Harnessing Spin‐Lattice Interplay in Metal Nitrides for Efficient Ammonia Electrosynthesis

Abstract Metal nitrides, renowned for their spin‐lattice‐charge interplay, offer vast potential in catalysis, electronics, and energy conversion. However, spin polarization manipulation in these nitrides remains a challenge for multi‐electron electrocatalytic processes. This study introduces Co 3 Mo 3 N with a low‐spin polarization configuration, achieved by incorporating spin‐free lattice Mo with 4 d orbitals into high‐spin polarization Co 4 N. This innovation delivers outstanding nitrate‐to‐ammonia electrosynthesis, ranking among the best to date. Mo inclusion induces competing magnetic exchange interactions, reducing the spin polarization degree and enabling rate‐determining step of NO 2 * to NO‐OH* conversion via vertex‐sharing NMo 6 octahedra. A paired electro‐refinery with a Co 3 Mo 3 N cathode achieves 2 000 mA cm −2 at 2.28 V and sustains an industrial‐scale current of 1 000 mA cm −2 for 2,100 h, with an NH 3 production rate of ≈70 mg NH 3 h −1 cm −2 . This work establishes a transformative platform for spin polarization degree‐engineered electrocatalysts, driving breakthroughs in energy conversion technologies.