which produces singlet oxygen instead of enzymes for oxidizing analytes creates opportunities for designing cost-efficient and sensitive photoelectrochemical sensors. We report that perfluoroisopropyl-substituted zinc phthalocyanine (F64PcZn) interacts specifically with a complex phenolic compound, the antibiotic rifampicin (RIF), but not with hydroquinone or another complex phenolic compound, the antibiotic doxycycline. The specificity is imparted by the selective preconcentration of RIF in the photocatalytic layer, as revealed by electrochemical and optical measurements, complemented by molecular modeling that confirms the important role of a hydrophobic cavity formed by the iso-perfluoropropyl groups of the photocatalyst. The preconcentration effect favorably enhances the RIF photoelectrochemical detection limit as well as sensitivity to nanomolar (ppb) concentrations, LOD = 7 nM (6 ppb) and 2.8 A.M-1.cm(-2), respectively. The selectivity to RIF, retained in the photosensitizer layer, is further enhanced by the selective removal of all unretained phenols via simple washing of the electrodes with pure buffer. The utility of the sensor for analyzing municipal wastewater was demonstrated. This first demonstration of enhanced selectivity and sensitivity due to intrinsic interactions of a molecular photocatalyst (photosensitizer) with an analyte, without use of a biorecognition element, may allow the design of related, robust, simple, and viable sensors. |
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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 |
000595550100021 |
Publication Date |
2020-10-29 |
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| |
Series Editor |
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Series Title |
|
Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2379-3694 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
8.9 |
Times cited |
|
Open Access |
|
|
| |
Notes |
|
Approved |
Most recent IF: 8.9; 2020 IF: NA |
|
| |
Call Number |
UA @ admin @ c:irua:176057 |
Serial |
7913 |
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| Permanent link to this record |
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| |
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Author |
Parrilla, M.; Detamornrat, U.; Domínguez-Robles, J.; Tunca, S.; Donnelly, R.F.; De Wael, K. |
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| |
Title |
Wearable microneedle-based array patches for continuous electrochemical monitoring and drug delivery : toward a closed-loop system for methotrexate treatment |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS sensors |
Abbreviated Journal |
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| |
Volume |
|
Issue |
|
Pages |
acssensors.3c01381-10 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
|
| |
Abstract |
Wearable devices based on microneedle (MN) technology have recently emerged as tools for in situ transdermal sensing or delivery in interstitial fluid (ISF). Particularly, MN-based electrochemical sensors allow the continuous monitoring of analytes in a minimally invasive manner through ISF. Exogenous small molecules found in ISF such as therapeutic drugs are ideal candidates for MN sensors due to their correlation with blood levels and their relevance for the optimal management of personalized therapies. Herein, a hollow MN array patch is modified with conductive pastes and functionalized with cross-linked chitosan to develop an MN-based voltammetric sensor for continuous monitoring of methotrexate (MTX). Interestingly, the chitosan coating avoids biofouling while enabling the adsorption of MTX at the electrode’s surface for sensitive analysis. The MN sensor exhibits excellent analytical performance in vitro with protein-enriched artificial ISF and ex vivo under a Franz diffusion cell configuration. The MN sensor shows a linear range from 25 to 400 μM, which fits within the therapeutic range of high-dose MTX treatment for cancer patients and an excellent continuous operation for more than two days. Moreover, an iontophoretic hollow MN array patch is developed with the integration of both the anode and cathode in the single MN array patch. The ex vivo characterization demonstrates the transdermal on-demand drug delivery of MTX. Overall, the combination of both MN patches represents impactful progress in closed-loop systems for therapeutic drug management in disorders such as cancer, rheumatoid arthritis, or psoriasis. |
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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 |
|
Wos |
001109702900001 |
Publication Date |
2023-10-19 |
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| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2379-3694 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
|
| |
Impact Factor |
8.9 |
Times cited |
|
Open Access |
Not_Open_Access: Available from 19.04.2024 |
|
| |
Notes |
|
Approved |
Most recent IF: 8.9; 2023 IF: NA |
|
| |
Call Number |
UA @ admin @ c:irua:200074 |
Serial |
8956 |
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| Permanent link to this record |
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| |
|
Author |
De Jong, M.; Sleegers, N.; Kim, J.; Van Durme, F.; Samyn, N.; Wang, J.; De Wael, K. |
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| |
Title |
Electrochemical fingerprint of street samples for fast on-site screening of cocaine in seized drug powders |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemical science |
Abbreviated Journal |
Chem Sci |
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| |
Volume |
|
Issue |
|
Pages |
1-7 |
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| |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
