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“Room-temperature study of iron gall ink impregnated paper degradation under various oxygen and humidity conditions : time-dependent monitoring by viscosity and X-ray absorption near-edge spectrometry measurements”. Rouchon V, Duranton M, Burgaud C, Pellizzi E, Lavédrine B, Janssens K, de Nolf W, Nuyts G, Vanmeert F, Hellemans K, Analytical chemistry 83, 2589 (2011). http://doi.org/10.1021/AC1029242
Abstract: Many western manuscripts were written using iron gall inks. These inks can damage the paper via two major mechanisms: (a) acid hydrolysis, enhanced by humidity, and (b) oxidative depolymerization provoked by the presence of oxygen and free iron(II) ions. The degradation of unsized Whatman paper impregnated with different combinations of iron sulfate, gallic acid, and gum arabic was studied at room temperature in order to assess the relative importance of each mechanism. The samples were stored in various environments including a dry and/or an oxygen-free atmosphere. The cellulose depolymerization was monitored by viscometry and related to changes in the oxidation state of iron, determined by X-ray absorption near-edge spectrometry. The results indicate that residual amounts of oxygen (less than 0.1%) promote cellulose depolymerization, whereas the level of relative humidity has no impact. The cellulose depolymerization also appears closely correlated to oxidative mechanisms. Regarding the oxidation of iron, it only occurs in the simultaneous presence of oxygen and moisture, suggesting the occurrence of rustlike oxidative mechanisms. Finally, the presence of gallic acid has a strong influence, which is only partially explained by its capacity to reduce iron(III) to iron(II).
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.32
Times cited: 28
DOI: 10.1021/AC1029242
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“Characterization of epicuticular wax structures on leaves of urban plant species and its association with leaf wettability”. Muhammad S, Wuyts K, Nuyts G, De Wael K, Samson R, Urban Forestry &, Urban Greening 47, 126557 (2020). http://doi.org/10.1016/J.UFUG.2019.126557
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.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.4
Times cited: 5
DOI: 10.1016/J.UFUG.2019.126557
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“Effect of ultra-fine fly ash on concrete performance and durability”. Kara De Maeijer P, Craeye B, Snellings R, Kazemi-Kamyab H, Loots M, Janssens K, Nuyts G, Construction And Building Materials 263, 120493 (2020). http://doi.org/10.1016/J.CONBUILDMAT.2020.120493
Abstract: In the present study ultra-fine fly ash as a novel by-product obtained by a dry and closed separation process was investigated as cement replacement in concrete. The impact of ultra-fine fly ash on material properties was investigated following an upscaling as an approach considering paste, mortar and concrete properties. Two types of cement, Portland cement (CEMI) and slag cement (CEMIII), two types of ultra-fly ashes, one with particle size d90< 9.3lm (FA1) and second with d90< 4.6lm (FA2) were used.At paste- and mortar- level, cement was replaced at 0%, 15%, 25%, 35% and 50% with FA1 and FA2. At concrete- level, cement was replaced at 0%, 15% and 25% with different ratios of FA1 and FA2. The results at paste- and mortar- level showed that an increased fineness of the fly ash (FA2) contributes to better workability of the mix. For CEMI, the compressive strength of concrete with FA2 at 25% cement replacement was already equal to the reference 0% replacement concrete at the age of 28 days. For CEMIII, the compressive strength of concrete mix with FA1 with 15% and FA2 with 25% cement replacements reached the reference concrete value at the age of 91 days. Regarding the durability, replacing cement with ultra-fine fly ash (FA2) had a positive influence on the resistivity, chloride migration coefficient and alkali-silica reaction (ASR), and a negative influence on the carbonation resistance.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Energy and Materials in Infrastructure and Buildings (EMIB)
Impact Factor: 7.4
DOI: 10.1016/J.CONBUILDMAT.2020.120493
