A DFT study of arsine adsorption on palladium doped graphene: Effects of palladium cluster size

Abstract In this study, we have investigated the size effects of palladium (Pd) doped single-vacancy defective graphene (SDG) surface to the adsorption of AsH3 and its dehydrogenated products on Pd using density functional theory calculations. Here, Pd cluster binding study revealed that Pd6 nanocluster bound strongest to the SDG surface, while adsorption of AsHx (x = 0–3) on the most stable Pdn doped SDG showed that dehydrogenated arsine compounds adsorbed onto the surface stronger than the pristine AsH3 molecule. Charge analysis revealed that considerable amount of charge migration from Pd to dehydrogenated arsine molecules after adsorption may constitute strong adsorption for dehydrogenated arsine. In addition, study of thermodynamic pathways of AsH3 dehydrogenation on Pdn doped SDG adsorbents indicated that Pd cluster doping on SDG adsorbent tends to be thermodynamically favorable for AsH3 decomposition than the single-Pd atom doped SDG. Hence, our study has indicated that Pd6 clusters doped SDG is more advantageous as adsorbent material for AsH3 removal.