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

Constructing catalysts that simultaneously contain 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 addressed the superiority of hybrid single-atom/nanocluster sites.