Computational Simulation of Ammonia Borane Adsorption and Activation on Transition Metal‐Doped Two‐Dimensional MoS 2

Abstract

Abstract

Based on first‐principles calculations within the framework of density functional theory (DFT), this study systematically investigates the adsorption and catalytic behavior of ammonia borane (H 3 BNH 3 , AB) molecules on transition metal (Ti, V, Cr, Fe, Co, Cu, Zn, Zr, Nb, Hf, Ta, W)‐doped MoS 2 surfaces. By analyzing the adsorption energy, BH bond elongation, charge transfer, and electronic structure characteristics, Zn‐, Co‐, and Cu‐doped systems were identified as high‐performance catalytic surfaces, among which Zn‐MoS 2 exhibits the most pronounced activation effect on the BH bond, with a maximum elongation of 18.3%. Further analysis combining charge density difference (CDD), Bader charge, and projected density of states (PDOS) reveals that the incorporation of Zn effectively modulates the electronic structure of the substrate, enhances charge transfer between the substrate and AB molecules, and promotes the accumulation of negative charge on hydrogen atoms, thereby significantly weakening the BH bond strength. This study elucidates the atomic‐ and electronic‐level features of AB adsorption and BH bond preactivation on doped MoS 2 surfaces, providing theoretical insights for the design of non‐noble metal catalysts toward the initial step of AB‐based hydrogen production.