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Author (up) Truta, F.M.; Cruz, A.G.; Dragan, A.-M.; Tertis, M.; Cowen, T.; Stefan, M.-G.; Topala, T.; Slosse, A.; Piletska, E.; Van Durme, F.; Kiss, B.; De Wael, K.; Piletsky, S.A.; Cristea, C.
Title Design of smart nanoparticles for the electrochemical detection of 3,4-methylenedioxymethamphetamine to allow in field screening by law enforcement officers Type A1 Journal article
Year 2023 Publication Drug testing and analysis Abbreviated Journal
Volume Issue Pages 1-14
Keywords A1 Journal article; Pharmacology. Therapy; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract A portable and highly sensitive sensor was designed for the specific detection of 3,4-methyl-enedioxy-methamphetamine (MDMA), in a range of field-testing situations. The sensor can detect MDMA in street samples, even when other controlled substances drugs, or adulterants are present. In this work, we report for the first time a sensor using electroactive molecularly imprinted polymer nanoparticles computationally designed to recognize MDMA and then produced using solid phase synthesis. A composite comprising chitosan, reduced graphene oxide, and molecularly imprinted polymer nanoparticles synthesized for MDMA for the first time was immobilized on screen-printed carbon electrodes. The sensors displayed a satisfactory sensitivity (106.8 nA x mu M-1), limit of detection (1.6 nM; 0.31 ng/mL), and recoveries (92-99%). The accuracy of the results was confirmed through validation using Ultra-High Performance Liquid Chromatography coupled with tandem Mass Spectrometry (UPLC-MS/MS). This technology could be used in forensic analysis and make it possible to selectively detect MDMA in street samples. A highly sensitive and portable sensor has been developed to detect MDMA in street samples. It uses electroactive molecularly imprinted polymer nanoparticles computationally designed to recognize MDMA, which were immobilized on screen-printed carbon electrodes with chitosan and graphene. The sensor showed good sensitivity and satisfactory recoveries (92-99%), confirmed with UPLC-MS/MS validation. This technology has the potential to be used in forensic analysis.image
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001107703400001 Publication Date 2023-11-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1942-7603; 1942-7611 ISBN Additional Links UA library record; WoS full record
Impact Factor 2.9 Times cited Open Access
Notes Approved Most recent IF: 2.9; 2023 IF: 3.469
Call Number UA @ admin @ c:irua:202058 Serial 9020
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Author (up) Van Echelpoel, R.; de Jong, M.; Daems, D.; van Espen, P.; De Wael, K.
Title Unlocking the full potential of voltammetric data analysis : a novel peak recognition approach for (bio)analytical applications Type A1 Journal article
Year 2021 Publication Talanta Abbreviated Journal Talanta
Volume 233 Issue Pages 122605
Keywords A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract Bridging the gap between complex signal data output and clear interpretation by non-expert end-users is a major challenge many scientists face when converting their scientific technology into a real-life application. Currently, pattern recognition algorithms are the most frequently encountered signal data interpretation algorithms to close this gap, not in the least because of their straight-forward implementation via convenient software packages. Paradoxically, just because their implementation is so straight-forward, it becomes cumbersome to integrate the expert's domain-specific knowledge. In this work, a novel signal data interpretation approach is presented that uses this domain-specific knowledge as its fundament, thereby fully exploiting the unique expertise of the scientist. The new approach applies data preprocessing in an innovative way that transcends its usual purpose and is easy to translate into a software application. Multiple case studies illustrate the straight-forward application of the novel approach. Ultimately, the approach is highly suited for integration in various (bio)analytical applications that require interpretation of signal data.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000668000500108 Publication Date 2021-06-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0039-9140; 1873-3573 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.162 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 4.162
Call Number UA @ admin @ c:irua:179417 Serial 8712
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Author (up) Van Echelpoel, R.; De Wael, K.
Title Voltammetric drug testing makes sense at the border Type A1 Journal article
Year 2024 Publication Nature Reviews Chemistry Abbreviated Journal
Volume Issue Pages 1-2
Keywords A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract The European BorderSens project leverages voltammetric sensors, developed with end-users' input, to rapidly and accurately detect illicit drugs. By embracing practicalities and validation, this technology has the potential to combat the illicit drug problem.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001142000900001 Publication Date 2024-01-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2397-3358 ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:202646 Serial 9112
Permanent link to this record
 

 
Author (up) Van Echelpoel, R.; Kranenburg, R.; van Asten, A.; De Wael, K.