|
| |
Abstract |
We report on a wearable fingertip sensor for on-the-spot identification of cocaine and its cutting agents in street samples. Traditionally, on-site screening is performed by means of colour tests which are difficult to interpret and lack selectivity. By presenting the distinct voltammetric response of cocaine, cutting agents, binary mixtures of cocaine and street samples in solution and powder street samples, we were able to elucidate the electrochemical fingerprint of all these compounds. The new electrochemical concept holds considerable promise as an on-site screening method. |
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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 |
|
Wos |
000371021900094 |
Publication Date |
2016-01-06 |
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| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2041-6520 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
8.668 |
Times cited |
37 |
Open Access |
|
|
| |
Notes |
; The authors acknowledge BELSPO for funding the APTADRU project (BR/314/PI/ APTADRU). ; |
Approved |
Most recent IF: 8.668 |
|
| |
Call Number |
UA @ admin @ c:irua:130404 |
Serial |
5591 |
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| Permanent link to this record |
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|
Author |
Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K. |
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| |
Title |
Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
32 |
Issue |
7 |
Pages |
2863-2873 |
|
| |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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| |
Abstract |
The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained. |
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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 |
000526394000016 |
Publication Date |
2020-04-14 |
|
| |
Series Editor |
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Series Title |
|
Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
8.6 |
Times cited |
8 |
Open Access |
OpenAccess |
|
| |
Notes |
Universiteit Antwerpen; Belgian Federal Science Policy Office; |
Approved |
Most recent IF: 8.6; 2020 IF: 9.466 |
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| |
Call Number |
EMAT @ emat @c:irua:168819 |
Serial |
6363 |
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| Permanent link to this record |
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Author |
Drăgan, A.-M.; Parrilla, M.; Feier, B.; Oprean, R.; Cristea, C.; De Wael, K. |
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Title |
Analytical techniques for the detection of amphetamine-type substances in different matrices : a comprehensive review |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Trac-Trends In Analytical Chemistry |
Abbreviated Journal |
Trac-Trend Anal Chem |
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| |
Volume |
145 |
Issue |
|
Pages |
116447 |
|
| |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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| |
Abstract |
This current review focuses on contributions to amphetamine-type substances (ATS) analysis. This type of synthetic illicit drugs has been increasingly present worldwide reaching 5% of the market on illicit drugs in 2019. The increment of their production in many clandestine laboratories and easy distribution among society are two of the main concerns towards the battle against synthetic drugs. Therefore, the first part of this review details the classification and mechanism of action of ATS in the human body. Second, the pharmacological and toxicological effects of ATS on human health are described to motivate the need of early detection of ATS. Subsequently, the most used laboratory-based and portable methods are presented and critically discussed along the review. Finally, a careful discussion on the advantages and disadvantages of portable techniques employed on the field are addressed as potential tools for on-site ATS detection by law enforcement officers. |
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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 |
|
Wos |
000723747000009 |
Publication Date |
2021-09-30 |
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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 |
0165-9936; 1879-3142 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
8.442 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 8.442 |
|
| |
Call Number |
UA @ admin @ c:irua:183268 |
Serial |
7460 |
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| Permanent link to this record |
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Author |
Daems, E.; Moro, G.; Campos, R.; De Wael, K. |
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Title |
Mapping the gaps in chemical analysis for the characterisation of aptamer-target interactions |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Trac-Trends In Analytical Chemistry |
Abbreviated Journal |
Trac-Trend Anal Chem |
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| |
Volume |
142 |
Issue |
|
Pages |
116311 |
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| |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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| |
Abstract |
