Abstract

This study delves into the potential of MB36 clusters (where M = Fe, Co, Ni) supported on graphene as effective single-atom catalysts (SACs). Our research is methodically segmented into several stages, each designed to validate the feasibility of the proposed material. We begin by investigating the potential energy surface of MB36 clusters. Our findings reveal a preference for metallic atoms to position themselves above the central hexagonal vacancy of the B36 cluster. This factor significantly contributes to the stabilization of the resultant MB36 system. Subsequently, we employ ab-initio molecular dynamic simulations to affirm the stability of the graphenesupported MB36 clusters. In the final stage, we evaluate the system's catalytic capability for the oxygen reduction reaction (ORR) by calculating the dissociation energy of O2 and OOH post their adsorption on the M atom of the graphene-supported MB36 cluster. These simulations suggest that FeB36 could maintain stability at room temperature, exhibiting activation energies for O2 and OOH dissociation lower than those previously reported on Fe/N/C-type SACs, approaching those found on the Pt(111) surface, the most efficient ORR electrocatalyst. This computational study suggests that graphene-supported FeB36 clusters could emerge as a promising candidate for SACs.