Surface Modification Strategy for Promoting the Performance of Non-noble Metal Single-Atom Catalysts in Low-Temperature CO Oxidation

As a bridge between homogeneous and heterogeneous catalyses, single-atom catalysts (SACs), especially the noble metal atoms, have received extensive attention from both the fundamental and applied perspectives recently. High cost and difficulty in synthesis are considerable factors, however, limiting the development and practical applications of SACs. Thus, seeking for non-noble SACs for substituting the noble ones is not only of vital importance but also a long-standing challenge. Herein, a surface modification strategy by introducing an oppositely charged dopant and inducing the charge transfer between the SAC and the substrate was proposed to improve the stability and catalytic performance of the non-noble Cu SAC. Using first-principles density functional theory (DFT) calculations, it was demonstrated that the introduction of C in the MoS₂ monolayer (C:MoS₂, experimentally available) can assist in stabilizing Cu and make it more positively charged, which will facilitate the adsorption of the reactants and further enhance the activity for CO oxidation. Strikingly, our results show that CO oxidation over Cu-C:MoS₂ is more favorable than over the Pt atom deposited on the pristine MoS₂ (Pt-MoS₂), exhibiting its potential in noble metal substitution and low-temperature CO oxidation. Additionally, Cu-C:MoS₂ was observed to have a response to visible light, which manifests that it may be a promising photocatalyst. The strategy proposed here provides an efficient route to regulate the electronic structures of SACs through charge transfer, which further promotes the reactivity of the non-noble metal SACs. We hope that this strategy can contribute to design more SACs with low cost and high efficiency, which will be beneficial for their practical applications.