Rational design of MoS2-supported single-atom catalysts for enhancing phenol deoxygenation: Unveiling synergistic electronic-geometric effects and a universal structure-activity descriptor

Exploring rationally descriptor is pivotal yet challenging in designing single atom catalysts. By doping single atoms (such as 3d, 4d and 5d transition metals) on the MoS 2 edge, efficient activation of the C-O bond in phenol is achieved. The study finds that the doped metal not only modulates the electronic structure of the C-O bond through electron effects but also restricts the adsorption mode of phenol through geometric effects. Based on these findings, a simple linear relationship Ψ , defined as degree-of-cleavage descriptor, was proposed. This descriptor quantitatively captures the combined impact of electronic and geometric effects and establishes a direct correlation between the descriptor and catalytic activity. Importantly, it comprehensively accounts for the combined effects stemming from the metal atoms in the active center and the MoS 2 edge support. • Designed an edge-confined Fe@MoS 2 for bio-oil conversion to aromatic products. • Proposed a new descriptor, Ψ , linking activity to catalyst structure in TM@MoS 2 . • Descriptor Ψ simplifies the selection of dopant atoms for catalyst design.