Complexed Semiconductor Cores Activate Hexaniobate Ligands as Nucleophilic Sites for Solar-Light Reduction of CO2 by Water

Guanyun Zhang, Fei Wang, Tal Tubul, Mark Baranov, Nitai Leffler, Alevtina Neyman, Josep M. Poblet, Ira A. Weinstock

Research output: Contribution to journalArticlepeer-review

16 Scopus citations

Abstract

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-NiII-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 NbV to NbIV, increasing electron density at bridging oxo atoms of Nb-μ-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.

Original languageEnglish
Article numbere202213162
JournalAngewandte Chemie - International Edition
Volume61
Issue number49
DOIs
StatePublished - 5 Dec 2022

Keywords

  • CO Reduction
  • Hexaniobate Anion
  • Molecular Complex
  • Nickel Oxide
  • Photocatalysis

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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