Precise synthesis of Fe-N2 with N vacancies coordination for boosting electrochemical artificial N2 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

Automated summary

This study investigated the impact of coordinative unsaturation and nitrogen vacancies on carbon-based catalysts for electrocatalytic ammonia synthesis, showing a synergistic improvement in catalytic activity, selectivity, and stability. This work provides new theoretical and synergistic guidance for the design of high-performance catalysts.