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 , Xiaofu Sun , Shuaiqiang Jia , Shitao Han , Dawei Zhou , Ting Yao , Min Wang , Minghui Fang , Haihong Wu , 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.