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 : 2025-01-21 Epub Date: 2024-11-14 DOI:10.1002/anie.202417066
Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Rong Cao, Minna Cao
{"title":"Constructing Ag/Cu<sub>2</sub>O Interface for Efficient Neutral CO<sub>2</sub> Electroreduction to C<sub>2</sub>H<sub>4</sub>.","authors":"Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Rong Cao, Minna Cao","doi":"10.1002/anie.202417066","DOIUrl":null,"url":null,"abstract":"<p><p>Neutral CO<sub>2</sub> electroreduction to multi-carbons (C<sub>2+</sub>) offers a promising pathway to reduce the CO<sub>2</sub> 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<sup>-2</sup>). Here, we reported an optimized Ag-Cu<sub>2</sub>O interfacial catalyst that exhibited C<sub>2+</sub> Faradaic efficiency (FE) of 73.6 % at 650 mA cm<sup>-2</sup> in a flow cell. Remarkably, it obtained FE<sub>C2H4</sub> of 66.0 % with a partial current density of 429.1 mA cm<sup>-2</sup>, making it stand out among the reported Cu-based electrocatalysts. In situ Raman spectra uncovered that the Ag/Cu<sub>2</sub>O interfaces enabled a high coverage of *CO around the partially reduced Cu<sup>+</sup>/Cu<sup>0</sup> active sites. Furthermore, theoretical calculations demonstrated the enhanced CO formation and C-C coupling at the Ag/Cu<sub>2</sub>O interface. This work reported an unprecedented neutral CO<sub>2</sub> electroreduction to C<sub>2</sub>H<sub>4</sub> performance and provided an in-depth comprehension of the role of the bimetallic interface.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202417066"},"PeriodicalIF":16.1000,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202417066","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/14 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

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。
求助全文
约1分钟内获得全文 求助全文
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.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信