Mesoporous Nitrogen‐Doped Carbon‐Nanosphere‐Supported Isolated Single‐Atom Pd Catalyst for Highly Efficient Semihydrogenation of Acetylene

Abstract Semihydrogenation of acetylene in the ethylene feed is a vital step for the industrial production of polyethylene. Despite their favorable reaction activity and ethylene selectivity, the Pd‐based intermetallic compound and single‐atom alloy catalysts still suffer from the limitation of atomic utilization derived from the partial exposure of active Pd atoms. Herein, a hard‐template Lewis acid doping strategy is reported that can overcome the inefficient utilization of Pd atoms. In this strategy, N‐coordinated isolated single‐atomic Pd sites are fully embedded on the inner walls of mesoporous nitrogen‐doped carbon foam nanospheres (ISA‐Pd/MPNC). This synthetic strategy has been proved to be applicable to prepare other ISA‐M/MPNC (M = Pt and Cu) materials. This ISA‐Pd/MPNC catalyst with both high specific surface area (633.8 m 2 g −1 ) and remarkably thin pore wall (1–2 nm) exhibits higher activity than that of its nonmesoporous counterpart (ISA‐Pd/non‐MPNC) catalyst by a factor of 4. This work presents an efficient way to tailor and optimize the catalytic activity and selectivity by atomic‐scale design and structural control.