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

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.