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Fine‐tuning the coordination environment and electronic structure of metal sites in metal–nitrogen–carbon (M–N–C) catalysts is an effective strategy for boosting the activity of electrocatalytic CO 2 reduction reaction (CO 2 RR), but remains challenges. Here, a negatively charged polyelectrolyte nanosphere ( n ‐PNS)‐confinement‐pyrolysis strategy is developed to rationally engineer bimetallic atomic sites anchored on a hierarchical porous carbon (HPC) derived from zeolitic imidazolate framework‐8 (ZIF‐8). Through precise design of Cu species (single atoms, atomic clusters, and nanoparticles), the electronic and coordination structures of Fe single‐atom sites are effectively tailored. Notably, X‐ray photoelectron spectroscopy and X‐ray absorption spectroscopy analysis confirms that the incorporation of Cu atomic clusters (Cu C ) adjacent to isolated Fe single atoms (Fe A ) induces significant electron transfer from Fe to Cu through metal–support interactions. By virtue of this electronic modulation, the Cu C Fe A /HPC catalyst exhibits exceptional electrocatalytic CO 2 RR performance, achieving a CO Faradaic efficiency of 91% and a CO current density of 5.57 mA cm −2 , as well as remarkable durability at −0.5 V versus RHE, surpassing the Cu C /HPC and Fe A /HPC references. This study proposes a novel approach for designing bimetallic M–N–C catalysts to achieve efficient CO 2 RR by utilizing the synergistic interactions between single atom and atomic cluster metal species.
Luo et al. (Tue,) studied this question.