Single-site heterogeneous catalysts play an increasingly significant role in various applications due to their high activity, high selectivity, and the maximized atomic utilization efficiency. From a computational perspective, the well-defined and isolated active site in single-site catalysts make elucidating reaction mechanisms relatively straightforward, enabling rational design of catalysts via developing composition-structure-reactivity relationships. In this talk, I will present our work of applying quantum mechanical simulations, i.e., density functional theory, to design different types of single-site catalysts for new energy and sustainability applications. I will begin with discussing graphene-based single atom catalysts – dispersing single metal atom coordinated with dopants on graphene – for electrochemical carbon dioxide upgrading, that can convert the most prevalent greenhouse gas to valuable fuels and chemical feedstocks using excess renewable electricity. I will talk about discovering single atom alloy catalysts – dispersing the minimum amount of an active metal in the surface layer of a less reactive host metal – for direct methane activation to multi-carbon hydrocarbons, that can make good use of earth-abundant resources without resorting to further petroleum extraction.
