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Zhang, Tong ; Schilling, Waldemar ; Khan, Shahid Ullah ; Ching, H. Y. Vincent ; Lu, Can ; Chen, Jianhong ; Jaworski, Aleksander ; Barcaro, Giovanni ; Monti, Susanna ; De Wael, Karolien ; Slabon, Adam ; Das, Shoubhik:
Atomic-Level Understanding for the Enhanced Generation of Hydrogen Peroxide by the Introduction of an Aryl Amino Group in Polymeric Carbon Nitrides.
In: ACS Catalysis.
Bd. 11
(2021)
Heft 22
.
- S. 14087-14101.
ISSN 2155-5435
DOI: https://doi.org/10.1021/acscatal.1c03733
Abstract
Heterogeneous catalysts are often “black boxes” 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–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·h–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, −NH2 terminal groups, and difluoromethylene units, reactants, and products.
Weitere Angaben
| Publikationsform: | Artikel in einer Zeitschrift |
|---|---|
| Begutachteter Beitrag: | Ja |
| Keywords: | atomic-level characterizations; hydrogen peroxide; aryl amino PCNs; 15N and 19F solid-state NMR spectroscopy; O2 reduction |
| Institutionen der Universität: | Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie Fakultäten Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie > Lehrstuhl Organische Chemie I > Lehrstuhl Organische Chemie I - Univ.-Prof. Dr. Das Shoubhik Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie > Lehrstuhl Organische Chemie I |
| Titel an der UBT entstanden: | Nein |
| Themengebiete aus DDC: | 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Eingestellt am: | 18 Jul 2023 11:45 |
| Letzte Änderung: | 08 Nov 2023 11:23 |
| URI: | https://eref.uni-bayreuth.de/id/eprint/86166 |