吡咯氮配位单原子铜催化剂的电催化二氧化碳还原性能  

Efficient Electrocatalytic CO_(2) Reduction over Pyrrole Nitrogen-coordinated Single-atom Copper Catalysts

作　　者：赵润瑶 纪桂鹏 刘志敏[1,2] ZHAO Runyao;JI Guipeng;LIU Zhimin(Beijing National Laboratory for Molecular Sciences(BNLMS),CAS Key Laboratory of Colloid,Interface and Chemical Thermodynamics,CAS Research/Education Center for Excellence in Molecular Sciences,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院化学研究所,北京分子科学国家研究中心,中国科学院胶体、界面与化学热力学重点实验室,中国科学院分子科学科教融合卓越创新中心,北京100190 [2]中国科学院大学,北京100049

出　　处：《高等学校化学学报》2022年第7期159-165,共7页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:22121002)资助.

摘　　要：采用温度控制的浸渍-热解法,合成了以碳纳米管为载体的一系列铜单原子催化剂.扩展X射线吸收精细结构(EXAFS)分析表明,催化剂中的单原子铜位点分别由吡啶氮和吡咯氮配位.电催化性能测试表明,所制备催化剂可用于电催化二氧化碳生成一氧化碳,由吡啶氮配位的铜单原子催化剂的反应选择性较差,而由吡咯氮配位的铜单原子催化剂则具有更强的活性,CO法拉第效率在−0.70 V(vs.RHE)时可达到96.3%;吡咯氮配位的铜单原子中心对于析氢反应具有更好的抑制效果.A series of carbon nanotube supported copper single-atom catalysts(SACu/CNT-x)was synthesized by a temperature-controlled impregnation-pyrolysis method.Extended X-ray absorption fine structure(EXAFS)analysis indicates that the single-atom copper sites were coordinated with pyridinic-N and pyrrolic-N,respectively,in the catalysts.The catalysts were applied in electrocatalytic carbon dioxide reduction.It was indicated that the catalyst with pyrrole N-coordinated copper single-atom sites showed high activity for CO_(2) electroreduction,affording a high CO Faradaic efficiency of 96.3% at−0.70 V(vs.RHE).Electrochemical experiments show that the pyrrole N-coordinated copper single-atom center has a good inhibitory effect on the hydrogen evolution reaction.

关 键 词：单原子催化剂 碳纳米管 扩展X射线吸收精细结构 电催化二氧化碳还原 一氧化碳 

分 类 号：O643[理学—物理化学]