物理化学学报2025，Vol.41Issue(3)：77-84,8.DOI:10.3866/PKU.WHXB202404012
碳修饰的铜催化剂实现安培级电流电化学还原CO2制C2+产物
Electrochemical CO2 Reduction to C2+Products with Ampere-Level Current on Carbon-Modified Copper Catalysts
摘要
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.关键词
CO2还原/电催化/多碳产物/绿色化学/安培电流Key words
CO2 reduction/Electrocatalysis/Multi-carbon products/Green chemistry/Ampere-level current分类
化学引用本文复制引用
董雪,韩布兴,孙晓甫,贾帅强,韩世涛,周达伟,姚婷,王敏,方明慧,吴海虹..碳修饰的铜催化剂实现安培级电流电化学还原CO2制C2+产物[J].物理化学学报,2025,41(3):77-84,8.基金项目
The work was supported by the National Key Research and Development Program of China(2023YFA1507901,2020YFA0710201)and National Natural Science Foundation of China(22293015,22121002). 国家重点研发计划项目(2023YFA1507901,2020YFA0710201)和国家自然科学基金项目(22293015,22121002)资助 （2023YFA1507901,2020YFA0710201）