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“Damages induced by synchrotron radiation-based X-ray microanalysis in chrome yellow paints and related Cr-compounds : assessment, quantification, and mitigation strategies”. Monico L, Cotte M, Vanmeert F, Amidani L, Janssens K, Nuyts G, Garrevoet J, Falkenberg G, Glatzel P, Romani A, Miliani C, Analytical Chemistry 92, 14164 (2020). http://doi.org/10.1021/ACS.ANALCHEM.0C03251
Abstract: Synchrotron radiation (SR)-based X-ray methods are powerful analytical tools for several purposes. They are widely used to probe the degradation mechanisms of inorganic artists' pigments in paintings, including chrome yellows (PbCr1-xSxO4; 0 <= x <= 0.8), a class of compounds often found in Van Gogh masterpieces. However, the high intensity and brightness of SR beams raise important issues regarding the potential damage inflicted on the analyzed samples. A thorough knowledge of the SR X-ray sensitivity of each class of pigment in the painting matrix is therefore required to find analytical strategies that seek to minimize the damage for preserving the integrity of the analyzed samples and to avoid data misinterpretation. Here, we employ a combination of Cr K-edge X-ray absorption near-edge structure spectroscopy, Cr-K-beta X-ray emission spectroscopy, and X-ray diffraction to monitor and quantify the effects of SR X-rays on the stability of chrome yellows and related Cr compounds and to define mitigation strategies. We found that the SR X-ray beam exposure induces changes in the oxidation state and local coordination environment of Cr ions and leads to a loss of the compound's crystalline structure. The extent of X-ray damage depends on some intrinsic properties of the samples (chemical composition of the pigment and the presence/absence and nature of the binder). It can be minimized by optimizing the overall fluence/dose released to the samples and by working in vacuum and under cryogenic conditions.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 7.4
DOI: 10.1021/ACS.ANALCHEM.0C03251
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“Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists&rsquo, Pigments”. 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, Chemistry Of Materials 32, 2863 (2020). http://doi.org/10.1021/acs.chemmater.9b04821
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.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 8.6
Times cited: 8
DOI: 10.1021/acs.chemmater.9b04821
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“Stable Rh particles in hydrotalcite-derived catalysts coated on FeCrAlloy foams by electrosynthesis”. Benito P, Nuyts G, Monti M, de Nolf W, Fornasari G, Janssens K, Scavetta E, Vaccari A, Applied catalysis : B : environmental 179, 321 (2015). http://doi.org/10.1016/J.APCATB.2015.05.035
Abstract: Rh-based structured catalysts for the Catalytic Partial Oxidation of CH4 to syngas were prepared by electrosynthesis of Rh/Mg/Al hydrotalcite-type compounds on FeCrAlloy foams and calcination. The effects of Rh content, total metal concentration, and partial replacement of Mg2+ by Ni2+ in the electrolytic solution on coating thickness, Rh speciation, metallic particle size, and catalytic activity were investigated by SEM/EDS, mu-XRF/XANES and tests under diluted and concentrated reaction conditions. The amount of Rh species, present as Mg (RhxAl1-x)(2)O-4, depended on the thickness of the electrosynthesised layer as well as the Rh particle size and dispersion. Smaller and more dispersed particles were obtained by decreasing the Rh concentration in the electrolytic solution from Rh/Mg/Al=11/70/19 to 5/70/25 and 2/70/28 atomic ratio% (a.r.%) and in thinner rather than thicker layers. Despite the improvement in metallic particles features, the CH4 conversion was negatively affected by the low amount of active sites in the coating, the high metal support interaction and possibly the oxidation of metallic particles and carbon formation. A larger amount of solid containing well dispersed Rh particles was deposited by increasing the total metal concentration from 0.03 M to 0.06 M with the Rh/Mg/Al=5/70/25 a.r.%, and the catalytic performances were enhanced. The partial replacement of Mg2+ by Ni2+ gave rise to a very active bimetallic Rh/Ni catalyst, CH4 conversion and selectivity to syngas were above 90%, however, it slightly deactivated with time-on-stream. (C) 2015 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 9.446
