Scientific Reports, Journal Year: 2025, Volume and Issue: 15(1)

Published: May 3, 2025

Abstract Recently, single-atom catalysts (SACs) based on transition metals (TMs) have been identified as highly active with excellent atomic efficiency, reduced consumption of expensive materials, well-defined centers, and tunable activity selectivity. Furthermore, when carbon-based supports (including graphene-derived materials) are employed in SACs, their unique structural electronic properties, such high electrical conductivity mechanical strength, can be integrated. However, for this application, the primary objective is to maintain proper stability-reactivity balance, ensuring system remains stable while preserving its chemical activity. In context, we explore adsorption behavior TM single atoms (Co, Ni, Rh, Pd, Ir, Pt) pristine graphene (pGR), hexagonal boron nitride (hBN), monovacancies (GRm) using DFT-PBE+D3 calculations. From energy trends, observe weak chemisorption pGR physisorption hBN, energies ranging from 0.5 eV (Co/hBN) 1.80 (Rh/pGR). contrast, strength significantly enhanced GRm (strong chemisorption), reaching up 9.11 Ir/GRm, attributed strong defect-induced reactivity improved orbital overlap. Electronic structure analysis reveals that retains semimetallic nature, hBN an insulator, transitions metallic due interactions between TM-C. Bader charge indicates significant transfer GRm, consistent catalytic potential, hybridization indices show substantial pd mixing, favoring anchoring. Thus, our results identify most promising substrate a balanced platform controlled reactivity, support selective catalysis or dielectric applications. Finally, defect engineering powerful strategy designing next-generation catalysts, right balance stability reactivity.

Language: Английский