Title Electrochemical detection of MDMA and 2C-B in ecstasy tablets using a selectivity enhancement strategy by in-situ derivatization Type A1 Journal article
Year 2022 Publication Forensic chemistry Abbreviated Journal
Volume 27 Issue Pages 100383
Keywords A1 Journal article; Pharmacology. Therapy; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Forensic drug laboratories are confronted with increasing amounts of drugs and a demand for faster results that are directly available on-site. In addition, the drug market is getting more complex with hundreds of new psychoactive substances (NPS) entering the market in recent years. Rapid and on-scene presumptive drug testing therefore faces a shift from manual colorimetric tests towards approaches that can detect a wider range of components and process results automatically. Electrochemical detection offers these desired characteristics, making it a suitable candidate for on-site drug detection. In this study, a two-step electrochemical sensor is introduced for the detection of MDMA and 2C-B. Firstly, a direct electrochemical analysis was performed to detect MDMA. Validation experiments on over 70 substances revealed that 2C-B was the only frequently encountered drug that gave a false positive result for MDMA in this first analysis. A second step using in-situ derivatization was subsequently introduced. To this end, formaldehyde was used for N-methylation of 2C-B thereby enhancing its electrochemical profile. The enriched electrochemical fingerprint in the second step allowed for clear differentiation between MDMA and 2C-B. The applicability of this approach was demonstrated with 71 ecstasy tablets seized by the Amsterdam Police. The MDMA/2C-B sensor correctly identified all 39 MDMA-containing tablets and 10 out of 11 tablets containing 2C-B. Most notably, correct results were also obtained for dark colored tablets in which both spectroscopic analysis and colorimetric tests failed due to obscured signals.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000725708200002 Publication Date 2021-11-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2468-1709 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.7 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 2.7
Call Number UA @ admin @ c:irua:183340 Serial 7149
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Author (up) Van Echelpoel, R.; Parrilla, M.; Sleegers, N.; Thiruvottriyur Shanmugam, S.; van Nuijs, A.L.N.; Slosse, A.; Van Durme, F.; De Wael, K.
Title Validated portable device for the qualitative and quantitative electrochemical detection of MDMA ready for on-site use Type A1 Journal article
Year 2023 Publication Microchemical journal Abbreviated Journal
Volume 190 Issue Pages 108693-10
Keywords A1 Journal article; Engineering sciences. Technology; Toxicological Centre; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Identifying and quantifying 3,4-methyl​enedioxy​methamphetamine (MDMA) on-site in suspected illicit drug samples, whether it be at recreational settings or manufacturing sites, is a major challenge for law enforcement agencies (LEAs). Various analytical techniques exist to fulfil this goal, e.g. colourimetry and portable spectroscopic techniques, each having its specific limitations (e.g. low accuracy, fluorescence, no quantification) and strengths (e.g. fast, easy to use). In this work, for the first time, an electrochemical MDMA sensor is presented to become a detection tool that can realistically be used on-site. More specifically, the use of a single buffer solution and an unmodified screen-printed electrode, along with the integration of a data analysis algorithm and mobile application permits the straightforward on-site identification and quantification of MDMA in suspicious samples. Multiple studies investigating different parameters, including pH, concentration, reproducibility, temperature and binary mixture analyses, were executed. To fully understand all the occurring redox processes, liquid chromatography coupled with high-resolution mass spectrometry analysis of partially electrolyzed MDMA samples was performed unravelling oxidation of the methylenedioxy group. Validation of the methodology was executed on 15 MDMA street samples analysed by gas chromatography coupled with mass spectrometry and compared with the performance of a commercial portable Raman and Attenuated Total Reflection Fourier Transform Infrared Spectroscopy (ATR-FTIR) device. The novel methodology outperformed the spectroscopic techniques, correctly identifying all 15 street samples. Additionally, the electrochemical sensor predicted the purity of the tablets with a mean absolute error of 2.3%. Overall, this new, electrochemical detection strategy provides LEAs the rapid, low-cost, on-site detection and quantification of MDMA in suspicious samples, without requiring specialized training.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000977060400001 Publication Date 2023-03-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0026-265x; 0026-265x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.8 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 4.8; 2023 IF: 3.034
Call Number UA @ admin @ c:irua:195415 Serial 8952
Permanent link to this record
 

 
Author (up) Van Echelpoel, R.; Schram, J.; Parrilla, M.; Daems, D.; Slosse, A.; Van Durme, F.; De Wael, K.
Title Electrochemical methods for on-site multidrug detection at festivals Type A1 Journal article
Year 2022 Publication Sensors & Diagnostics Abbreviated Journal
Volume 1 Issue 1 Pages 793-802
Keywords A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Two electrochemical methodologies, i.e. flowchart and dual-sensor, were developed to aid law enforcement present at festivals to obtain a rapid indication of the presence of four illicit drugs in suspicious samples encountered.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2022-06-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record
Impact Factor Times cited Open Access OpenAccess
Notes Approved no
Call Number UA @ admin @ c:irua:188521 Serial 8856
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Author (up) 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.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000663216500001 Publication Date 2021-04-06
Series Editor Series Title Abbreviated Series Title
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
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Author (up) Van Loon, J.; De Jong, M.; De Wael, K.; Du Bois, E.
