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Author |
Pauwels, D.; Ching, H.Y.V.; Samanipour, M.; Neukermans, S.; Hereijgers, J.; Van Doorslaer, S.; De Wael, K.; Breugelmans, T. |
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Title |
Identifying intermediates in the reductive intramolecular cyclisation of allyl 2-bromobenzyl ether by an improved electron paramagnetic resonance spectroelectrochemical electrode design combined with density functional theory calculations |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Electrochimica acta |
Abbreviated Journal |
Electrochim Acta |
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Volume |
271 |
Issue |
271 |
Pages |
10-18 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
The electrochemical activation of C-X bonds requires very negative electrode potentials. Lowering the overpotentials and increasing the catalytic activity requires intensive electrocatalytic research. A profound understanding of the reaction mechanism and the influence of the electrocatalyst allows optimal tuning of the electrocatalyst. This can be achieved by combining electrochemical techniques with electron paramagnetic resonance (EPR) spectroscopy. Although this was introduced in the mid-twentieth century, the application of this combined approach in electrocatalytic research is underexploited. Several reasons can be listed, such as the limited availability of EPR instrumentation and electrochemical devices for such in situ experiments. In this work, a simple and inexpensive construction adapted for in situ EPR electrocatalytic research is proposed. The proof of concept is provided by studying a model reaction, namely the reductive cyclisation of allyl 2-bromobenzyl ether which has interesting industrial applications. |
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Wos |
000430369800002 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2018-03-20 |
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Edition |
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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 |
4.798 |
Times cited |
2 |
Open Access |
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Notes |
; The authors would like to thank Melissa Van Landeghem for her assistance with the experimental work and analysis of the data. Jonas Hereijgers greatly acknowledges the Research Foundation Flanders (FWO) for support through a Post-Doctoral grant (12Q8817N). H.Y. Vincent Ching gratefully acknowledges the University of Antwerp for a Post-Doctoral grant. Sabine Van Doorslaer and Tom Breugelmans acknowledge the FWO for research funding (research grant G093317N). ; |
Approved |
Most recent IF: 4.798 |
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Call Number |
UA @ admin @ c:irua:150463 |
Serial |
5652 |
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Permanent link to this record |
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Author |
Van Dijck, J.G.; Mampuys, P.; Ching, H.Y.V.; Krishnan, D.; Baert, K.; Hauffman, T.; Verbeeck, J.; Van Doorslaer, S.; Maes, B.U.W.; Dorbec, M.; Buekenhoudt, A.; Meynen, V. |
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Title |
Synthesis – properties correlation and the unexpected role of the titania support on the Grignard surface modification |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Applied Surface Science |
Abbreviated Journal |
Appl Surf Sci |
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Volume |
527 |
Issue |
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Pages |
146851-17 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Organic synthesis (ORSY); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
While the impact of reaction conditions on surface modification with Grignard reactants has been studied for silica supports, such information is absent for metal oxides like titania. Differences between modified titania and silica are observed, making it paramount to explore the reaction mechanism. A detailed study on the impact of the reaction conditions is reported, with a focus on the chain length of the alkyl Grignard reactant, its concentration, the reaction time and temperature, and the type of titania support. While the increase in the chain length reduces the amount of organic groups on the surface, the concentration, time and temperature show little/no influence on the modification degree. However, the type of titania support used and the percentage of amorphous phase present has a significant impact on the amount of grafted groups. Even though the temperature and concentration show no clear impact on the modification degree, they can cause changes in the surface hydroxyl population, which are thus not linked to the modification degree. Furthermore, the titania support is reduced during functionalization. This reduction dependents on the reaction temperature, the titania support and the chain length of the Grignard reactant. Similarly, this reduction is not linked to the modification degree. |
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Wos |
000564205300003 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2020-06-03 |
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Edition |
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ISSN |
0169-4332 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.7 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
; The FWO (Fonds Wetenschappelijk Onderzoek) is gratefully acknowledged for the VITO-FWO grant of fellow Jeroen G. Van Dijck (11W9416N) and the financial support granted in project GO12712N. The E.U. is acknowledged for H.Y. Vincent Ching's H2020-MSCA-IF (grant number 792946, iSPY). Dileep Krishnan and Johan Verbeeck acknowledge funding from GOA project “solarpaint” of the University of Antwerp. ; |
Approved |
Most recent IF: 6.7; 2020 IF: 3.387 |
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Call Number |
UA @ admin @ c:irua:169722 |
Serial |
6712 |
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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 |
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Year |
2021 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
11 |
Issue |
22 |
Pages |
14087-14101 |
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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) |
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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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Wos |
000758012900020 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2021-11-05 |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 10.614 |
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Call Number |
UA @ admin @ c:irua:187276 |
Serial |
7534 |
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Author |
Thiruvottriyur Shanmugam, S.; Van Echelpoel, R.; Boeye, G.; Eliaerts, J.; Samanipour, M.; Ching, H.Y.V.; Florea, A.; Van Doorslaer, S.; Van Durme, F.; Samyn, N.; Parrilla, M.; De Wael, K. |
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Title |
Towards developing a screening strategy for ecstasy : revealing the electrochemical profile |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemelectrochem |
Abbreviated Journal |
Chemelectrochem |
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Volume |
8 |
Issue |
24 |
Pages |
4826-4834 |
