Enhanced interfacial effect-induced asymmetric coupling boost electroreduction of CO2 to ethylene

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-25 DOI:10.1016/j.apcatb.2023.123666

Yong Zhang , FeiFei Chen , Xiaoya Hao , Yingda Liu , Wentao Wu , Xinghua Zhang , Zehao Zang , Hong Dong , Weihua Wang , Feng Lu , Zunming Lu , Hui Liu , Hui Liu , Feng Luo , Yahui Cheng

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Abstract

Electroreduction of CO₂ to C₂H₄ is a promising strategy for carbon neutralization. However, the kinetic challenge of *CO dimerization, particularly at high current-density, limits its suitability for industrial production. Here, we report that Cu/Ag bimetallic catalyst (Cu₅₂Ag₄₈) with strong interfacial effect can promote high C₂H₄ selectivity at high current-density. We find that the elaborately designed Cu/Ag interface not only inhibits HER and ethanol formation by weakening H adsorption, but also promotes the formation of *CHO intermediates, achieving an unusual asymmetric *CO-*CHO coupling instead of the common symmertic *CO-*CO coupling. Subsequently, the Faradaic efficiency of C₂H₄ over Cu₅₂Ag₄₈ is significantly increased to 69.2% at a high current-density of up to 450 mA cm⁻². The interfacial effect-induced *CO-*CHO coupling can be extended to other metals with weak H and O adsorption such as Cu/Zn and Cu/Au, thereby boosting the production of C₂H₄ in CO₂RR.

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增强界面效应诱导的不对称耦合促进二氧化碳电还原成乙烯

将 CO2 电还原为 C2H4 是一种很有前景的碳中和策略。然而，*CO 二聚化的动力学难题，尤其是在高电流密度下，限制了其在工业生产中的适用性。在此，我们报告了具有强界面效应的铜/银双金属催化剂（Cu52Ag48）可在高电流密度下促进高 C2H4 选择性。我们发现，精心设计的 Cu/Ag 界面不仅能通过削弱 H 的吸附来抑制 HER 和乙醇的形成，还能促进 *CHO 中间体的形成，实现不寻常的不对称 *CO-*CHO 偶联，而不是常见的对称 *CO-*CO 偶联。随后，在 450 mA cm-2 的高电流密度下，C2H4 在 Cu52Ag48 上的法拉第效率显著提高到 69.2%。界面效应诱导的 *CO-*CHO 偶联可扩展到其他具有弱 H 和 O 吸附性的金属，如 Cu/Zn 和 Cu/Au，从而促进 CO2RR 中 C2H4 的产生。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.