Stabilizing and Activating Active Sites: 1T‐MoS₂ Supported Pd Single Atoms for Efficient Hydrogen Evolution Reaction

Abstract

Metallic 1T‐MoS2 with high intrinsic electronic conductivity performs Pt‐like catalytic activity for hydrogen evolution reaction (HER). However, obtaining pure 1T‐MoS2 is challenging due to its high formation energy and metastable properties. Herein, an in situ SO42−‐anchoring strategy is reported to synthesize a thin layer of 1T‐MoS2 loaded on commercial carbon. Single Pd atoms, constituting a substantial loading of 7.2 wt%, are then immobilized on the 1T‐phase MoS2 via Pd─S bonds to modulate the electronic structure and ensure a stable active phase. The resulting Pd1/1T‐MoS2/C catalyst exhibits superior HER performance, featuring a low overpotential of 53 mV at the current density of 10 mA cm−2, a small Tafel slope of 37 mV dec−1, and minimal charge transfer resistance in alkaline electrolyte. Moreover, the catalyst also demonstrates efficacy in acid and neutral electrolytes. Atomic structural characterization and theoretical calculations reveal that the high activity of Pd1/1T‐MoS2/C is attributed to the near‐zero hydrogen adsorption energy of the activated sulfur sites on the two adjacent shells of atomic Pd.