From Plasma Modification to Plasma Catalysis: Discharge Time‐Controlled Tuning of Ni‐MOF‐74 for Enhanced Ammonia Synthesis

ABSTRACT This study employed argon plasma technology for the surface modification of Ni‐MOF‐74, systematically investigating the influence of different treatment durations on the material's structure and catalytic performance. It was found that Ni‐MOF‐74 (Ar 120 s) exhibited an outstanding synergistic effect in the plasma‐catalytic synthesis of ammonia. The ammonia synthesis rate increased to 10.77 mmol·g −1 ·h −1 , with a nitrogen conversion rate of 0.4% and an energy yield of 1.54 g·kWh −1 , representing a 1.9 times improvement compared to the pristine sample. Density functional theory (DFT) simulations revealed the mechanism of plasma‐induced defect formation at the electronic structure level, clarifying the structure−activity relationship between material modification and catalytic performance.