Cu-Ag纳米团簇CO_(2)电催化还原性能和机理  

Catalytic performance and mechanism of CO_(2)electroreduction of Cu-Ag nanoclusters

作　　者：谢鑫瑶 万芬 伏炫羽 范雨婷 陈令修 李鹏[1] XIE Xinyao;WAN Fen;FU Xuanyu;FAN Yuting;CHEN Lingxiu;LI Peng(College of Environment Science and Spatial Informatics,China University of Mining and Technology,Xuzhou 221116,Jiangsu,China;No.270 Research Institute of Nuclear Industry,Nanchang 330299,Jiangxi,China;School of Materials Science and Physics,China University of Mining and Technology,Xuzhou 221116,Jiangsu,China)

机构地区：[1]中国矿业大学环境与测绘学院,江苏徐州221116 [2]核工业二七〇研究所,江西南昌330299 [3]中国矿业大学材料与物理学院,江苏徐州221116

出　　处：《化工进展》2025年第3期1387-1395,共9页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(52104173);江苏省基础研究计划青年基金(BK20210519)。

摘　　要：电催化二氧化碳还原是有效减少二氧化碳排放和促进能源绿色发展的技术,要实现将CO_(2)转化为高价值化合物和燃料(C_(2+))且走向工业化规模仍面临诸多难题。本文利用磁控共溅射技术在碳纸(CP)上成功负载Cu-Ag合金纳米团簇,并通过调控Ag靶材的溅射频率,制备了5种不同Cu/Ag配比的碳基Cu-Ag电极(Cu-Ag/CP),其中Cu-Ag20W/CP颗粒尺寸在228~285nm之间,并评估其电化学性能。结果表明,Cu-Ag/CP有效抑制析氢反应和提高C_(2+)产物的产量,其C_(2+)法拉第效率(FE_(C_(2+)))是碳基Cu电极的2.21倍。Cu-Ag20W/CP在恒电位为−1.07V(vs.RHE)和CO_(2)气体流速为5sccm下,FE_(C_(2+))达78.74%,电流密度达67.92mA/cm^(2),且在连续运行8h后其催化性能和表面结构较为稳定。Cu-Ag/CP具有较大的电化学活性面积和导电性,且明显具有串联催化剂的特征,Ag引入使得*CO生成位点增加,脱附*CO转移至Cu表面进行*CO二聚反应。Cu-Ag/CP是一种具有前景的电催化材料,同时该材料合成方法适合大批量连续生产模式,且产物是高价值的C_(2+)产品,有望为未来电催化CO_(2)工业化提供技术参考。Electrocatalytic carbon dioxide reduction is an effective technology to mitigate CO_(2)emissions and promote green energy development.However,the conversion of CO_(2)into high-value compounds and fuels(C_(2+))on an industrial scale still faces many challenges.In this paper,Cu-Ag alloy nanoclusters were successfully loaded on carbon paper(CP)by magnetron co-sputtering technology,and five carbon-based Cu-Ag electrodes(Cu-Ag/CP)with different Cu/Ag ratios were prepared by adjusting the sputtering frequency of Ag targets,in which Cu-Ag20W/CP particle sizes ranged from 228nm to 285nm,and their electrochemical performance were evaluated.The results showed that Cu-Ag/CP could effectively inhibit the hydrogen evolution reaction and increase the production of C_(2+).Its Faraday efficiency of C_(2+)(FE_(C_(2+)))was 2.21 times that of carbon-based Cu electrode.Under constant potential of-1.07V vs.RHE and CO_(2)gas flow rate of 5 sccm,the FE_(C_(2+))could reach 78.74%and the current density could reach 67.92mA/cm^(2).After continuous operation for 8h,its catalytic performance and surface structure were relatively stable.Cu-Ag/CP had a large electrochemical active area and electrical conductivity,and obviously had the characteristics of tandem catalyst.The introduction of Ag increased the formation site of*CO,and desorption*CO transferred to the Cu surface for*CO dimerization.Cu-Ag/CP was a promising electrocatalytic material,the synthesis method of this material was suitable for large-scale continuous production mode,and the product was a high-value C_(2+)product,which was expected to provide a technical reference for the industrialization of electrocatalytic CO_(2)in the future.

关 键 词：Cu-Ag催化剂 电化学 二氧化碳 还原 磁控共溅射 C_(2+)产物 

分 类 号：TQ151.1[化学工程—电化学工业]