Aptamers are promising biorecognition elements with a wide applicability from therapeutics to bio-sensing. However, to successfully use these biomolecules, a complete characterisation of their bindingperformance in the presence of the target is crucial. Several multi-analytical approaches have been re-ported including techniques to describe kinetic and thermodynamic aspects of the aptamer-targetinteraction, and techniques which allow an in-depth understanding of the aptamer-target structures.Recent literature shows the need of a critical data interpretation, a combination of characterisationtechniques and suggests the key role of the characterisation protocol design. Indeed, thefinal applicationof the aptamer should be considered before choosing the characterisation method. All the limitations andcapabilities of the analytical tools in use for aptamer characterisation should be taken into account. Here,we present a critical overview of the current methods and multi-analytical approaches to study aptamer-target binding, aiming to provide researchers with guidelines for the design of characterisation protocols. |
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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 |
000682179000010 |
Publication Date |
2021-04-28 |
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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 |
0165-9936; 1879-3142 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.442 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 8.442 |
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Call Number |
UA @ admin @ c:irua:179407 |
Serial |
8203 |
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| Permanent link to this record |
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Author |
Pilehvar, S.; Rather, J.A.; Dardenne, F.; Robbens, J.; Blust, R.; De Wael, K. |
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Title |
Carbon nanotubes based electrochemical aptasensing platform for the detection of hydroxylated polychlorinated biphenyl in human blood serum |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
Biosensors and bioelectronics |
Abbreviated Journal |
Biosens Bioelectron |
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| |
Volume |
54 |
Issue |
|
Pages |
78-84 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
A novel strategy to sense target molecules in human blood serum is achieved by immobilizing aptamers (APTs) on multiwalled carbon nanotubes (MWCNT) modified electrodes. In this work, the aminated aptamer selected for hydroxylated polychlorinated biphenyl (OHPCB) was covalently immobilized on the surface of the MWCNTCOOH modified glassy carbon electrode through amide linkage. The aptamers function as recognition probes for OHPCB by the binding induced folding of the aptamer. The developed aptasensing device was characterized by Electrochemical Impedance Spectroscopy (EIS), Atomic Force Microscopy (AFM) and Fourier Transform Infrared Spectroscopy (FTIR). The aptasensor displayed excellent performance for OHPCB detection with a linear range from 0.16 to 7.5 μM. The sensitivity of the developed aptasensing platform is improved (1×10−8 M) compared to the published report (1×10−6 M) for the determination of OH-PCB (Turner et al., 2007). The better performance of the sensor is due to the unique platform, i.e. the presence of APTs onto electrodes and the combination with nanomaterials. The aptamer density on the electrode surface was estimated by chronocoulometry and was found to be 1.4×1013 molecules cm−2. The validity of the method and applicability of the aptasensor was successfully evaluated by the detection of OHPCB in a blood serum sample. The described approach for aptasensing opens up new perspectives in the field of biomonitoring providing a device with acceptable stability, high sensitivity, good accuracy and precision. |
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Place of Publication |
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Wos |
000333071500012 |
Publication Date |
2013-11-01 |
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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 |
0956-5663 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.78 |
Times cited |
40 |
Open Access |
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Notes |
; We are thankful to UA-DOCPRO and BELSPO for financial support (respectively S. Pilehvar and J. Ahmad Rather). We also thank Prof. A. Covaci (UA) for the kind gift of human blood serum samples. Special thanks to Prof. L Van Vaeck and Y. Vercammen (UA) for AFM imaging and Prof. V. Meynen and M. Kus (LADCA, UA) for performing IR measurements. ; |
Approved |
Most recent IF: 7.78; 2014 IF: 6.409 |
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Call Number |
UA @ admin @ c:irua:111262 |
Serial |
5495 |
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| Permanent link to this record |
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Author |
Moro, G.; Bottari, F.; Van Loon, J.; Du Bois, E.; De Wael, K.; Moretto, L.M. |
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Title |
Disposable electrodes from waste materials and renewable sources for (bio) electroanalytical applications |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Biosensors and bioelectronics |
Abbreviated Journal |
Biosens Bioelectron |
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Volume |
146 |
Issue |
146 |
Pages |
111758 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Product development |
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Abstract |