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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) |
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Abstract |
This article describes the development of an electrochemical screening strategy for 3,4-methylenedioxymethamphetamine (MDMA), the regular psychoactive compound in ecstasy (XTC) pills. We have investigated the specific electrochemical profile of MDMA and its electro-oxidation mechanisms at disposable graphite screen-printed electrodes. We have proved that the formation of a radical cation and subsequent reactions are indeed responsible for the electrode surface passivation, as evidenced by using electron paramagnetic resonance spectroscopy and electrochemistry. Thereafter, pure cutting agents and MDMA as well as simulated binary mixtures of compounds with MDMA were subjected to square wave voltammetry at pH 7 to understand the characteristic electrochemical profile. An additional measurement at pH 12 was able to resolve false positives and negatives occurring at pH 7. Finally, validation of the screening strategy was done by measuring a set of ecstasy street samples. Overall, our proposed electrochemical screening strategy has been demonstrated for the rapid, sensitive, and selective detection of MDMA, resolving most of the false positives and negatives given by the traditional Marquis color tests, thus exhibiting remarkable promises for the on-site screening of MDMA. |
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000735883700020 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2021-12-22 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
2196-0216 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.136 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 4.136 |
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Call Number |
UA @ admin @ c:irua:184371 |
Serial |
8680 |
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Permanent link to this record |
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Author |
Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S. |
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Title |
Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS Sustainable Chemistry and Engineering |
Abbreviated Journal |
Acs Sustain Chem Eng |
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Volume |
10 |
Issue |
1 |
Pages |
530-540 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY) |
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Abstract |
Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free
heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental
evidence. |
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Wos |
000736518000001 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2022-01-10 |
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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 |
2168-0485 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.4 |
Times cited |
24 |
Open Access |
OpenAccess |
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Notes |
We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. |
Approved |
Most recent IF: 8.4 |
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Call Number |
EMAT @ emat @c:irua:184744 |
Serial |
6900 |
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Permanent link to this record |
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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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Wos |
000786254500002 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2022-03-22 |
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Abbreviated Series Title |
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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:187522 |
Serial |
7141 |
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Permanent link to this record |
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Author |
Ren, P.; Zhang, T.; Jain, N.; Ching, H.Y.V.; Jaworski, A.; Barcaro, G.; Monti, S.; Silvestre-Albero, J.; Celorrio, V.; Chouhan, L.; Rokicinska, A.; Debroye, E.; Kustrowski, P.; Van Doorslaer, S.; Van Aert, S.; Bals, S.; Das, S. |
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Title |
An atomically dispersed Mn-photocatalyst for generating hydrogen peroxide from seawater via the Water Oxidation Reaction (WOR) |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
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Volume |
145 |
Issue |
30 |
Pages |
16584-16596 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY); Theory and Spectroscopy of Molecules and Materials (TSM²) |
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Abstract |
In this work, we have fabricatedan aryl amino-substitutedgraphiticcarbon nitride (g-C3N4) catalyst with atomicallydispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibitedexcellent reactivity, obtaining up to 2230 & mu;M H2O2 in 7 h from alkaline water and up to 1800 & mu;Mfrom seawater under identical conditions. More importantly, the catalystwas quickly recovered for subsequent reuse without appreciable lossin performance. Interestingly, unlike the usual two-electron oxygenreduction reaction pathway, the generation of H2O2 was through a less common two-electron water oxidation reaction(WOR) process in which both the direct and indirect WOR processesoccurred; namely, photoinduced h(+) directly oxidized H2O to H2O2 via a one-step 2e(-) WOR, and photoinduced h(+) first oxidized a hydroxide (OH-) ion to generate a hydroxy radical ((OH)-O-& BULL;), and H2O2 was formed indirectly by thecombination of two (OH)-O-& BULL;. We have characterized thematerial, at the catalytic sites, at the atomic level using electronparamagnetic resonance, X-ray absorption near edge structure, extendedX-ray absorption fine structure, high-resolution transmission electronmicroscopy, X-ray photoelectron spectroscopy, magic-angle spinningsolid-state NMR spectroscopy, and multiscale molecular modeling, combiningclassical reactive molecular dynamics simulations and quantum chemistrycalculations. |
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Wos |
001034983300001 |
Publication Date ![sorted by Publication Date field, ascending order (up)](img/sort_asc.gif) |
2023-07-24 |
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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 |
21 |
Open Access |
Not_Open_Access |
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Notes |
S.D. thanks the IOF grant and Francqui start up grant from the University of Antwerp, Belgium, for the financial support. P.R. thanks CSC and T.Z. thanks FWO for their financial assistance to finish this work. E.D. would like to thank the KU Leuven Research Fund for financial support through STG/21/010. J.S.A. acknowledges financial support from MCIN/AEI/10.13039/501100011033 and EU NextGeneration/PRTR (Project PCI2020-111968/3D-Photocat) and Diamond Synchrotron (rapid access proposal SP32609). This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). S.B. and S.V.A. acknowledge financial support from the Research Foundation Flanders (FWO, Belgium, project G.0346.21 N). We also thank Mr. Jian Zhu and Mr. Shahid Ullah Khan from the University of Antwerp, Belgium, for helpful discussions. |
Approved |
Most recent IF: 15; 2023 IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:198426 |
Serial |
8831 |
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Permanent link to this record |