Times cited: 14
DOI: 10.1016/J.APCATB.2015.05.035
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“Role of coating-metallic support interaction in the properties of electrosynthesized Rh-based structured catalysts”. Benito P, de Nolf W, Nuyts G, Janssens K, et al, ACS catalysis 4, 3779 (2014). http://doi.org/10.1021/CS501079K
Abstract: Rh-structured catalysts for the catalytic partial oxidation of CH4 to syngas were prepared by electrosynthesis of Rh-containing hydrotalcite-type (HT) compounds on FeCrAlloy foams followed by calcination at 900 degrees C. During the calcination the simultaneous decomposition of the layered HT structure and formation of the protective FeCrAlloy outer shell in alumina occurred. Here, we studied the role of the coating-metallic support interaction in the properties of the catalysts after calcination, H-2 reduction, and catalytic tests, by a combination of electron (FEG-SEM/EDS) and synchrotron X-ray (XRF/XRPD and XRF/XANES) microscopic techniques. The characterization of crystalline phases in the metallic support and coating and distribution of Rh active species was carried out on several samples prepared by modifying the Rh content in the electrolytic solution (Rh/Mg/Al = 11.0/70.0/19.0, 5.0/70.0/25.0, 0/70.0/30.0 atomic ratio). A sample was also prepared with no aluminum in the electrolytic solution (Rh/Mg/Al = 13.6/86.4/0.0 atomic ratio) and calcined at 550 and 900 degrees C. The interaction between the elements of the metallic support and the catalytic coating increased the film adhesion during the thermal treatment and catalytic tests and modified the catalyst crystalline phases. A chemical reaction between Al corning from the foam and Mg in the coating occurred during calcination at high temperature leading to the formation of spinel phases in which rhodium is solved, together with some Rh2O3 and Rh. The metallic support was oxidized forming the corundum scale and chromium oxides, moreover t-Al2O3 was identified. For the Rh11.0Mg70.0Al19.0 catalyst the inclusion of Rh in the spinel phase decreased its reducibility in the H-2 pretreatment. The reduction continued during catalytic tests by feeding diluted CH4/O-2/He gas mixtures, evidenced by the catalyst activation. While under concentrated gas mixtures the deactivation occurred, probably by oxidation.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 10.614
Times cited: 13
DOI: 10.1021/CS501079K
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“Synchrotron XRF analysis identifies cerium accumulation colocalized with pharyngeal deformities in CeO₂, NP-exposed caenorhabditis elegans”. Rossbach LM, Brede DA, Nuyts G, Cagno S, Olsson RMS, Oughton DH, Falkenberg G, Janssens K, Lind OC, Environmental science and technology 56, 5081 (2022). http://doi.org/10.1021/ACS.EST.1C08509
Abstract: A combination of synchrotron radiation-based elementalimaging, in vivo redox status analysis, histology, and toxic responses was usedto investigate the uptake, biodistribution, and adverse effects of Cenanoparticles (CeO2NP; 10 nm; 0.5-34.96 mg Ce L-1) or Ce(NO3)3(2.3-26 mg Ce L-1)inCaenorhabditis elegans. Elemental mapping of theexposed nematodes revealed Ce uptake in the alimentary canal prior todepuration. Retention of CeO2NPs was low compared to that of Ce(NO3)3in depurated individuals. X-rayfluorescence (XRF) mapping showed that Cetranslocation was confined to the pharyngeal valve and foregut. Ce(NO3)3exposure significantly decreased growth, fertility, and reproduction, causedslightly reduced fecundity. XRF mapping and histological analysis revealedsevere tissue deformities colocalized with retained Ce surrounding thepharyngeal valve. Both forms of Ce activated the sod-1 antioxidant defense,particularly in the pharynx, whereas no significant effects on the cellular redox balance were identified. The CeO2NP-induceddeformities did not appear to impair the pharyngeal function or feeding ability as growth effects were restricted to Ce(NO3)3exposure. The results demonstrate the utility of integrated submicron-resolution SR-based XRF elemental mapping of tissue-specificdistribution and adverse effect analysis to obtain robust toxicological evaluations of metal-containing contaminants.