The numerous advantages of disposable and screen-printed electrodes (SPEs) particularly in terms of portability, sensibility, sensitivity and low-cost led to the massive application of these electroanalytical devices. To limit the electronic waste and recover precious materials, new recycling processes were developed together with alternative SPEs fabrication procedures based on renewable, biocompatible sources or waste materials, such as paper, agricultural byproducts or spent batteries. The increased interest in the use of eco-friendly materials for electronics has given rise to a new generation of highly performing green modifiers. From paper based electrodes to disposable electrodes obtained from CD/DVD, in the last decades considerable efforts were devoted to reuse and recycle in the field of electrochemistry. Here an overview of recycled and recyclable disposable electrodes, sustainable electrode modifiers and alternative fabrication processes is proposed aiming to provide meaningful examples to redesign the world of disposable electrodes. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000497250600003 |
Publication Date |
2019-10-07 |
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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 |
0956-5663 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.78 |
Times cited |
2 |
Open Access |
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Notes |
; This research received funding from FWO and IOF (UAntwerpen). ; |
Approved |
Most recent IF: 7.78 |
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Call Number |
UA @ admin @ c:irua:164563 |
Serial |
5578 |
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| Permanent link to this record |
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Author |
Amiri-Aref, M.; Raoof, J.B.; Kiekens, F.; De Wael, K. |
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Title |
Mixed hemi/ad-micelles coated magnetic nanoparticles for the entrapment of hemoglobin at the surface of a screen-printed carbon electrode and its direct electrochemistry and electrocatalysis |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Biosensors and bioelectronics |
Abbreviated Journal |
Biosens Bioelectron |
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Volume |
74 |
Issue |
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Pages |
518-525 |
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Keywords |
A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
An efficient procedure for the physical entrapment of proteins within a biocompatible matrix and their immobilization on electrode surfaces is of utmost importance in the fabrication of biosensors. In this work, the magnetic entrapment of hemoglobin (Hb) at the surface of a screen-printed carbon electrode (SPCE), through mixed hemi/ad-micelles (MHAM) array of positively charged surfactant supported iron oxide magnetic nanoparticles (Mag-NPs), is reported. The Hb/MHAM@Mag-NPs biocomposite is captured at SPCE by a super magnet (Hb/MHAM@Mag-NPs/SPCE). To gain insight in the configuration of the mixed hemi/ad-micelles of CTAB at Mag-NPs, zeta-potential measurements were performed. The entrapment of Hb at MHAM@Mag-NPs was confirmed by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and Fourier transform infrared spectroscopy (FT-IR). Direct electron transfer of the Hb intercalated into the composite film showed a pair of well-defined quasi-reversible redox peak at formal potential of −0.255 V vs. Ag/AgCl corresponding to heme Fe(III)/Fe(II) redox couple. It shows that the MHAM@Mag-NPs composite could increase the adsorption ability for Hb, thus provides a facile direct electron transfer between the Hb and the substrate. The proposed biosensor showed excellent electrocatalytic activity to the H2O2 reduction in the wide concentration range from 5.0 to 300.0 µM obtained by amperometric measurement. The MichaelisMenten constant (Km) value of Hb at the modified electrode is 55.4 µM, showing its high affinity. Magnetic entrapment offers a promising design for fast, convenient and effective immobilization of protein within a few minutes for determination of the target molecule in low sample volume at disposable cost-effective SPCE. |
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Place of Publication |
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Wos |
000360772800071 |
Publication Date |
2015-07-05 |
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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 |
0956-5663 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.78 |
Times cited |
14 |
Open Access |
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Notes |
; We are thankful for the BOF financial support from the University of Antwerp and Hercules financial support (SEM). ; |
Approved |
Most recent IF: 7.78; 2015 IF: 6.409 |
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Call Number |
UA @ admin @ c:irua:126535 |
Serial |
5731 |
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| Permanent link to this record |
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Author |
Daems, D.; De Wael, K.; Vissenberg, K.; Van Camp, G.; Nagels, L. |
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Title |
Potentiometric sensors doped with biomolecules as a new approach to small molecule/biomolecule binding kinetics analysis |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Biosensors and bioelectronics |
Abbreviated Journal |
Biosens Bioelectron |
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Volume |
54 |
Issue |
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Pages |
