Precise Synthesis Of Fe-N-2 With N Vacancies Coordination For Boosting Electrochemical Artificial N-2 Fixation

The construction of definitive correlation between structure and catalytic properties for electrochemical artificial N2 fixation is still challenging yet significative. Herein, we have explored the coordinative unsaturation (Fe-N-2) in isolated Fe atoms with nitrogen vacancies (V-N, which are located at the opposite coordination sites of the Fe atom) on interconnected carbon for electrocatalytic ammonia synthesis. Benefiting from dual active centers (Fe-N-2 and V-N) and the spin density on both of them, the novel catalyst exhibits a synergistic improvement of catalytic activity, selectivity, and stability. This work guides the design of the catalyst theoretically and synergistically and combines the advantages of Fe-N-2 with V-N structure creation, defect and spin-state engineering introduction toward the concurrent fulfillment of effective N-2 adsorption and activation. We believe our strategy will incite more investigation into designing high-performance catalysts with well-defined coordinative