During the last few years,the electrocatalytic nitrogen reduction reaction(NRR)has provided an environmentally friendly and promising alternative to the Haber–Bosch process.However,due to the competing hydrogen evolu...During the last few years,the electrocatalytic nitrogen reduction reaction(NRR)has provided an environmentally friendly and promising alternative to the Haber–Bosch process.However,due to the competing hydrogen evolution reaction and the hard-to-break strong NuN bond with high bond energy(941 kJ mol^(-1)),the synthesis of efficient NRR catalysts is still a challenge.Herein,we report a cost-effective layered double hydroxide(LDH)derived bimetallic NiFe selenide(Ni_(0.75)Fe_(0.25)Se_(2))in Li_(2)SO_(4)solution for NRR under ambient conditions,which exhibits an NH_(3)yield rate of 5.64μg h^(-1)cm^(-2)_(cat)and faradaic efficiency of 12.3%at−0.1 V vs.RHE,being superior to those of pristine NiFe–LDH,NiSe_(2),and FeSe_(2)as well as several state-of-the-art noble metal catalysts.The high electrocatalytic NRR activity and selectivity of Ni_(0.75)Fe_(0.25)Se_(2)demonstrate the first example of NiFe selenide catalyst with a facile synthesis strategy towards efficient nitrogen fixation.展开更多
基金supported by the National Natural Science Foundation of China(grant no.21771021,21822501,and 22061130206)the Beijing Municipal Natural Science Foundation(JQ20003)+4 种基金the Newton Advanced Fellowship award(NAF\R1\201285)the Fok Ying-Tong Education Foundation(grant no.171008)the Beijing Nova Program(grant no.xx2018115)the Measurements Fund of Beijing Normal Universitythe Fundamental Research Funds for the Central Universities.
文摘During the last few years,the electrocatalytic nitrogen reduction reaction(NRR)has provided an environmentally friendly and promising alternative to the Haber–Bosch process.However,due to the competing hydrogen evolution reaction and the hard-to-break strong NuN bond with high bond energy(941 kJ mol^(-1)),the synthesis of efficient NRR catalysts is still a challenge.Herein,we report a cost-effective layered double hydroxide(LDH)derived bimetallic NiFe selenide(Ni_(0.75)Fe_(0.25)Se_(2))in Li_(2)SO_(4)solution for NRR under ambient conditions,which exhibits an NH_(3)yield rate of 5.64μg h^(-1)cm^(-2)_(cat)and faradaic efficiency of 12.3%at−0.1 V vs.RHE,being superior to those of pristine NiFe–LDH,NiSe_(2),and FeSe_(2)as well as several state-of-the-art noble metal catalysts.The high electrocatalytic NRR activity and selectivity of Ni_(0.75)Fe_(0.25)Se_(2)demonstrate the first example of NiFe selenide catalyst with a facile synthesis strategy towards efficient nitrogen fixation.
