Constructing Ag/Cu2O Interface for Efficient Neutral CO2 Electroreduction to C2H4

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-10-29 DOI:10.1002/anie.202417066
Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Rong Cao, 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.

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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。
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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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