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Engineering vacancy and hydrophobicity of spherical coral-like CuO catalyst for effective electrochemical CO2 reduction to ethylene

Journal 2023 · IF 6.2 · 发表于 2023 年 4 月 5 日
作者: Tianbo Jia,Linlin Wang,Lina Zhang,Zhouhao Zhu,Kun Zhang,Baikang Zhu,Xin Li,Chunyang Zhai,Shunli Li,Yingtang Zhou,Hengcong Tao
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摘要

Electrochemical carbon dioxide reduction (ECR) to ethylene by using renewable energy is a viable way to tackle the global climate change, and beneficial to facilitate closing the carbon cycle . Herein, a sulfur-doped spherical coral-like CuO (S-CuO) catalyst was facile synthesized, which is enabling efficient conversion CO 2 -to-C 2 H 4 . The obtained 5% S-CuO can reach the Faradaic efficiency (C 2 H 4 ) of 48.4% with a current density of 15 mA cm −2 at -1.3 V vs. RHE, which maintained stability over 20 h in 0.1 M KHCO 3 electrolyte. XPS , SEM, TEM, and XRD were applied in the characterization of the materials. EPR, CO 2 adsorption measurements and density functional theory calculations results indicate that the incorporation of S can promote CO 2 adsorption, activation and the formation of *COOH intermediate, which is boosting CO 2 conversion enabling the high selectivity to C 2 H 4 . Compared to unmodified CuO, electrocatalytic studies show that the greatly increased C 2 H 4 activity on S-CuO is because of the fast electron transfer . Meanwhile, the contact angle measurement reveals the excellent selectivity is derived from the suppression of the hydrogen evolution reaction after the S doping.

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