515-520 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Integrated Molecular Plant Physiology Research (IMPRES); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The most successful binding kinetics analysis systems at this moment include surface plasmon resonance (SPR), quartz microcrystal balance (QMB) and surface acoustic wave (SAW). Although these are powerful methods, they generally are complex, expensive and require the use of monolayers. Here, we report on potentiometric sensors as an inexpensive and simple alternative to do binding kinetics analysis between small molecules in solution and biomolecules (covalently) attached in a biopolymer sensor coating layer. As an example, dopamine and an anti-dopamine aptamer were used as the small molecule and the biomolecule respectively. Binding between both follows a Langmuir adsorption type model and creates a surface potential. The system operates in Flow Injection Analysis mode (FIA). Besides being an interesting new binding kinetics tool, the approach allows systematic design of potentiometric biosensors (in the present study a dopamine sensor), and gives new insights into the functioning of ion-selective electrodes (ISEs). |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000333071500077 |
Publication Date |
2013-11-24 |
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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 |
0956-5663 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.78 |
Times cited |
10 |
Open Access |
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Notes |
; Financial support for this work was provided by the University of Antwerp by granting L.N. and G.V.C. a BOF interdisciplinary research project. ; |
Approved |
Most recent IF: 7.78; 2014 IF: 6.409 |
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Call Number |
UA @ admin @ c:irua:111678 |
Serial |
5780 |
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Author |
Rahemi, V.; Trashin, S.; Hafideddine, Z.; Van Doorslaer, S.; Meynen, V.; Gorton, L.; De Wael, K. |
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Title |
Amperometric flow-injection analysis of phenols induced by reactive oxygen species generated under daylight irradiation of titania impregnated with horseradish peroxidase |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Analytical Chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
92 |
Issue |
92 |
Pages |
3643-3649 |
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Keywords |
A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Titanium dioxide (TiO2) is a unique material for biosensing applications due to its capability of hosting enzymes. For the first time, we show that TiO2 can accumulate reactive oxygen species (ROS) under daylight irradiation and can support the catalytic cycle of horseradish peroxidase (HRP) without the need of H2O2 to be present in the solution. Phenolic compounds, such as hydroquinone (HQ) and 4-aminophenol (4-AP), were detected amperometrically in flow-injection analysis (FIA) mode via the use of an electrode modified with TiO2 impregnated with HRP. In contrast to the conventional detection scheme, no H2O2 was added to the analyte solution. Basically, the inherited ability of TiO2 to generate reactive oxygen species is used as a strategy to avoid adding H2O2 in the solution during the detection of phenolic compounds. Electron paramagnetic resonance (EPR) spectroscopy indicates the presence of ROS on titania which, in interaction with HRP, initiate the electrocatalysis toward phenolic compounds. The amperometric response to 4-AP was linear in the concentration range between 0.05 and 2 μM. The sensitivity was 0.51 A M–1 cm–2, and the limit of detection (LOD) 26 nM. The proposed sensor design opens new opportunities for the detection of phenolic traces by HRP-based electrochemical biosensors, yet in a more straightforward and sensitive way following green chemistry principles of avoiding the use of reactive and harmful chemical, such as H2O2. |
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Place of Publication |
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Wos |
000518234700023 |
Publication Date |
2020-01-27 |
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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 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.4 |
Times cited |
3 |
Open Access |
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Notes |
; The authors thank Scientific Reseatch-Flanders (F-WO) (grant 12T4219N) for funding. ; |
Approved |
Most recent IF: 7.4; 2020 IF: 6.32 |
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Call Number |
UA @ admin @ c:irua:166241 |
Serial |
5463 |
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Author |
Schram, J.; Parrilla, M.; Sleegers, N.; Samyn, N.; Bijvoets, S.M.; Heerschop, M.W.J.; van Nuijs, A.L.N.; De Wael, K. |
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Title |
Identifying Electrochemical Fingerprints of Ketamine with Voltammetry and Liquid Chromatography–Mass Spectrometry for Its Detection in Seized Samples |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Analytical Chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
92 |
Issue |
19 |
Pages |
13485-13492 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Toxicological Centre |
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Abstract |
Herein, a straightforward electrochemical approach for the determination of ketamine in street samples and seizures is presented by employing screen-printed electrodes (SPE). Square wave voltammetry (SWV) is used to study the electrochemical behavior of the illicit drug, thus profiling the different oxidation states of the substance at different pHs. Besides, the oxidation pathway of ketamine on SPE is investigated for the first time with liquid chromatography–high-resolution mass spectrometry. Under the optimized conditions, the calibration curve of ketamine at buffer solution (pH 12) exhibits a sensitivity of 8.2 μA μM–1, a linear relationship between 50 and 2500 μM with excellent reproducibility (RSD = 2.2%, at 500 μM, n = 7), and a limit of detection (LOD) of 11.7 μM. Subsequently, binary mixtures of ketamine with adulterants and illicit drugs are analyzed with SWV to investigate the electrochemical fingerprint. Moreover, the profile overlapping between different substances is addressed by the introduction of an electrode pretreatment and the integration of a tailor-made script for data treatment. Finally, the approach is tested on street samples from forensic seizures. Overall, this system allows for the on-site identification of ketamine by law enforcement agents in an easy-to-use and rapid manner on cargos and seizures, thereby disrupting the distribution channel and avoiding the illicit drug reaching the end-user. |
