2D Multivariate‐Metal‐Organic Frameworks (2D‐M2OF) for High Yield Ammonia Synthesis from Nitrate

Abstract Ammonia synthesis from nitrate offers a promising approach for both nitrate removal and nitrogen recycling. In this study, a series of 2D multivariate‐metal‐organic frameworks (M 2 OFs) is synthesized, incorporating transition metals such as Co, Ni, Mn, and Ag to enhance these processes. These M 2 OFs exhibit remarkable ammonia production performance, with the highest performance achieved using the quaternary structure exceeding a current density of 1 A cm −2 at −0.8 V vs RHE, with an ammonia Faradic efficiency (F.E.) of ≈90%, and a yield rate of 68 mg h −1 cm −2 . Our findings reveal that the synergy among different metal centers in M 2 OFs provides a new efficient reaction pathway for nitrate reduction via surface hydrogen co‐adsorption, a mechanism not attainable with single‐metal MOFs.