Selective CO2 reduction to acetate via controlled sp2/sp3 carbon hybridization

Chujun Wang, Gong Zhang, Ran Luo, Yixian Wang, Xiao Ma, Mengmeng Zhang, Xin Chang, Zhi-Jian Zhao (), Tuo Wang () and Jinlong Gong ()
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Chujun Wang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Gong Zhang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Ran Luo: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Yixian Wang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Xiao Ma: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Mengmeng Zhang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Xin Chang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Zhi-Jian Zhao: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Tuo Wang: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education
Jinlong Gong: Tianjin University, School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Electrocatalytic reduction of CO2 to fuels and chemicals represents a promising pathway for CO2 utilization and energy conversion. However, metal-based catalysts often suffer from diminished selectivity in the direct reduction of CO2 to acetate due to suboptimal intermediate adsorption energy imposed by the linear scaling relationship of d-band theory. We describe a deposition-etching strategy that tunes the sp2/sp3 hybridization of carbon in diamond to tune the adsorption equilibrium of intermediates for CO2 reduction to acetate, which circumvents the constraints of the d-band electrons. This metal-free catalyst achieves a Faradaic efficiency of 62.7% for CO2-to-acetate conversion and demonstrated 100 hours durability. Mechanistic studies reveal that introducing sp2-carbons into the sp3-carbon matrix can control the adsorption energies of *CO2 and *CO. The sp2/sp3-carbon active sites facilitate the formation of the *CHO intermediate, which is asymmetrically coupled with the *COL to generate acetate.

Date: 2025
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DOI: 10.1038/s41467-025-65504-6

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