Unveiling the mechanism of CO oxidation catalyzed by sulfur-doped fullerenes with the DFT calculations

As an important intermediate for dual carbon targets, catalytic CO oxidation under mild conditions has received sufficient attention, as the reaction mechanism is directly related to the type of employed catalyst. High performance computing is performed with density functional theory to elucidate the mechanism of CO oxidation catalyzed by sulfur doped fullerene (C_60-xS_x (x = 1 ∼ 3)). The total activation energy for the first CO oxidation on C₅₉S, C₅₈S₂, and C₅₇S₃ increases gradually, as implies that the CO oxidation on C₅₉S should be easier than those on the other two dopants. Distinct electrons (0.852 e and 1.479 e) are transferred to oxygen atoms (O₂) from C₅₉S with the adsorption of O₂ and CO. There is no synergistic effect for the doping S atoms. All elementary reactions on C₅₉S are exothermic processes. This means that C₅₉S is a potential material for addressing environmental protection issues and H₂ purification for fuel cell applications.