Optimizing *CO Interaction on Cu-Fe Bimetallic Sites Synergized with Boron and Nitrogen Co-doped Graphene for Efficient CO2 Electroreduction

A central challenge, however, lies in achieving high product selectivity, hindered by the prevalence of competing reaction pathways. Rational manipulation of active site configurations is an effective strategy for precisely tuning the binding interaction with key intermediates, thereby dictating the selectivity towards desired products.

Herein, we engineered an oxophilic Fe-modified Cu nanoparticles anchored on a boron- and nitrogen-codoped porous graphene matrix (CuFe-BNPG). It was found that the catalyst achieved a CH4 faradaic efficiency of 21.5 %, which is approximately 3.6 times that of the monometallic Cu counterpart (Cu-BNPG). Mechanistic investigations by experiments and theoretical calculations revealed that the incorporation of Fe efficiently optimized the binding interaction with *CO, orchestrating a beneficial energetic landscape for subsequent hydrogenation steps.