First-principles study on Fe_(2)B_(2)as efficient catalyst for nitrogen reduction reaction

摘要

[18_(T)D$IF]Ammonia(NH_(3))is considered an attractive candidate as a clean,highly efficient energy carrier.The electrocatalytic nitrogen reduction reaction(NRR)can reduce energy input and carbon footprint;therefore,rational design of effective electrocatalysts is essential for achieving high-efficiency electrocatalytic NH_(3)synthesis.Herein,we report that the enzymatic mechanism is the more favourable pathway for NRR,due to lower limiting potential(-0.44 V),lower free energy(only 0.02 eV)of the first hydrogenation step(*N–N to*NH–N),and more electron transfer from Fe_(2)B_(2)to the reaction species.In addition,both vacancies and dopants can be helpful in reducing the reaction energy barrier of the potential-determining step.Therefore,we have demonstrated that Fe_(2)B_(2)is a potential new candidate for effective NRR and highlighted its potential for applications in electrocatalytic NH_(3)synthesis.