Modulating CoFe2O4 nanocube with oxygen vacancy and carbon wrapper towards enhanced electrocatalytic nitrogen reduction to ammonia

• Key Words:CO3O4 NANOSHEETS; HIGH-PERFORMANCE; FIXATION; OXIDE
• Abstract:Electrocatalytic nitrogen reduction reaction is increasingly deemed as a promising route for massive ammonia synthesis. Herein, hollow bimetallic CoFe2O4 nanocube derived from prussian blue analogue is elaborately wrapped by thin carbon layer and modified by rich oxygen vacancies, achieving splendid ammonia yield rate of 30.97 mu g h-1 mgcat.- 1 and Faradaic efficiency of 11.65 % at -0.4 V versus reversible hydrogen electrode in 0.1 M Na2SO4. In addition, C@CoFe2O4-x nanocube can withstand long-term and repetitive electrolysis without obvious structure collapse, constituent change and activity decay. The prominent activity is strongly associated with improved nitrogen adsorption and activation, collaboratively benefiting from the intrinsic unoccupied d orbitals of transition metal components, reformative electronic structure by oxygen vacancies and elevated electron injection possibility into the antibonding orbital of nitrogen molecule via conductive carbon wrapper. Both actual experiments and theoretical investigations attest the catalytic activity improvement mechanism, rendering the C@CoFe2O4-x nanocube design strategy efficient and valid.
• Volume:297
• Issue:
• Translation or Not:no