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Identification of Cu(100)/Cu(111) Interfaces as Superior Active Sites for CO Dimerization During CO 2 Electroreduction

2021; American Chemical Society; Volume: 144; Issue: 1 Linguagem: Inglês

10.1021/jacs.1c09508

1943-2984

Zhi‐Zheng Wu, Xiaolong Zhang, Zhuang‐Zhuang Niu, Fei‐Yue Gao, Peng‐Peng Yang, Li‐Ping Chi, Lei Shi, Wensen Wei, Ren Liu, Zhi Chen, Shao‐Jin Hu, Xiao Zheng, Min‐Rui Gao,

Electrochemical Analysis and Applications

The electrosynthesis of valuable multicarbon chemicals using carbon dioxide (CO2) as a feedstock has substantially progressed recently but still faces considerable challenges. A major difficulty lines in the sluggish kinetics of forming carbon-carbon (C-C) bonds, especially in neutral media. We report here that oxide-derived copper crystals enclosed by six {100} and eight {111} facets can reduce CO2 to multicarbon products with a high Faradaic efficiency of 74.9 ± 1.7% at a commercially relevant current density of 300 mA cm-2 in 1 M KHCO3 (pH ∼ 8.4). By combining the experimental and computational studies, we uncovered that Cu(100)/Cu(111) interfaces offer a favorable local electronic structure that enhances *CO adsorption and lowers C-C coupling activation energy barriers, performing superior to Cu(100) and Cu(111) surfaces, respectively. On this catalyst, no obvious degradation was observed at 300 mA cm-2 over 50 h of continuous operation.