Abstract
This study investigates the enhancement of catalytic activity in single-atom catalysts (SACs) through coordination engineering. By introducing non-metallic atoms (X = N, O, or F) into the basal plane of MoS(2) via defect engineering and subsequently anchoring hetero-metallic Ru atoms, we created 10 types of non-metal-coordinated Ru SACs (Ru-X-MoS(2)). Computations indicate that non-metal atom X significantly modifies the electronic structure of Ru, optimizing the hydrogen evolution reaction (HER). Across acidic, neutral, and alkaline electrolytes, Ru-X-MoS(2) catalysts exhibit significantly improved HER performance compared with Ru-MoS(2), even surpassing commercial Pt/C catalysts. Among these, the Ru-O-MoS(2) catalyst, characterized by its asymmetrically coordinated O(2)-Ru-S(1) active sites, demonstrates the most favorable electrocatalytic behavior and exceptional stability across all pH ranges. Consequently, single-atom coordination engineering presents a powerful strategy for enhancing SAC catalytic performance, with promising applications in various fields.