Title Transposing testing from lab to on-site environment : a case of cocaine powder sampling Type P3 Proceeding
Year 2020 Publication Abbreviated Journal
Volume Issue Pages
Keywords P3 Proceeding; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Product development
Abstract This paper reports on the transition process to convert a specific lab technique to the on-site, real-life environment. Bringing a lab test to an on-site environment involves many difficulties regarding to the context, people skills and environmental support. Within this project, a case about sampling for an electrochemical measurement, was investigated as a basis to reason upon some general conclusions related to the process of transposing lab-tests to an on-site environment. The current lab test was analysed and compared with a focus group discussion with future users. Based on the findings, assumptions for the new sampling technique in the specific case were formulated. New low-tech methods to achieve the sampling were extensively tested and verified. Starting from this chosen case an argumentation was set up to generalise the conclusions, by reasoning on other cases of products that already passed this transition to the field. Based on a comparison, we could discuss that the selected parameters related to impact of the context environment, of the people that should handle the tests, related to the reasons for transposing the technology, and related to the technology that will be transposed to the on-site environment, were of importance of almost all cases and can therefore be considered as context-independent and related to the transfer to on-site testing.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN 978-94-6384-131-3 Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:169896 Serial 6637
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Author (up) Vermeulen, M.; Janssens, K.; Sanyova, J.; Rahemi, V.; McGlinchey, C.; De Wael, K.
Title Assessing the stability of arsenic sulfide pigments and influence of the binding media on their degradation by means of spectroscopic and electrochemical techniques Type A1 Journal article
Year 2018 Publication Microchemical journal Abbreviated Journal Microchem J
Volume 138 Issue 138 Pages 82-91
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract In this paper, we used the semiconducting and lightfastness properties of synthetic and mineral arsenic sulfide pigments to study their stability by means of electrochemical and microfadometric techniques. A combination of these techniques shows that in the early stage of the degradation process, amorphous arsenic sulfides are more stable than both crystalline forms, while upon longer exposure time, amorphous pigments will fade more than both mineral pigments, making it less suitable. While the stability study was carried out on unbound pigments, the influence of the organic binder on the relative degradation of the arsenic sulfide pigments was investigated through a multi-analytical approach on pigment/binder mock-up paint samples. For this purpose, the formation of arsenic trioxide was assessed by micro Fourier transform infrared (μ-FTIR) spectroscopy while the influence of the binder on the formation of sulfates was studied by means of synchrotron radiation X-ray near edge structure (μ-XANES). Both techniques elucidate a higher stability of all pigments in gum arabic while the use of egg yolk as binder leads to the most degradation, most likely due to its sulfur-rich composition. In the context of the degradation of arsenic sulfide pigments, other binders such as animal glue, egg white or linseed oil show an intermediate impact.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000428103000010 Publication Date 2018-01-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0026-265x; 0026-265x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.034 Times cited 4 Open Access
Notes ; This research is made possible with the support of the Belgian Science Policy Office (BELSPO, Brussels) through the research program Science for a Sustainable Development – SDD, “Long-term role and fate of metal-sulfides in painted works of art – S2ART” (grant number SD/RI/04A). We gratefully acknowledge Megane Willems (Institut Paul-Lambin) for her help with mu-FFIR analyses and realization of the mock-up paint samples. We acknowledge the Paul Scherrer Institut, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline Phoenix of the SLS. ; Approved Most recent IF: 3.034
Call Number UA @ admin @ c:irua:150149 Serial 5482
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Author (up) Vermeulen, M.; Sanyova, J.; Janssens, K.; Nuyts, G.; De Meyer, S.; De Wael, K.
