Tailoring Surface Adsorption and Reactivity of Fullerene-Based Compounds: A Theoretical Probe into C2–Gas–Fullerene Surface Interactions

Abstract

Density functional theory investigations of palladium and nickel substituted fullerenes (C59M; M = Pd/Ni) were carried out probing the changes in their surface adsorption potential. Structure and bonding in the proposed heterofullerenes were established with insights into metal–carbon bond character, stability, and adsorption potential. C2-gases were used as probe gases for adsorption tests. Adsorption of acetylene, ethylene, and ethane was studied with different sites over pure and heterofullerenes. Adsorption of acetylene was stronger than the adsorption of ethylene and ethane over C60 with the bridge site sharing hexagonal rings being the energetically favored adsorption site. Surface modification of the fullerene molecule with a foreign metal enhanced the gas-substrate (C2-heterofullerene) interactions. Enhanced surface interactions and differential adsorption behavior of different heterofullerenes made them potential candidates as selective acetylene hydrogenation catalysts. Free energy landscapes fo...