A Molecular Z-Scheme Artificial Photosynthetic System Under the Bias-Free Condition for CO 2 Reduction Coupled with Two-electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H 2 O 2 .

Autor: Kuttassery F; Department of Chemistry, University of Calicut, Malappuram, Kerala, 673635, India., Ohsaki Y; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan., Thomas A; Department of Chemistry, St. Stephen's College, Uzhavoor, Kerala, 686634, India., Kamata R; Department of Chemistry, Tokyo Institute of Technology, 2-12-1-NE-1 O-okayama, Meguro, Tokyo, 152-8550, Japan., Ebato Y; Department of Chemistry, Tokyo Institute of Technology, 2-12-1-NE-1 O-okayama, Meguro, Tokyo, 152-8550, Japan., Kumagai H; Research Center for Advanced Science and Technology, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8904, Japan., Nakazato R; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan., Sebastian A; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan., Mathew S; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan., Tachibana H; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan., Ishitani O; Department of Chemistry, Tokyo Institute of Technology, 2-12-1-NE-1 O-okayama, Meguro, Tokyo, 152-8550, Japan.; Department of Chemistry, Graduate School of Advanced Science and Engineering, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima, Hiroshima, 739-8526, Japan., Inoue H; Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397, Japan.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2023 Oct 02; Vol. 62 (40), pp. e202308956. Date of Electronic Publication: 2023 Aug 24.
DOI: 10.1002/anie.202308956
Abstrakt: Bio-inspired molecular-engineered systems have been extensively investigated for the half-reactions of H 2 O oxidation or CO 2 reduction with sacrificial electron donors/acceptors. However, there has yet to be reported a device for dye-sensitized molecular photoanodes coupled with molecular photocathodes in an aqueous solution without the use of sacrificial reagents. Herein, we will report the integration of Sn IV - or Al III -tetrapyridylporphyrin (SnTPyP or AlTPyP) decorated tin oxide particles (SnTPyP/SnO 2 or AlTPyP/SnO 2 ) photoanode with the dye-sensitized molecular photocathode on nickel oxide particles containing [Ru(diimine) 3 ] 2+ as the light-harvesting unit and [Ru(diimine)(CO) 2 Cl 2 ] as the catalyst unit covalently connected and fixed within poly-pyrrole layer (RuCAT-RuC 2 -PolyPyr-PRu/NiO). The simultaneous irradiation of the two photoelectrodes with visible light resulted in H 2 O 2 on the anode and CO, HCOOH, and H 2 on the cathode with high Faradaic efficiencies in purely aqueous conditions without any applied bias is the first example of artificial photosynthesis with only two-electron redox reactions.
(© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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