High-throughput computational screening of two-dimensional metal organic framework as promising catalysts for electrochemical nitric oxide reduction

• High-throughput DFT screening of 2D TM–Tp MOFs for NO reduction reactions (NORR). • Fe–Tp and Ru–Tp identified as efficient catalysts with low limiting potentials. • Strong NO adsorption suppresses competing hydrogen evolution reactions (HER). • AIMD simulations confirm the high thermal stability of Fe–Tp and Ru–Tp. • Study guides the design of MOF electrocatalysts for sustainable NH 3 production. Two-dimensional transition metal–organic frameworks (TM–MOFs) have emerged as promising catalysts for the electrochemical nitric oxide reduction reaction (NORR) for ammonia production. Using the first-principles calculations and high-throughput computational screening approach, we have investigated the structural stability, NO adsorption behavior, reaction energetics, and selectivity for NORR of TM–Tp MOFs (TM = Sc to Au; Tp = triformylphloroglucinol). Among the screened candidates, Fe–Tp and Ru–Tp emerged as the most efficient catalysts due to their favorable thermodynamic and electrochemical stability, strong NO adsorption, and low energy barrier for the hydrogenation steps. A detailed investigation of the reaction pathways reveals that Fe–Tp and Ru–Tp have low limiting potentials of –0.32 V and –0.35 V, respectively. The selectivity volcano analysis shows that both MOFs preferentially adsorb NO over hydrogen, suppressing the competing hydrogen evolution reaction. Furthermore, ab initio molecular dynamics simulations confirmed their excellent thermal stability. The volcano plot shows that Fe–Tp and Ru–Tp are at the top of the catalytic performance curve, indicating an optimal balance between activity and intermediate binding strength. This work highlights Fe–Tp and Ru–Tp MOFs as highly promising, stable, and selective NORR electrocatalysts for sustainable and efficient electrochemical ammonia synthesis.