Constructing Ag/Cu2O interface for efficient neutral CO2 electroreduction to C2H4.

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Rong Cao, Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Minna Cao
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Abstract

Neutral CO2 electroreduction to multi-carbons (C2+) offers a promising pathway to reduce the CO2 and energy losses originating from the carbonate formation. However, the sluggish kinetics of C-C coupling brings a significant challenge of achieving high selectivity of a single product (such as ethylene), especially at industrial-relevant current densities (> 300 mA cm-2). Here, we reported an optimized Ag-Cu2O interfacial catalyst that exhibited C2+ Faradaic efficiency (FE) of 73.6% at 650 mA cm-2 in a flow cell. Remarkably, it obtained FEC2H4 of 66.0% with a partial current density of 429.1 mA cm-2, making it stand out among the reported Cu-based electrocatalysts. In situ Raman spectra uncovered that the Ag/Cu2O interfaces enabled a high coverage of *CO around the partially reduced Cu+/Cu0 active sites. Furthermore, theoretical calculations demonstrated the enhanced CO formation and C-C coupling at the Ag/Cu2O interface. This work reported an unprecedented neutral CO2 electroreduction to C2H4 performance and provided an in-depth comprehension of the role of the bimetallic interface.

构建 Ag/Cu2O 界面,实现高效中性 CO2 电还原为 C2H4。
中性二氧化碳电还原为多碳化合物(C2+)提供了一条很有前景的途径,可以减少二氧化碳和碳酸盐形成所造成的能量损失。然而,C-C 偶联的缓慢动力学给实现单一产物(如乙烯)的高选择性带来了巨大挑战,尤其是在工业相关的电流密度(> 300 mA cm-2)条件下。在此,我们报告了一种优化的银-铜氧化物界面催化剂,该催化剂在流动池中 650 mA cm-2 的条件下,C2+ 法拉第效率 (FE) 为 73.6%。值得注意的是,在部分电流密度为 429.1 mA cm-2 时,它获得了 66.0% 的 FEC2H4,使其在已报道的铜基电催化剂中脱颖而出。原位拉曼光谱显示,Ag/Cu2O 界面使得*CO 在部分还原的 Cu+/Cu0 活性位点周围有很高的覆盖率。此外,理论计算也证明了在 Ag/Cu2O 界面上 CO 生成和 C-C 耦合的增强。这项工作报告了前所未有的中性 CO2 电还原为 C2H4 的性能,并深入理解了双金属界面的作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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