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Place of Publication |
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Wos |
000580426800091 |
Publication Date |
2020-10-06 |
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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 |
0003-2700 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.4 |
Times cited |
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Open Access |
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Notes |
Universiteit Antwerpen; H2020 Societal Challenges, 833787 ; Fonds Wetenschappelijk Onderzoek, 1S3765817N 1SB8120N ; |
Approved |
Most recent IF: 7.4; 2020 IF: 6.32 |
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Call Number |
AXES @ axes @c:irua:170523 |
Serial |
6435 |
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Author |
Neven, L.; Barich, H.; Ching, H.Y.V.; Khan, S.U.; Colomier, C.; Patel, H.H.; Gorun, S.M.; Verbruggen, S.; Van Doorslaer, S.; De Wael, K. |
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Title |
Correlation between the fluorination degree of perfluorinated zinc phthalocyanines, their singlet oxygen generation ability, and their photoelectrochemical response for phenol sensing |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
94 |
Issue |
13 |
Pages |
5221-5230 |
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Keywords |
A1 Journal article; Organic synthesis (ORSY); Sustainable Energy, Air and Water Technology (DuEL); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
Electron-withdrawing perfluoroalkyl peripheral groups grafted on phthalocyanine (Pc) macrocycles improve their single-site isolation, solubility, and resistance to self-oxidation, all beneficial features for catalytic applications. A high degree of fluorination also enhances the reducibility of Pcs and could alter their singlet oxygen (1O2) photoproduction. The ethanol/toluene 20:80 vol % solvent mixture was found to dissolve perfluorinated FnPcZn complexes, n = 16, 52, and 64, and minimize the aggregation of the sterically unencumbered F16PcZn. The 1O2 production ability of FnPcZn complexes was examined using 9,10-dimethylanthracene (DMA) and 2,2,6,6-tetramethylpiperidine (TEMP) in combination with UV–vis and electron paramagnetic resonance (EPR) spectroscopy, respectively. While the photoreduction of F52PcZn and F64PcZn in the presence of redox-active TEMP lowered 1O2 production, DMA was a suitable 1O2 trap for ranking the complexes. The solution reactivity was complemented by solid-state studies via the construction of photoelectrochemical sensors based on TiO2-supported FnPcZn, FnPcZn|TiO2. Phenol photo-oxidation by 1O2, followed by its electrochemical reduction, defines a redox cycle, the 1O2 production having been found to depend on the value of n and structural features of the supported complexes. Consistent with solution studies, F52PcZn was found to be the most efficient 1O2 generator. The insights on reactivity testing and structural–activity relationships obtained may be useful for designing efficient and robust sensors and for other 1O2-related applications of FnPcZn. |
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Place of Publication |
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Editor |
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Wos |
000786254500002 |
Publication Date |
2022-03-22 |
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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 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.4 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 7.4 |
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Call Number |
UA @ admin @ c:irua:187522 |
Serial |
7141 |
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Author |
Khan, S.U.; Trashin, S.; Beltran, V.; Korostei, Y.S.; Pelmus, M.; Gorun, S.M.; Dubinina, T., V.; Verbruggen, S.W.; De Wael, K. |
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Title |
Photoelectrochemical behavior of phthalocyanine-sensitized TiO₂ in the presence of electron-shuttling mediators |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
94 |
Issue |
37 |
Pages |
12723-12731 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
Dye-sensitized TiO(2 )has found many applications for dye sensitized solar cells (DSSC), solar-to-chemical energy conversion, water/air purification systems, and (electro)chemical sensors. We report an electrochemical system for testing dye-sensitized materials that can be utilized in photoelectrochemical (PEC) sensors and energy conversion. Unlike related systems, the reported system does not require a direct electron transfer from semiconductors to electrodes. Rather, it relies on electron shuttling by redox mediators. A range of model photocatalytic materials were prepared using three different TiO2 materials (P25, P90, and PC500) and three sterically hindered phthalocyanines (Pcs) with electron-rich tert-butyl substituents (t-Bu4PcZn, t-Bu4PcAlCl, and t-Bu4PcH2). The materials were compared with previously developed TiO(2 )modified by electron-deficient, also sterically hindered fluorinated phthalocyanine F64PcZn, a singlet oxygen (O-1(2)) producer, as well as its metal-free derivative, F64PcH2. The PEC activity depended on the redox mediator, as well as the type of TiO2 and Pc. By comparing the responses of one-electron shuttles, such as K4Fe(CN)(4), and O-1(2)-reactive electron shuttles, such as phenol, it is possible to reveal the action mechanism of the supported photosensitizers, while the overall activity can be assessed using hydroquinone. t-Bu4PcAlCl showed significantly lower blank responses and higher specific responses toward chlorophenols compared to t-Bu4PcZn due to the electron-withdrawing effect of the Al3+ metal center. The combination of reactivity insights and the need for only microgram amounts of sensing materials renders the reported system advantageous for practical applications. |
