Substrate‐Adatom Interface Engineering of Transition Metal Decorated Boron‐Doped Graphene Sheet for Enhanced Adsorption of Xe and Kr – A Systematic Ab initio Study

Abstract

Efficient adsorption and segregation of Xe and Kr gases are of high importance in commercial and nuclear industries. Systematic ab initio calculations reveal that transition-metal (TM) decorated boron-doped graphene (BDG-TM) sheet can act as an efficient substrate for adsorptive capture of Xe and Kr (adatoms). Substantial enhancement in the adsorption energy (E ads ) is obtained on BDG-TM substrates, and it varies as BDG-Cu > BDG-Ni > BDG-Fe > BDG-Zn. The improvement is approximately four times that of the pristine BDG and twice that of the conventional metallic substrates. TM-decoration alters the charge distribution at the substrate-adatom interface, which brings a considerable change in the polarization and induced dipole moment of adatom, leading to significant improvement in the E ads . Partial density of states analysis shows a splitting and significant interaction of Xe-p with TM-d orbitals near the Fermi level of Fe, Ni, and Cu decorated systems, unveiling strong adsorption. Further, the effect of clustering and dispersion of Cu atoms on E ads are analyzed using a first-principle-based genetic algorithm, which reveals that clustering of Cu atoms deteriorates the E ads of Xe and Kr. Thus, for experimental realization, a BDG sheet with uniformly dispersed fine Cu particles is proposed as a substrate.