Structural evolution and strain generation of derived-Cu catalysts during CO2 electroreduction

Qiong Lei, Liang Huang, Jun Yin (), Bambar Davaasuren, Youyou Yuan, Xinglong Dong, Zhi-Peng Wu, Xiaoqian Wang, Ke Xin Yao, Xu Lu () and Yu Han ()
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Qiong Lei: King Abdullah University of Science and Technology (KAUST)
Liang Huang: Clean Combustion Research Center, KAUST
Jun Yin: King Abdullah University of Science and Technology (KAUST)
Bambar Davaasuren: Imaging and Characterization Core Lab, KAUST
Youyou Yuan: Imaging and Characterization Core Lab, KAUST
Xinglong Dong: King Abdullah University of Science and Technology (KAUST)
Zhi-Peng Wu: King Abdullah University of Science and Technology (KAUST)
Xiaoqian Wang: King Abdullah University of Science and Technology (KAUST)
Ke Xin Yao: Chongqing University
Xu Lu: Clean Combustion Research Center, KAUST
Yu Han: King Abdullah University of Science and Technology (KAUST)

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Copper (Cu)-based catalysts generally exhibit high C2+ selectivity during the electrochemical CO2 reduction reaction (CO2RR). However, the origin of this selectivity and the influence of catalyst precursors on it are not fully understood. We combine operando X-ray diffraction and operando Raman spectroscopy to monitor the structural and compositional evolution of three Cu precursors during the CO2RR. The results indicate that despite different kinetics, all three precursors are completely reduced to Cu(0) with similar grain sizes (~11 nm), and that oxidized Cu species are not involved in the CO2RR. Furthermore, Cu(OH)2- and Cu2(OH)2CO3-derived Cu exhibit considerable tensile strain (0.43%~0.55%), whereas CuO-derived Cu does not. Theoretical calculations suggest that the tensile strain in Cu lattice is conducive to promoting CO2RR, which is consistent with experimental observations. The high CO2RR performance of some derived Cu catalysts is attributed to the combined effect of the small grain size and lattice strain, both originating from the in situ electroreduction of precursors. These findings establish correlations between Cu precursors, lattice strains, and catalytic behaviors, demonstrating the unique ability of operando characterization in studying electrochemical processes.

Date: 2022
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DOI: 10.1038/s41467-022-32601-9

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