Pyrolysis‐Free Synthesis of Synergistic Single‐Atom/Nanocluster Electrocatalysts for Hydrogen Evolution

Constructing catalysts that simultaneously containing single atom/metal nanocluster active sites is a promising strategy to enhance the original catalytic behavior and accelerate the catalysis involving multi‐electron reactions or multi‐intermediates. Herein, the pyrolysis‐free synthetic method is developed to integrate single atoms and nanoclusters towards highly satisfactory catalytic performances for both acidic and alkaline hydrogen electrocatalysis. The controllable pyrolysis‐free strategy allows the precise modulation of the active centers, realizing the optimization of the adsorption energy and the regulation of the synergistic active components. Specially, the as‐prepared catalysts with hybrid single‐atom/nanocluster sites exhibited superior catalytic activities for hydrogen evolution in both acidic and alkaline media with low over‐potentials at ‐10 mA cm‐2 of 25 mV and 8.6 mV, respectively, combining with outstanding durability towards high current density and methanol poisoning. This work developed a universal synthetic strategy for the single atom/nanocluster synergy systems and further demonstrated the superiority of heterogeneous components.