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Corporate Author |
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Place of Publication |
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Editor |
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Wos |
000855284300001 |
Publication Date |
2022-09-12 |
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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 |
0003-2700; 5206-882x |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.4 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 7.4 |
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Call Number |
UA @ admin @ c:irua:190602 |
Serial |
7190 |
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Author |
Almabadi, M.H.; Truta, F.M.; Adamu, G.; Cowen, T.; Tertis, M.; Alanazi, K.D.M.; Stefan, M.-G.; Piletska, E.; Kiss, B.; Cristea, C.; De Wael, K.; Piletsky, S.A.; Cruz, A.G. |
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Title |
Integration of smart nanomaterials for highly selective disposable sensors and their forensic applications in amphetamine determination |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Electrochimica acta |
Abbreviated Journal |
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Volume |
446 |
Issue |
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Pages |
142009-142010 |
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Keywords |
A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
Screening drugs on the street and biological samples pose a challenge to law enforcement agencies due to existing detection methods and instrument limitations. Herein we present a graphene-assisted molecularly imprinted polymer nanoparticle-based sensor for amphetamine. These nanoparticles are electroactive by incorporating ferrocene in their structure. These particles act as specific actuators in electrochemical sensors, and the presence of a ferrocene redox probe embedded in the structure allows the detection of non-electroactive amphetamine. In a control approach, nanoparticles were covalently immobilised onto electrochemical sensors by drop-casting using silanes. Alternatively, nanoparticles were immobilised employing 3D printing and a graphene ink composite. The electrochemical performance of both approaches was evaluated. As a result, 3D printed nanoMIPs/graphene sensors displayed the highest selectivity in spiked human plasma, with sensitivity at 73 nA nM-1, LOD of 68 nM (RSD 2.4%) when compared to the silane drop cast electrodes. The main advantage of the optimised 3D printing technology is that it allows quantitative determination of amphetamine, a nonelectroactive drug, challenging to detect with conventional electrochemical sensors. In addition, the costefficient 3D printing method makes these sensors easy to manufacture, leading to robust, highly selective and sensitive sensors. As proof of concept, sensors were evaluated on the street specimens and clinically relevant samples and successfully validated using UPLC-MS. |
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Wos |
000953087600001 |
Publication Date |
2023-02-09 |
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ISSN |
0013-4686 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 6.6; 2023 IF: 4.798 |
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Call Number |
UA @ admin @ c:irua:196145 |
Serial |
8888 |
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Author |
Muhammad, S.; Wuyts, K.; Nuyts, G.; De Wael, K.; Samson, R. |
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Title |
Characterization of epicuticular wax structures on leaves of urban plant species and its association with leaf wettability |
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A1 Journal article |
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Year |
2020 |
Publication |
Urban Forestry & Urban Greening |
Abbreviated Journal |
Urban For Urban Gree |
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Volume |
47 |
Issue |
47 |
Pages |
126557 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Epicuticular wax (EW) protects the plant’s integrity and acts as a barrier against biotic and abiotic stresses. The micro-structured three-dimensional EW’s and presence of leaf trichomes influence the wettability of a leaf surface. In this study, leaves of 96 perennial urban plant species were examined to determine an association between epicuticular wax structure (EWS) types and leaf wettability and investigate their seasonal variation. The EWS types were identified using Scanning Electron Microscopy (SEM), while leaf wettability was analyzed by measuring the drop contact angle (DCA) on both the abaxial and the adaxial sides of leaves collected from a common garden in June and September 2016. Four distinct EWS types namely thin film, platelets, crusts, and tubules were observed on leaves of investigated plant species in both June