Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO 2 to methane.

Autor: Li XY; Department of Chemistry, Shantou University, Shantou, 515063, PR China.; Guangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou University, Shantou, 515063, PR China., Zhu ZL; Center of Super-Diamond and Advanced Films (COSDAF) and Department of Chemistry, City University of Hong Kong, Hong Kong SAR, PR China., Dagnaw FW; Department of Chemistry, Shantou University, Shantou, 515063, PR China., Yu JR; Department of Chemistry, Shantou University, Shantou, 515063, PR China., Wu ZX; Laboratory of Organic Electronics, Department of Science and Technology (ITN), Linköping University, Norrköping, SE, 60174, Sweden., Chen YJ; Department of Chemistry, Shantou University, Shantou, 515063, PR China., Zhou MH; Department of Chemistry, Shantou University, Shantou, 515063, PR China., Wang T; Guangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou University, Shantou, 515063, PR China., Tong QX; Department of Chemistry, Shantou University, Shantou, 515063, PR China. qxtong@stu.edu.cn.; Key Laboratory for Preparation and Application of Ordered Structural Material of Guangdong Province, Shantou University, Shantou, 515063, PR China. qxtong@stu.edu.cn., Jian JX; Department of Chemistry, Shantou University, Shantou, 515063, PR China. jxjian@stu.edu.cn.; Guangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou University, Shantou, 515063, PR China. jxjian@stu.edu.cn.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Jul 13; Vol. 15 (1), pp. 5882. Date of Electronic Publication: 2024 Jul 13.
DOI: 10.1038/s41467-024-50244-w
Abstrakt: Solar-driven CO 2 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 CO 2 reduction catalysts for selective CO 2 -to-methane conversion. Kinetically, the przpOs and trzpOs exhibit high CO 2 reduction catalytic rate constants of 0.544 and 6.41 s -1 , respectively. Under AM1.5 G irradiation, the optimal Si/TiO 2 /trzpOs have CH 4 as the main product and >90% Faradaic efficiency, reaching -14.11 mA cm -2 photocurrent density at 0.0 V RHE . Density functional theory calculations reveal that the N atoms on the bipyrazole and triazole ligands effectively stabilize the CO 2 -adduct intermediates, which tend to be further hydrogenated to produce CH 4 , leading to their ultrahigh CO 2 -to-CH 4 selectivity. These results are comparable to cutting-edge Si-based photocathodes for CO 2 reduction, revealing a vast research potential in employing molecular catalysts for the photoelectrochemical conversion of CO 2 to methane.
(© 2024. The Author(s).)
Databáze: MEDLINE
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