Unified Catalyst for Efficient and Stable Hydrogen Production by Both the Electrolysis of Water and the Hydrolysis of Ammonia Borane

Abstract Hydrogen is a promising energy carrier for a future sustainable energy economy. The two most promising routes for its large‐scale production in high purity are electrocatalytic water splitting and chemical release from hydrogen‐storage materials. The rational design and synthesis of robust catalysts for hydrogen evolution are crucial stages in the development of hydrogen as an energy source. This work reports the production of a novel hydrogen evolution catalyst consisting of uniform hollow porous carbon spheres loaded with ruthenium nanoclusters via a simple hydrothermal process at low temperature. The catalyst not only exhibits extraordinary catalytic activity for the hydrogen evolution reaction, with extremely low overpotentials at all pH values, but also shows outstanding activity for hydrolysis of ammonia borane (AB) with a high turnover frequency. Furthermore, the catalyst remains stable during both reactions, thus allowing one unified catalyst to facilitate hydrogen generation by two different methods for highly efficient and superstable hydrogen production. This work may provide a template method for rational design and fabrication of various metals/N‐doped carbon catalysts that promote hydrogen production through both the electrolysis of water and the hydrolysis of AB, which will advance the development of hydrogen as an energy source.