Title The darkening of copper- or lead-based pigments explained by a structural modification of natural orpiment : a spectroscopic and electrochemical study Type A1 Journal article
Year 2017 Publication Journal of analytical atomic spectrometry Abbreviated Journal J Anal Atom Spectrom
Volume 32 Issue 7 Pages 1331-1341
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract A combined Raman and electrochemical study of natural orpiment (As2S3), an arsenic sulfide pigment, was used to assess the quick formation of oxidized species such as arsenic oxide (As2O3) upon exposing the pigment to 405 nm or 532 nm monochromatic light while simultaneously recording the Raman spectra of the exposed sample. During this process, a distortion of the main band at 355 cm−1, associated with the stretching of the AsS3/2 pyramids of natural orpiment, was observed as well as an increased intensity of the 359 cm−1 band, corresponding to covalent AsAs bonds in natural orpiment. The distortion was accompanied by an overall decrease of the global Raman signal for natural orpiment, which could be explained by a loss in the crystal structure. The same phenomena were recorded in reference natural orpiment model paint samples stored for a long time together with verdigris (Cu(OH)2·(CH3COO)2·5H2O) and minium (Pb3O4) paints, the latter two appearing darkened on their sides closest to the orpiment sample as well as in several historical samples containing natural orpiment mixed with various blue pigments. By SEM-EDX and XRPD analysis, respectively on loose material and cast thin-sections of model paint samples, the darkening was identified as dark sulfide species such as chalcocite (Cu2S) and galena (PbS), suggesting the release of volatile sulfide or related species by the natural orpiment paint. XANES analyses of paint samples presenting AsAs bond increase indicated the presence of sulfur species most likely identified as organosulfur compounds formed upon the AsAs bond formation and explained the darkening of the Cu- and Pb-based pigments. To the best of our knowledge, this article reports for the first time the light-induced formation of AsAs bonds in natural orpiment used as an artists' pigment and objectively demonstrates the incompatibility between orpiment and (arsenic) sulfide-sensitive pigments.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000404998500007 Publication Date 2017-05-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0267-9477 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.379 Times cited 10 Open Access
Notes ; This research is made possible with the support of the Belgian Science Policy Office (BELSPO, Brussels) through the research program Science for a Sustainable Development – SDD, “Long-term role and fate of metal-sulfides in painted works of art – S2ART” (SD/RI/04A). We gratefully acknowledge Julie Arslanoglu (Conservation and Scientific Research Department at the Metropolitan Museum of Art, New York, USA) for providing us the orpiment, verdigris and minium mock-up samples. We gratefully acknowledge the Paul Scherrer Institut, Villigen, Switzerland and the German Electron Synchrotron (DESY) for provision of synchrotron radiation beamtimes at respectively beamlines of the SLS and Petra III. ; Approved Most recent IF: 3.379
Call Number UA @ admin @ c:irua:144384 Serial 5564
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Author (up) Wuyts, K.; Hofman, J.; van Wittenberghe, S.; Nuyts, G.; De Wael, K.; Samson, R.
Title A new opportunity for biomagnetic monitoring of particulate pollution in an urban environment using tree branches Type A1 Journal article
Year 2018 Publication Atmospheric environment : an international journal Abbreviated Journal Atmos Environ
Volume 190 Issue 190 Pages 177-187
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract Environmental magnetism, and the magnetic leaf signal in particular, is amply investigated and applied as proxy for atmospheric particulate matter pollution. In this study, we investigated the magnetic signal of annual segments of tree branches, and the composition of particles deposited hereon. Branches are, contrary to leaves of deciduous trees, available during leaf-off seasons and exposed to air pollution year-round. We examined the intra- and inter-tree variation in saturation isothermal remanent magnetization (SIRM) of branch internodes of London plane (Platanus x aeerifolia Willd.) trees in an urban environment. The branch SIRM, normalized by surface area, ranged from 18 to 650 x 10(-6) angstrom; the median amounted to 106 x 10(-6) angstrom. Most of the branch magnetic signal was attributed to the epidermis or bark, and the presence of metal-containing particles on the branch surfaces was confirmed by SEM-EDX. The location of the trees and the height, the depth in the crown and the age of the branches significantly influenced the branch SIRM. The median branch SIRM was up to 135% higher near a busy ring road than in quiet environments (city park and quiet street canyon), and was linked to the presence of Fe-rich particles with co-occurrence of trace metals such as Cr, Cu, Zn and Mn on the branch surface. Within the tree crowns, the branch SIRM generally decreased with increasing height, and was 22% higher in the interior than at the periphery of the crowns. Within the branches, the SIRM increased with each year of exposure, but did not relate to year-to-year variation in particle concentrations due to branch surface changes (epidermis shedding). Our results provide indications that branches can be a valuable alternative for biomagnetic monitoring of particulate pollution, but intra-tree variability in branch SIRM can be substantial due to the branch's location in the tree and branch age.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000444659400017 Publication Date 2018-07-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1352-2310 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.629 Times cited 3 Open Access
Notes ; We would like to thank the city council services of the city of Antwerp for their logistical support. We are grateful to Ana Castanheiro and Leen Van Ham for laboratory and SEM assistance. JH is supported as postdoctoral fellow of the Research Foundation Flanders (FWO; 12I4816N) and SVW is supported by a Marie Sklodowska-Curie Individual Fellowship under the grant agreement no 701815 FLUOPHOT. ; Approved Most recent IF: 3.629
Call Number UA @ admin @ c:irua:153607 Serial 5454
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Author (up) 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.
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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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000758012900020 Publication Date 2021-11-05
Series Editor Series Title Abbreviated Series Title
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
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