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Ren, Peng ; Zhang, Tong ; Jain, Noopur ; Ching, H. Y. Vincent ; Jaworski, Aleksander ; Barcaro, Giovanni ; Monti, Susanna ; Silvestre-Albero, Joaquin ; Celorrio, Veronica ; Chouhan, Lata ; Rokicińska, Anna ; Debroye, Elke ; Kuśtrowski, Piotr ; Van Doorslaer, Sabine ; Van Aert, Sandra ; Bals, Sara ; Das, Shoubhik:
An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR).
In: Journal of the American Chemical Society.
Bd. 145
(2023)
Heft 30
.
- S. 16584-16596.
ISSN 1520-5126
DOI: https://doi.org/10.1021/jacs.3c03785
Abstract
In this work, we have fabricated an aryl amino-substituted graphitic carbon nitride (g-C3N4) catalyst with atomically dispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibited excellent reactivity, obtaining up to 2230 μM H2O2 in 7 h from alkaline water and up to 1800 μM from seawater under identical conditions. More importantly, the catalyst was quickly recovered for subsequent reuse without appreciable loss in performance. Interestingly, unlike the usual two-electron oxygen reduction 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 processes occurred; 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), and H2O2 was formed indirectly by the combination of two •OH. We have characterized the material, at the catalytic sites, at the atomic level using electron paramagnetic resonance, X-ray absorption near edge structure, extended X-ray absorption fine structure, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, magic-angle spinning solid-state NMR spectroscopy, and multiscale molecular modeling, combining classical reactive molecular dynamics simulations and quantum chemistry calculations.
Weitere Angaben
| Publikationsform: | Artikel in einer Zeitschrift |
|---|---|
| Begutachteter Beitrag: | Ja |
| 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: | 30 Aug 2023 06:30 |
| Letzte Änderung: | 08 Nov 2023 11:23 |
| URI: | https://eref.uni-bayreuth.de/id/eprint/86713 |