The electrochemical conversion of toxic nitrite(NO_(2)-)is a promising approach for the simultaneous removal of nitrogen contaminants and synthesis of ammonia(NH_(3)).In this study,we present the Er-doping-induced ele...The electrochemical conversion of toxic nitrite(NO_(2)-)is a promising approach for the simultaneous removal of nitrogen contaminants and synthesis of ammonia(NH_(3)).In this study,we present the Er-doping-induced electronic modulation of CoP integrated with nitrogen-doped carbon(CN)nanosheets supported on a titanium mesh(Er-CoP@NC/TM)for the electrocatalytic NO_(2)-reduction reaction(eNO_(2)-RR)for NH_(3)synthesis.The catalyst demonstrates a high Faraday efficiency of 97.08±2.22%and a high yield of 2087.60±17.10μmol h^(-1)cm^(-2)for NH_(3)production.Characterization and theoretical calculations revealed that Er-doping facilitated the electronic modulation of CoP in Er-CoP@NC/TM,which regulated the adsorption behaviors of intermediates and was the rate-limiting step for the eNO_(2)-RR,thereby enhancing the electrocatalytic performance.Quenching experiments and electron paramagnetic resonance tests suggest that both direct electrocatalytic reduction by active hydrogen and electron transfer are critical for the eNO_(2)-RR for NH_(3)synthesis.Furthermore,Er-CoP@NC/TM exhibited high performance across a wide range of NO_(2)-concentrations(0.05-0.1 mol L^(-1))and pH values(4-13).In addition,the catalyst demonstrated strong resistance to anions and a long cycle life in simulated wastewater environments.This study offers a powerful approach for the remediation of NO_(2)-wastewater and recovery of valuable inorganic compounds.展开更多
文摘The electrochemical conversion of toxic nitrite(NO_(2)-)is a promising approach for the simultaneous removal of nitrogen contaminants and synthesis of ammonia(NH_(3)).In this study,we present the Er-doping-induced electronic modulation of CoP integrated with nitrogen-doped carbon(CN)nanosheets supported on a titanium mesh(Er-CoP@NC/TM)for the electrocatalytic NO_(2)-reduction reaction(eNO_(2)-RR)for NH_(3)synthesis.The catalyst demonstrates a high Faraday efficiency of 97.08±2.22%and a high yield of 2087.60±17.10μmol h^(-1)cm^(-2)for NH_(3)production.Characterization and theoretical calculations revealed that Er-doping facilitated the electronic modulation of CoP in Er-CoP@NC/TM,which regulated the adsorption behaviors of intermediates and was the rate-limiting step for the eNO_(2)-RR,thereby enhancing the electrocatalytic performance.Quenching experiments and electron paramagnetic resonance tests suggest that both direct electrocatalytic reduction by active hydrogen and electron transfer are critical for the eNO_(2)-RR for NH_(3)synthesis.Furthermore,Er-CoP@NC/TM exhibited high performance across a wide range of NO_(2)-concentrations(0.05-0.1 mol L^(-1))and pH values(4-13).In addition,the catalyst demonstrated strong resistance to anions and a long cycle life in simulated wastewater environments.This study offers a powerful approach for the remediation of NO_(2)-wastewater and recovery of valuable inorganic compounds.
