Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an ef...Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an efficient NO_(2)-RR catalyst.Theoretical calculations and in situ electrochemical measurements reveal the creation of Bi1-Ru dual sites which can remarkably promote NO_(2)-activation and suppress proton adsorption,while accelerating the NO_(2)-RR protonation energetics to render a high NO_(2)--to-NH_(3)conversion efficiency.Remarkably,Bi1Ru assembled in a flow cell delivers an NH_(3)yield rate of 1901.4μmol h^(-1)cm^(-2)and an NH_(3)-Faradaic efficiency of 94.3%at an industrial-level current density of 324.3 mA cm^(-2).This study offers new perspectives for designing and constructing p-block single-atom alloys as robust and high-current-density NO_(2)-RR catalysts toward the ammonia electrosynthesis.展开更多
基金Longyuan Youth Innovative and Entrepreneurial Talents ProjectProgram for Top Leading Talents of Gansu Province。
文摘Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an efficient NO_(2)-RR catalyst.Theoretical calculations and in situ electrochemical measurements reveal the creation of Bi1-Ru dual sites which can remarkably promote NO_(2)-activation and suppress proton adsorption,while accelerating the NO_(2)-RR protonation energetics to render a high NO_(2)--to-NH_(3)conversion efficiency.Remarkably,Bi1Ru assembled in a flow cell delivers an NH_(3)yield rate of 1901.4μmol h^(-1)cm^(-2)and an NH_(3)-Faradaic efficiency of 94.3%at an industrial-level current density of 324.3 mA cm^(-2).This study offers new perspectives for designing and constructing p-block single-atom alloys as robust and high-current-density NO_(2)-RR catalysts toward the ammonia electrosynthesis.
