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Structural evolution and strain generation of derived-Cu catalysts during CO(2) electroreduction

Copper (Cu)-based catalysts generally exhibit high C(2+) selectivity during the electrochemical CO(2) reduction reaction (CO(2)RR). 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 Rama...

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Detalles Bibliográficos
Autores principales: Lei, Qiong, Huang, Liang, Yin, Jun, Davaasuren, Bambar, Yuan, Youyou, Dong, Xinglong, Wu, Zhi-Peng, Wang, Xiaoqian, Yao, Ke Xin, Lu, Xu, Han, Yu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9388520/
https://www.ncbi.nlm.nih.gov/pubmed/35982055
http://dx.doi.org/10.1038/s41467-022-32601-9
Descripción
Sumario:Copper (Cu)-based catalysts generally exhibit high C(2+) selectivity during the electrochemical CO(2) reduction reaction (CO(2)RR). 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 CO(2)RR. 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 CO(2)RR. Furthermore, Cu(OH)(2)- and Cu(2)(OH)(2)CO(3)-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 CO(2)RR, which is consistent with experimental observations. The high CO(2)RR 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.