Active and durable catalysts toward the N_(2) reduction reaction(NRR)play a crucial role in electrocatalytic fixation of N_(2) to NH_(3).Herein,we designed an efficient NiO-based NRR electrocatalyst by introducing oxy...Active and durable catalysts toward the N_(2) reduction reaction(NRR)play a crucial role in electrocatalytic fixation of N_(2) to NH_(3).Herein,we designed an efficient NiO-based NRR electrocatalyst by introducing oxygen vacancies(OVs)through a facile plasma technique.Although the pristine NiO nanosheets exhibited poor NRR activity,the plasma-engineered NiO nanosheets with enriched OVs delivered significantly enhanced NRR activity with an NH_(3) yield of 29.1μg h^(-1) mg^(-1) and a faradaic efficiency of 10.8%in 0.1 M Na_(2)SO_(4) at-0.5 V(RHE)under ambient conditions,comparable or superior to most reported NRR catalysts.Density functional theory calculations revealed that OV introduction could readily tailor the electronic structures of NiO to result in enhanced conductivity,improved N_(2) adsorption,a reduced reaction energy barrier,and a less-promoted hydrogen evolution reaction.展开更多
基金supported by the National Natural Science Foundation of China(51761024)the CAS“Light of West China”Program,the“Feitian Scholar”Program of Gansu Province,and the Foundation of A Hundred Youth Talents Training Program of Lanzhou Jiaotong University.
文摘Active and durable catalysts toward the N_(2) reduction reaction(NRR)play a crucial role in electrocatalytic fixation of N_(2) to NH_(3).Herein,we designed an efficient NiO-based NRR electrocatalyst by introducing oxygen vacancies(OVs)through a facile plasma technique.Although the pristine NiO nanosheets exhibited poor NRR activity,the plasma-engineered NiO nanosheets with enriched OVs delivered significantly enhanced NRR activity with an NH_(3) yield of 29.1μg h^(-1) mg^(-1) and a faradaic efficiency of 10.8%in 0.1 M Na_(2)SO_(4) at-0.5 V(RHE)under ambient conditions,comparable or superior to most reported NRR catalysts.Density functional theory calculations revealed that OV introduction could readily tailor the electronic structures of NiO to result in enhanced conductivity,improved N_(2) adsorption,a reduced reaction energy barrier,and a less-promoted hydrogen evolution reaction.