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 11.4
DOI: 10.1021/ACS.EST.1C08509
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“Synchrotron XRF and histological analyses identify damage to digestive tract of uranium NP-exposed Daphnia magna”. Byrnes I, Rossbach LM, Jaroszewicz J, Grolimund D, Sanchez DF, Gomez-Gonzalez MA, Nuyts G, Reinoso-Maset E, Janssens K, Salbu B, Brede DA, Lind OC, Environmental science and technology 57, 1071 (2023). http://doi.org/10.1021/ACS.EST.2C07174
Abstract: Micro-and nanoscopic X-ray techniques were used to investigate the relationship between uranium (U) tissue distributions and adverse effects to the digestive tract of aquatic model organism Daphnia magna following uranium nanoparticle (UNP) exposure. X-ray absorption computed tomography measure-ments of intact daphnids exposed to sublethal concentrations of UNPs or a U reference solution (URef) showed adverse morphological changes to the midgut and the hepatic ceca. Histological analyses of exposed organisms revealed a high proportion of abnormal and irregularly shaped intestinal epithelial cells. Disruption of the hepatic ceca and midgut epithelial tissues implied digestive functions and intestinal barriers were compro-mised. Synchrotron-based micro X-ray fluorescence (XRF) elemental mapping identified U co-localized with morphological changes, with substantial accumulation of U in the lumen as well as in the epithelial tissues. Utilizing high-resolution nano-XRF, 400-1000 nm sized U particulates could be identified throughout the midgut and within hepatic ceca cells, coinciding with tissue damages. The results highlight disruption of intestinal function as an important mode of action of acute U toxicity in D. magna and that midgut epithelial cells as well as the hepatic ceca are key target organs.
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 11.4
DOI: 10.1021/ACS.EST.2C07174
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“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”. Beltran V, Marchetti A, Nuyts G, Leeuwestein M, Sandt C, Borondics F, De Wael K, Angewandte Chemie-International Edition 60, 22753 (2021). http://doi.org/10.1002/ANIE.202106058
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.
Keywords: A1 Journal article; Art; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 11.994
DOI: 10.1002/ANIE.202106058
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“Probing the chemistry of CdS paints in The Scream by in situ noninvasive spectroscopies and synchrotron radiation x-ray techniques”. Monico L, Cartechini L, Rosi F, Chieli A, Grazia C, De Meyer S, Nuyts G, Vanmeert F, Janssens K, Cotte M, De Nolf W, Falkenberg G, Sandu ICA, Tveit ES, Mass J, De Freitas RP, Romani A, Miliani C, Science Advances 6, eaay3514 (2020). http://doi.org/10.1126/SCIADV.AAY3514
Abstract: The degradation of cadmium sulfide (CdS)-based oil paints is a phenomenon potentially threatening the iconic painting The Scream (ca. 1910) by Edvard Munch (Munch Museum, Oslo) that is still poorly understood. Here, we provide evidence for the presence of cadmium sulfate and sulfites as alteration products of the original CdS-based paint and explore the external circumstances and internal factors causing this transformation. Macroscale in situ noninvasive spectroscopy studies of the painting in combination with synchrotron-radiation x-ray microspectroscopy investigations of a microsample and artificially aged mock-ups show that moisture and mobile chlorine compounds are key factors for promoting the oxidation of CdS, while light (photodegradation) plays a less important role. Furthermore, under exposure to humidity, parallel/secondary reactions involving dissolution, migration through the paint, and recrystallization of water-soluble phases of the paint are associated with the formation of cadmium sulfates.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 13.6
Times cited: 4
DOI: 10.1126/SCIADV.AAY3514
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“Novel optical photothermal infrared (O-PTIR) spectroscopy for the noninvasive characterization of heritage glass-metal objects”. Marchetti A, Beltran V, Nuyts G, Borondics F, De Meyer S, Van Bos M, Jaroszewicz J, Otten E, Debulpaep M, De Wael K, Science Advances 8, eabl6769 (2022). http://doi.org/10.1126/SCIADV.ABL6769
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.
