Electroreduction of CO2 to methane with triazole molecular catalysts

Zhanyou Xu, Ruihu Lu, Zih-Yi Lin, Weixing Wu, Hsin-Jung Tsai, Qian Lu, Yuguang C. Li, Sung-Fu Hung (), Chunshan Song, Jimmy C. Yu, Ziyun Wang () and Ying Wang ()
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Zhanyou Xu: Hong Kong S. A. R.
Ruihu Lu: University of Auckland
Zih-Yi Lin: National Yang Ming Chiao Tung University
Weixing Wu: Hong Kong S. A. R.
Hsin-Jung Tsai: National Yang Ming Chiao Tung University
Qian Lu: Hong Kong S. A. R.
Yuguang C. Li: The State University of New York
Sung-Fu Hung: National Yang Ming Chiao Tung University
Chunshan Song: Hong Kong S. A. R.
Jimmy C. Yu: Hong Kong S. A. R.
Ziyun Wang: University of Auckland
Ying Wang: Hong Kong S. A. R.

Nature Energy, 2024, vol. 9, issue 11, 1397-1406

Abstract: Abstract The electrochemical CO2 reduction reaction towards value-added fuel and feedstocks often relies on metal-based catalysts. Organic molecular catalysts, which are more acutely tunable than metal catalysts, are still unable to catalyse CO2 to hydrocarbons under industrially relevant current densities for long-term operation, and the catalytic mechanism is still elusive. Here we report 3,5-diamino-1,2,4-triazole-based membrane electrode assemblies for CO2-to-CH4 conversion with Faradaic efficiency of (52 ± 4)% and turnover frequency of 23,060 h−1 at 250 mA cm−2. Our mechanistic studies suggest that the CO2 reduction at the 3,5-diamino-1,2,4-triazole electrode proceeds through the intermediary *CO2–*COOH–*C(OH)2–*COH to produce CH4 due to the spatially distributed active sites and the suitable energy level of the molecular orbitals. A pilot system operated under a total current of 10 A (current density = 123 mA cm−2) for 10 h is able to produce CH4 at a rate of 23.0 mmol h−1.

Date: 2024
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DOI: 10.1038/s41560-024-01645-0

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