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- Title
Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO<sub>2</sub> to methane.
- Authors
Li, Xing-Yi; Zhu, Ze-Lin; Dagnaw, Fentahun Wondu; Yu, Jie-Rong; Wu, Zhi-Xing; Chen, Yi-Jing; Zhou, Mu-Han; Wang, Tieyu; Tong, Qing-Xiao; Jian, Jing-Xin
- 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. Solar-driven CO2 conversion to produce solar fuels is an attractive way to harness solar energy and reduce carbon emissions. Here, the authors report two osmium complexes as highly active and selective CO2 reduction catalysts for selective CO2-to-methane conversion on Si-based photocathodes.
- Subjects
PHOTOELECTROCHEMISTRY; OSMIUM; METHANE; PHOTOELECTROCHEMICAL cells; DENSITY functional theory; PHOTOCATHODES; METHANE as fuel; CARBON emissions; SOLAR energy
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-50244-w