Graphdiyne‐Induced Iron Vacancy for Efficient Nitrogen Conversion

An iron vacancy‐rich ferroferric oxide/graphdiyne heterostructure (IVR‐FO/GDY) is rationally designed and fabricated for high‐efficiency electrocatalytic nitrogen fixation to ammonia (ENFA). Experimental and theoretical results show that the GDY‐induced iron vacancies in IVR‐FO/GDY promote the electrocatalysis, and activate the local O sites to transfer electrons towards GDY to boost ENFA, resulting in promising electrocatalytic performances with a highest ammonia yield (Y(NH3)) of 134.02 µg h(−1) mg(cat.) (−1) and Faradaic efficiency (FE) of up to 60.88%, as well as the high long‐term stability in neutral electrolytes. The cationic vacancy activation strategy proposed in this work has strong general and universal guiding significance to the design of new efficient electrocatalysts for various electrochemical energy conversion reactions. Such defect engineering may be used efficiently in electrocatalysis, leading to the development and progress of energy industry.