and September. The EWS types varied significantly between functional plant types and plant families in both June and September. In June, the abaxial DCA ranged from 56° to 147°, and the adaxial DCA ranged from 56° to 136°. In September, the abaxial DCA ranged from 54° to 130°, and the adaxial DCA ranged from 51° to 125°. The effect of time, leaf side, and EWS type on leaf wettability were significant. Plant species which showed a change in EWS type or clustering from June to September did not show a more pronounced reduction in DCA compared to those species which exhibited a constant EWS type. Findings from our study illustrate that DCA is not a good indicator in determining the different EWS types due to overlapping DCA intervals between the identified EWS types. However, the identified EWS types remained fairly stable throughout the in-leaf season and do not require repeated measurements for characterization. |
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000508389000028 |
Publication Date |
2019-12-05 |
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ISSN |
1618-8667 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.4 |
Times cited |
5 |
Open Access |
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Notes |
; The research was funded by the Ontario Student Assistance Program (OSAP # 15103399). The SEM equipment was funded by FWO/Hercules. The authors acknowledge the help of the ENdEMIC group involved in the upkeep of the experimental site. The authors would like to thank the anonymous reviewers for their critical comments and constructive suggestions in improving the quality of the article. ; |
Approved |
Most recent IF: 6.4; 2020 IF: 2.113 |
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Call Number |
UA @ admin @ c:irua:164906 |
Serial |
5504 |
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Author |
Rahemi, V.; Sarmadian, N.; Anaf, W.; Janssens, K.; Lamoen, D.; Partoens, B.; De Wael, K. |
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Title |
Unique opto-electronic structure and photo reduction properties of sulfur doped lead chromates explaining their instability in paintings |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Analytical chemistry |
Abbreviated Journal |
Anal Chem |
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Volume |
89 |
Issue |
89 |
Pages |
3326-3334 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Chrome yellow refers to a group of synthetic inorganic pigments that became popular as an artists material from the second quarter of the 19th century. The color of the pigment, in which the chromate ion acts as a chromophore, is related to its chemical composition (PbCr1-xSxO4, with 0≤x≤0.8) and crystalline structure (monoclinic/orthorhombic). Their shades range from the yellow-orange to the paler yellow tones with increasing sulfate amount. These pigments show remarkable signs of degradation after limited time periods. Pure PbCrO4 (crocoite in its natural form) has a deep yellow color and is relatively stable, while the co-precipitate with lead sulfate (PbCr1-xSxO4) has a paler shade and seems to degrade faster. This degradation is assumed to be related to the reduction of Cr(VI) to Cr(III). We show that on increasing the sulfur(S)-content in chrome yellow, the band gap increases. Typically, when increasing the band gap, one might assume that a decrease in photo activity is the result. However, the photo activity relative to the Cr content, and thus Cr reduction, of sulfur-rich PbCr1-xSxO4 is found to be much higher compared to the sulfur-poor or non-doped lead chromates. This discrepancy can be explained by the evolution of the crystal and electronic structure as function of the sulfur content: first-principles density functional theory calculations show that both the absorption coefficient and reflection coefficients of the lead chromates change as a result of the sulfate doping in such a way that the generation of electron-hole pairs under illumination relative to the total Cr content increases. These changes in the material properties explain why paler shade yellow colors of this pigment are more prone to discoloration. The electronic structure calculations also demonstrate that lead chromate and its co-precipitates are p-type semiconductors, which explains the observed reduction reaction. As understanding this phenomenon is valuable in the field of cultural heritage, this study is the first joint action of photo-electrochemical measurements and first-principles calculations to approve the higher tendency of sulfur-rich lead chromates to darken. |
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Washington, D.C. |
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Wos |
000397478300015 |
Publication Date |
2017-02-23 |
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ISSN |
0003-2700 |
ISBN |
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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 |
7 |
Open Access |
OpenAccess |
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Notes |
; The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the Hercules Foundation and the Flemish Government, department EWI. The BOF-GOA action SOLARPAINT of the University of Antwerp Research Council is acknowledged for financial support. W.A. acknowledges support from BELSPO project S2-ART. Dr. L. Monico and Dr. C. Miliani (ISTM, Perugia) are gratefully acknowledged for helpful discussions and for providing some of the initial batches of the materials studied. ; |
Approved |
Most recent IF: 6.32 |
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Call Number |
UA @ lucian @ c:irua:140886 |
Serial |
4451 |
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