Achieving more meaningful N2 conversion by reducing the energy input and carbon footprint is now being investigated through a method of N2 fixation instead of the Haber-Bosch process.Unfortunately,the electrochemical ...Achieving more meaningful N2 conversion by reducing the energy input and carbon footprint is now being investigated through a method of N2 fixation instead of the Haber-Bosch process.Unfortunately,the electrochemical N2 reduction reaction(NRR)method as a rising approach currently still shows low selectivity(Faradaic efficiency<10%)and high-energy consumption[applied potential at least-0.2 V versus the reversible hydrogen electrode(RHE)].Here,the role of molybdenum aluminum boride single crystals,belonging to a family of ternary transition metal aluminum borides known as MAB phases,is reported for the electrochemical NRR for the first time,at a low applied potential(-0.05 V versus RHE)under ambient conditions and in alkaline media.Due to the unique nano-laminated crystal structure of the MAB phase,these inexpensive materials have been found to exhibit excellent electrocatalytic performances(NH3 yield:9.2μg h^-1cm^-2mgcat^-1.,Faradaic efficiency:30.1%)at the low overpotential,and to display a high chemical stability and sustained catalytic performance.In conjunction,further mechanism studies indicate B and Al as main-group metals show a highly selective affinity to N2 due to the strong interaction between the B 2p/Al 3p band and the N 2p orbitals,while Mo exhibits specific catalytic activity toward the subsequent reduction reaction.Overall,the MAB-phase catalyst under the synergy of the elements within ternary compound can suppress the hydrogen evolution reaction and achieve enhanced NRR performance.The significance of this work is to provide a promising candidate in the future synthesis of ammonia.展开更多
文摘Achieving more meaningful N2 conversion by reducing the energy input and carbon footprint is now being investigated through a method of N2 fixation instead of the Haber-Bosch process.Unfortunately,the electrochemical N2 reduction reaction(NRR)method as a rising approach currently still shows low selectivity(Faradaic efficiency<10%)and high-energy consumption[applied potential at least-0.2 V versus the reversible hydrogen electrode(RHE)].Here,the role of molybdenum aluminum boride single crystals,belonging to a family of ternary transition metal aluminum borides known as MAB phases,is reported for the electrochemical NRR for the first time,at a low applied potential(-0.05 V versus RHE)under ambient conditions and in alkaline media.Due to the unique nano-laminated crystal structure of the MAB phase,these inexpensive materials have been found to exhibit excellent electrocatalytic performances(NH3 yield:9.2μg h^-1cm^-2mgcat^-1.,Faradaic efficiency:30.1%)at the low overpotential,and to display a high chemical stability and sustained catalytic performance.In conjunction,further mechanism studies indicate B and Al as main-group metals show a highly selective affinity to N2 due to the strong interaction between the B 2p/Al 3p band and the N 2p orbitals,while Mo exhibits specific catalytic activity toward the subsequent reduction reaction.Overall,the MAB-phase catalyst under the synergy of the elements within ternary compound can suppress the hydrogen evolution reaction and achieve enhanced NRR performance.The significance of this work is to provide a promising candidate in the future synthesis of ammonia.
