Electrocatalytic nitrate reduction reaction(NO_(3^(-))RR)is a green and competitive method for removing nitrate from water,requiring highly active and long-term stable electrocatalysts.In this work,we report a Cu^(0)n...Electrocatalytic nitrate reduction reaction(NO_(3^(-))RR)is a green and competitive method for removing nitrate from water,requiring highly active and long-term stable electrocatalysts.In this work,we report a Cu^(0)nanorod catalyst with disordered structure(re-Cu NRs),prepared by electrochemical in situ reconfiguration of copper-based nitrides(Cu_(3)N NRs).The amorphous structure allows the exposure of abundant active sites to enhance the electrocatalytic activity because of the disordered atomic arrangement.At a potential of-1.2 V vs.Ag/Ag Cl,the re-Cu NRs catalyst achieved nearly 100%nitrate conversion within 120 min at a low nitrate concentration(50 mg/L),without the accumulation of nitrite.Insitu DEMS detection reveals that the NO3-RR on re-Cu NRs followed the pathway of^(*)NO3^(-)→^(*)NO2^(-)→^(*)NO→^(*)N→^(*)NH→^(*)NH_(2)→^(*)NH_(3).Furthermore,combining this proposed pathway with electrochlorination could efficiently transform ammonia into harmless N2(~99.41%).Theoretical calculations confirm that the amorphous structure on the surface of re-Cu NRs catalysts can facilitate strongly adsorbed nitrate,weaken the rate-determining step of^(*)NH_(3)→NH_(3),and suppress hydrogen evolution reaction(HER).This study provides a new approach for designing efficient and stable amorphous catalysts for electrocatalytic nitrate reduction.展开更多
基金supported by the National Natural Science Foundation of China(No.21876105)Shaanxi“Scientist&Engineer”Team(No.2023KXJ-131)Xianyang Key S&T Special Projects(No.L2023-ZDKJ-QCY-SXGG-GY-007)。
文摘Electrocatalytic nitrate reduction reaction(NO_(3^(-))RR)is a green and competitive method for removing nitrate from water,requiring highly active and long-term stable electrocatalysts.In this work,we report a Cu^(0)nanorod catalyst with disordered structure(re-Cu NRs),prepared by electrochemical in situ reconfiguration of copper-based nitrides(Cu_(3)N NRs).The amorphous structure allows the exposure of abundant active sites to enhance the electrocatalytic activity because of the disordered atomic arrangement.At a potential of-1.2 V vs.Ag/Ag Cl,the re-Cu NRs catalyst achieved nearly 100%nitrate conversion within 120 min at a low nitrate concentration(50 mg/L),without the accumulation of nitrite.Insitu DEMS detection reveals that the NO3-RR on re-Cu NRs followed the pathway of^(*)NO3^(-)→^(*)NO2^(-)→^(*)NO→^(*)N→^(*)NH→^(*)NH_(2)→^(*)NH_(3).Furthermore,combining this proposed pathway with electrochlorination could efficiently transform ammonia into harmless N2(~99.41%).Theoretical calculations confirm that the amorphous structure on the surface of re-Cu NRs catalysts can facilitate strongly adsorbed nitrate,weaken the rate-determining step of^(*)NH_(3)→NH_(3),and suppress hydrogen evolution reaction(HER).This study provides a new approach for designing efficient and stable amorphous catalysts for electrocatalytic nitrate reduction.
