Electrochemical CO2 reduction to C2+ products with ampere-level current on carbon-modified copper catalysts

IF 10.8 2区 化学 Q1 CHEMISTRY, PHYSICAL
Xue Dong , Xiaofu Sun , Shuaiqiang Jia , Shitao Han , Dawei Zhou , Ting Yao , Min Wang , Minghui Fang , Haihong Wu , Buxing Han
{"title":"Electrochemical CO2 reduction to C2+ products with ampere-level current on carbon-modified copper catalysts","authors":"Xue Dong ,&nbsp;Xiaofu Sun ,&nbsp;Shuaiqiang Jia ,&nbsp;Shitao Han ,&nbsp;Dawei Zhou ,&nbsp;Ting Yao ,&nbsp;Min Wang ,&nbsp;Minghui Fang ,&nbsp;Haihong Wu ,&nbsp;Buxing Han","doi":"10.3866/PKU.WHXB202404012","DOIUrl":null,"url":null,"abstract":"<div><div>Copper-based electrocatalysts have great potential to produce high-value products in CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR), offering a promising way to achieve negative carbon emissions. Additionally, achieving ampere-level currents is crucial for realizing the industrialization of multi-carbon (C<sub>2+</sub>) products. However, the C<sub>2+</sub> selectivity at industrial current densities remains unsatisfactory due to complex electron transport processes and inevitable side reactions. Herein, we developed a carbon-modification strategy aimed at optimizing the local environment and regulating the adsorption of intermediates at Cu active sites. Our findings demonstrated the effectiveness of Cu-C<sub><em>x</em></sub> catalysts (where ‘<em>x</em>’ denoted the atomic percentage of C in the catalysts) in facilitating CO<sub>2</sub>RR for producing C<sub>2+</sub> products. Especially, over Cu–C<sub>6%</sub>, the current density could reach to 1.25 A cm<sup>−2</sup> at −0.72 V <em>vs</em>. RHE (<em>versus</em> reversible hydrogen electrode) in a flow cell, and the Faradaic efficiency (FE) of C<sub>2</sub>H<sub>4</sub> and C<sub>2+</sub> products could reach to 54.4 % and 80.2 %, respectively. <em>In situ</em> spectral analysis and density functional theory (DFT) calculations showed that the presence of C regulated the adsorption of ∗CO on Cu surface, reduced the energy barrier of C–C coupling, thus promoting the production of C<sub>2+</sub> products.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 3","pages":"Article 100024"},"PeriodicalIF":10.8000,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"物理化学学报","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1000681824000249","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Copper-based electrocatalysts have great potential to produce high-value products in CO2 reduction reaction (CO2RR), offering a promising way to achieve negative carbon emissions. Additionally, achieving ampere-level currents is crucial for realizing the industrialization of multi-carbon (C2+) products. However, the C2+ selectivity at industrial current densities remains unsatisfactory due to complex electron transport processes and inevitable side reactions. Herein, we developed a carbon-modification strategy aimed at optimizing the local environment and regulating the adsorption of intermediates at Cu active sites. Our findings demonstrated the effectiveness of Cu-Cx catalysts (where ‘x’ denoted the atomic percentage of C in the catalysts) in facilitating CO2RR for producing C2+ products. Especially, over Cu–C6%, the current density could reach to 1.25 A cm−2 at −0.72 V vs. RHE (versus reversible hydrogen electrode) in a flow cell, and the Faradaic efficiency (FE) of C2H4 and C2+ products could reach to 54.4 % and 80.2 %, respectively. In situ spectral analysis and density functional theory (DFT) calculations showed that the presence of C regulated the adsorption of ∗CO on Cu surface, reduced the energy barrier of C–C coupling, thus promoting the production of C2+ products.

Abstract Image

求助全文
约1分钟内获得全文 求助全文
来源期刊
物理化学学报
物理化学学报 化学-物理化学
CiteScore
16.60
自引率
5.50%
发文量
9754
审稿时长
1.2 months
期刊介绍:
×
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