Keywords: A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 13.6
DOI: 10.1126/SCIADV.ABL6769
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“Synchrotron-based X-ray fluorescence imaging elucidates uranium toxicokinetics in Daphnia magna”. Byrnes I, Rossbach LM, Brede DA, Grolimund D, Sanchez DF, Nuyts G, Cuba V, Reinoso-Maset E, Salbu B, Janssens K, Oughton D, Scheibener S, Teien H-C, Lind OC, ACS nano 17, 5296 (2023). http://doi.org/10.1021/ACSNANO.2C06111
Abstract: A combination of synchrotron-based elemental anal-ysis and acute toxicity tests was used to investigate the biodistribution and adverse effects in Daphnia magna exposed to uranium nanoparticle (UNP, 3-5 nm) suspensions or to uranium reference (Uref) solutions. Speciation analysis revealed similar size distributions between exposures, and toxicity tests showed com-parable acute effects (UNP LC50: 402 mu g L-1 [336-484], Uref LC50: 268 mu g L-1 [229-315]). However, the uranium body burden was 3 -to 5-fold greater in UNP-exposed daphnids, and analysis of survival as a function of body burden revealed a similar to 5-fold higher specific toxicity from the Uref exposure. High-resolution X-ray fluorescence elemental maps of intact, whole daphnids from sublethal, acute exposures of both treatments revealed high uranium accumulation onto the gills (epipodites) as well as within the hepatic ceca and the intestinal lumen. Uranium uptake into the hemolymph circulatory system was inferred from signals observed in organs such as the heart and the maxillary gland. The substantial uptake in the maxillary gland and the associated nephridium suggests that these organs play a role in uranium removal from the hemolymph and subsequent excretion. Uranium was also observed associated with the embryos and the remnants of the chorion, suggesting uptake in the offspring. The identification of target organs and tissues is of major importance to the understanding of uranium and UNP toxicity and exposure characterization that should ultimately contribute to reducing uncertainties in related environmental impact and risk assessments.
Keywords: A1 Journal article; Engineering sciences. Technology; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 17.1
DOI: 10.1021/ACSNANO.2C06111
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“Plasmonic gold-embedded TiO2 thin films as photocatalytic self-cleaning coatings”. Peeters H, Keulemans M, Nuyts G, Vanmeert F, Li C, Minjauw M, Detavernier C, Bals S, Lenaerts S, Verbruggen SW, Applied Catalysis B-Environmental 267, 118654 (2020). http://doi.org/10.1016/j.apcatb.2020.118654
Abstract: Transparent photocatalytic TiO2 thin films hold great potential in the development of self-cleaning glass sur-
faces, but suffer from a poor visible light response that hinders the application under actual sunlight. To alleviate this problem, the photocatalytic film can be modified with plasmonic nanoparticles that interact very effectively with visible light. Since the plasmonic effect is strongly concentrated in the near surroundings of the nano- particle surface, an approach is presented to embed the plasmonic nanostructures in the TiO2 matrix itself, rather than deposit them loosely on the surface. This way the interaction interface is maximised and the plasmonic effect can be fully exploited. In this study, pre-fabricated gold nanoparticles are made compatible with the organic medium of a TiO2 sol-gel coating suspension, resulting in a one-pot coating suspension. After spin coating, homogeneous, smooth, highly transparent and photoactive gold-embedded anatase thin films are ob- tained.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 22.1
Times cited: 57
DOI: 10.1016/j.apcatb.2020.118654
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