Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO2 to methane

Xing-Yi Li, Ze-Lin Zhu, Fentahun Wondu Dagnaw, Jie-Rong Yu, Zhi-Xing Wu, Yi-Jing Chen, Mu-Han Zhou, Tieyu Wang, Qing-Xiao Tong () and Jing-Xin Jian ()
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Xing-Yi Li: Shantou University
Ze-Lin Zhu: City University of Hong Kong
Fentahun Wondu Dagnaw: Shantou University
Jie-Rong Yu: Shantou University
Zhi-Xing Wu: Linköping University
Yi-Jing Chen: Shantou University
Mu-Han Zhou: Shantou University
Tieyu Wang: Shantou University
Qing-Xiao Tong: Shantou University
Jing-Xin Jian: Shantou University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Solar-driven CO2 reduction to yield high-value chemicals presents an appealing avenue for combating climate change, yet achieving selective production of specific products remains a significant challenge. We showcase two osmium complexes, przpOs, and trzpOs, as CO2 reduction catalysts for selective CO2-to-methane conversion. Kinetically, the przpOs and trzpOs exhibit high CO2 reduction catalytic rate constants of 0.544 and 6.41 s−1, respectively. Under AM1.5 G irradiation, the optimal Si/TiO2/trzpOs have CH4 as the main product and >90% Faradaic efficiency, reaching −14.11 mA cm−2 photocurrent density at 0.0 VRHE. Density functional theory calculations reveal that the N atoms on the bipyrazole and triazole ligands effectively stabilize the CO2-adduct intermediates, which tend to be further hydrogenated to produce CH4, leading to their ultrahigh CO2-to-CH4 selectivity. These results are comparable to cutting-edge Si-based photocathodes for CO2 reduction, revealing a vast research potential in employing molecular catalysts for the photoelectrochemical conversion of CO2 to methane.

Date: 2024
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DOI: 10.1038/s41467-024-50244-w

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