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Engineering the Coordination Interface of Isolated Co Atomic Sites Anchored on N-Doped Carbon for Effective Hydrogen Evolution Reaction.

The regulation of the coordination environment of the central metal atom is considered as an alternative way to enhance the performance of single-atom catalysts (SACs). Herein, we design an electrocatalyst with active sites of isolated Co atoms coordinated with four sulfur atoms supported on N-doped carbon frameworks (Co1-S4/NC), confirmed by high-angle annular dark-field scanning transmission electron microscope (HADDF-STEM) and synchrotron-radiation-based X-ray absorption fine structure (XAFS) spectroscopy. The Co1-S4/NC possesses higher hydrogen evolution reaction (HER) catalytic activity than other Co species and exceptional stability, which exhibits a small Tafel slope of 60 mV dec-1 and a low overpotential of 114 mV at 10 mA cm-2 during the HER in 0.5 M H2SO4 solution. Furthermore, through in situ X-ray absorption spectrum tests and density functional theory (DFT) calculations, we reveal the catalytic mechanism of Co1-S4 moieties and find that the increasing number of sulfur atoms in the Co coordination environment leads to a substantial reduction of the theoretical HER overpotential. This work may point a new direction for the synthesis, performance regulation, and practical application of single-metal-atom catalysts.