期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 49, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202213162
关键词
CO2 Reduction; Hexaniobate Anion; Molecular Complex; Nickel Oxide; Photocatalysis
资金
- Israel Science Foundation [280/21]
- PBC-Israel
- Spanish Ministry of Science and Innovation [PID2020-112762GB-I00]
- European Union [713679]
- Universitat Rovira i Virgili (URV)
This study demonstrates the use of molecular complexation as a method to utilize electron-dense polyoxoniobate anions as nucleophilic photocatalysts for solar-light driven activation and reduction of small molecules.
Although pure and functionalized solid-state polyniobates such as layered perovskites and niobate nanosheets are photocatalysts for renewable-energy processes, analogous reactions by molecular polyoxoniobate cluster-anions are nearly absent from the literature. We now report that under simulated solar light, hexaniobate cluster-anion encapsulated 30-Ni-II-ion fragments of surface-protonated cubic-phase-like NiO cores activate the hexaniobate ligands towards CO2 reduction by water. Photoexcitation of the NiO cores promotes charge-transfer reduction of Nb-V to Nb-IV, increasing electron density at bridging oxo atoms of Nb-mu-O-Nb linkages that bind and convert CO2 to CO. Photogenerated NiO holes simultaneously oxidize water to dioxygen. The findings point to molecular complexation of suitable semiconductor fragments as a general method for utilizing electron-dense polyoxoniobate anions as nucleophilic photocatalysts for solar-light driven activation and reduction of small molecules.
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