Visible-light-driven CO2 reduction on a hybrid photocatalyst consisting of a Ru(ii) binuclear complex and a Ag-loaded TaON in aqueous solutions

Chemical Science
Akinobu NakadaOsamu Ishitani

Abstract

A hybrid photocatalyst consisting of a Ru(ii) binuclear complex and a Ag-loaded TaON reduced CO2 by visible light even in aqueous solution. The distribution of the reduction products was strongly affected by the pH of the reaction solution. HCOOH was selectively produced in neutral conditions, whereas the formation of HCOOH competed with H2 evolution in acidic conditions. Detailed mechanistic studies revealed that the photocatalytic CO2 reduction proceeded via 'Z-schematic' electron transfer with step-by-step photoexcitation of TaON and the photosensitizer unit in the Ru(ii) binuclear complex. The maximum turnover number for HCOOH formation was 750 based on the Ru(ii) binuclear complex under visible-light irradiation, and the optimum external quantum efficiency of the HCOOH formation was 0.48% using 400 nm monochromic light with ethylenediaminetetraacetic acid disodium salt as a sacrificial reductant. Even in aqueous solution, the hybrid could also convert visible-light energy into chemical energy (ΔG0 = +83 kJ mol-1) by the reduction of CO2 to HCOOH with methanol oxidation.

References

Apr 4, 2007·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Shunsuke SatoOsamu Ishitani
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Sep 21, 2013·Chemical Communications : Chem Comm·Kazuhiko MaedaOsamu Ishitani
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Apr 29, 2015·Proceedings of the National Academy of Sciences of the United States of America·Leila AlibabaeiThomas J Meyer

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Citations

Sep 13, 2019·Chemical Communications : Chem Comm·Lang PeiZhigang Zou
Mar 11, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Yoshiyuki AsaiYasuomi Yamazaki
May 29, 2018·Chemical Communications : Chem Comm·Seán Hennessey, Pau Farràs
Nov 23, 2017·Chemical Science·Alejandro CadranelDirk M Guldi
Nov 29, 2016·Chemical Communications : Chem Comm·Gaia NeriAlexander J Cowan
Dec 5, 2017·Advanced Science·Jinghua WuYanguang Li
May 21, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Xing ZhuHisao Yoshida
Feb 15, 2019·Chemical Reviews·Xin LiXiaobo Chen
Oct 5, 2016·ACS Applied Materials & Interfaces·Yongchao HuangYexiang Tong
May 4, 2017·Journal of the American Chemical Society·Moritz F KuehnelErwin Reisner

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Methods Mentioned

BETA
X-ray
surface plasmon resonance
electrophoresis

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