Dual‐Metal Interbonding as the Chemical Facilitator for Single‐Atom Dispersions

Abstract Atomically dispersed catalysts, with maximized atom utilization of expensive metal components and relatively stable ligand structures, offer high reactivity and selectivity. However, the formation of atomic‐scale metals without aggregation remains a formidable challenge due to thermodynamic stabilization driving forces. Here, a top‐down process is presented that starts from iron nanoparticles, using dual‐metal interbonds (RhFe bonding) as a chemical facilitator to spontaneously convert Fe nanoparticles to single atoms at low temperatures. The presence of RhFe bonding between adjacent Fe and Rh single atoms contributes to the thermodynamic stability, which facilitates the stripping of a single Fe atom from the Fe nanoparticles, leading to the stabilized single atom. The dual single‐atom Rh–Fe catalyst renders excellent electrocatalytic performance for the hydrogen evolution reaction in an acidic electrolyte. This discovery of dual‐metal interbonding as a chemical facilitator paves a novel route for atomic dispersion of chemical metals and the design of efficient catalysts at the atomic scale.