To date, noble metals (e.g., Pt, Pd, and Rh) are regarded as the most efficient materials to catalyze the conversion of H 3O + (acid) and H 2O (alkaline) to H 2 7. Electrocatalytic hydrogen evolution reaction (HER) enabled by renewable electricity holds great promise as a safe, scalable, low-cost, and environmental-friendly pathway for hydrogen production 4, 5, 6. Nowadays the majority of hydrogen is still produced from steam-reformed methane, which is derived from limited fossil resources and greatly increases CO 2 emission. Hydrogen has emerged as a green and sustainable fuel to meet the demand for future global energy 1, 2, 3. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction.

Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Tuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts.

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