Anti‐Perovskite Type Ni ₃ InC _0.5 Anchored on Defective Nano Diamond‐Graphene for Highly Efficient Acetylene Semi‐Hydrogenation

Abstract Designing low‐cost, nontoxic, and earth‐abundant transition metal catalysts for the selective hydrogenation of alkynes is important but high selectivity and hydrogenation activity simultaneously remains challenging. Herein, an anti‐perovskite crystal structure Ni 3 InC 0.5 catalyst supported on a defective nanodiamond graphene (ND@G) is reported, which exhibits excellent catalytic performance for the selective conversion of C 2 H 2 to C 2 H 4 , i.e., with high conversion (95%), high selectivity (85%), and good stability (over 250 h). Density functional theory calculations and performance analysis reveal that synergistic effect between ND@G support and Ni 3 InC 0.5 nanoparticles enable highly efficient C 2 H 2 semi‐hydrogenation. ND@G support makes Ni more electron‐rich through strong metal‐support interactions, as a result of reducing the energy barrier of rate determining step and improving hydrogenation activity. Meanwhile, the crystal geometric structure of Ni 3 InC 0.5 can effectively promote desorption of C 2 H 4 and suppressed the reaction pathway of C 2 H 4 over‐hydrogenation, thus improved the semi‐hydrogenation selectivity. This work provides insights into the design of anti‐perovskite type catalysts with engineered metal‐support interactions, offering potential applications in industrial catalysis.