Tailoring Cu–Zn Dual-Atom Sites with Reordering d‑Orbital Splitting Manner for Highly Efficient Acetylene Semihydrogenation

The design of inexpensive, nontoxic, and abundant transition metal catalysts for the selective hydrogenation of alkynes remains a significant challenge faced by both the industrial and academic communities. Here, we report a novel catalyst comprising a well-defined Cu–Zn dual-atom catalyst supported on defective pyrolyzed ZIF-8 material (CuZn/NC2), resulting in enhanced d-electron domination near the Fermi level and reordered d-orbital Splitting manner. This catalyst exhibited outstanding performance in the selective hydrogenation of acetylene to ethylene, demonstrating high conversion rates (97%), remarkable selectivity (97.5%), and excellent stability (over 70 h). The unique structural characteristics of Cu–Zn dual-atom sites, anchored to the carrier through Cu–N3&Zn–N3 configurations, ensured effective acetylene activation and easy desorption of ethylene. These features are pivotal to the catalyst’s exceptional activity and selectivity. This work presents a new approach to the design of nonprecious metal catalysts for the selective hydrogenation of acetylene.