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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...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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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 |
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. |
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