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吡咯氮配位单原子铜催化剂的电催化二氧化碳还原性能
引用本文:赵润瑶,纪桂鹏,刘志敏. 吡咯氮配位单原子铜催化剂的电催化二氧化碳还原性能[J]. 高等学校化学学报, 2022, 43(7): 20220272. DOI: 10.7503/cjcu20220272
作者姓名:赵润瑶  纪桂鹏  刘志敏
作者单位: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
基金项目:国家自然科学基金(22121002)
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.

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  
收稿时间:2022-04-24

Efficient Electrocatalytic CO2 Reduction over Pyrrole Nitrogen-coordinated Single-atom Copper Catalysts
ZHAO Runyao,JI Guipeng,LIU Zhimin. Efficient Electrocatalytic CO2 Reduction over Pyrrole Nitrogen-coordinated Single-atom Copper Catalysts[J]. Chemical Research In Chinese Universities, 2022, 43(7): 20220272. DOI: 10.7503/cjcu20220272
Authors:ZHAO Runyao  JI Guipeng  LIU Zhimin
Affiliation:1.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;2.University of Chinese Academy of Sciences,Beijing 100049,China
Abstract: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 CO2 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.
Keywords:Single-atom catalyst  Carbon nanotubes  EXAFS  Electrocatalytic carbon dioxide reduction  CO  
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