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Enhancing the kinetics of electrocatalytic water splitting, including the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), under alkaline conditions is of key importance for producing high purity and renewable hydrogen on a large scale. Owing to their unique structural features, two-dimensional (2D) heterostructures have been regarded as promising next-generation electrocatalysts for overall water splitting. Herein, we successfully synthesized three-dimensional (3D) flower-like Co–Ni–P/MoS2 heterostructural hybrid spheres assembled from heterostructural 2D nanosheets. Benefiting from well-exposed interfaces and favorable diffusion channels, the as-prepared 3D flower-like Co–Ni–P/MoS2 heterostructural hybrid spheres manifest excellent overall water splitting performance in an alkaline solution with a low Tafel slope of 71 and 41 mV dec−1 for oxygen and hydrogen evolution reactions, and show significantly improved long-term durability. Furthermore, the 3D flower-like Co–Ni–P/MoS2 heterostructural hybrid spheres used in both the anode and cathode show a low cell voltage of 1.53 V at a 10 mA cm−2 current density. Using DFT calculations, we found the outstanding chemisorption of hydrogen and oxygen-containing intermediates making Co–Ni–P/MoS2 heterostructures an efficient bifunctional overall electrochemical water splitting catalyst. In summary, this work opens up an important direction for exploring efficient and durable bifunctional electrocatalysts for the overall water splitting. [ABSTRACT FROM AUTHOR]

Flower-like P-doped graphitic carbon nitride (g-C3N4) with a high surface area and porosity has been prepared via a facile, template-free, cost-effective and thermal copolymerization route, using phosphoric acid as the phosphorus source and a cyanuric acid–melamine complex as the supramolecular precursor. It could be found that phosphoric acid could stabilize the three-dimensional character of the as-prepared P-doped g-C3N4 and the g-C3N4 micro-flower consisted of ultrathin nanosheets which possessed abundant mesopores. The unique structure, combined with phosphorus heteroatom doping, promoted the utilization of visible light and improved the separation and mobility of photogenerated charges. The obtained P-doped g-C3N4 exhibited prominent photocatalytic performance in the water splitting for the hydrogen evolution reaction under visible light irradiation. The hydrogen evolution rate reached 256.4 μmol h−1, almost 24 times higher than that of pristine g-C3N4. Meanwhile, a possible mechanism for photocatalytic hydrogen evolution was proposed according to the results. [ABSTRACT FROM AUTHOR]