Electrocatalytic hydrogen evolution reaction, the cornerstone of the emerging hydrogen economy, can be essentially facilitated by robustly heterostructural electrocatalysts. Herein, we report a highly active and stably heterostructural electrocatalyst consisting of NiCoP nanowires decorated with CoP nanoparticles on a nickel foam (NiCoP–CoP/NF) for effective hydrogen evolution. The CoP nanoparticles are strongly interfaced with NiCoP nanowires producing abundant electrocatalytically active sites. Combined with the integrated catalyst design, NiCoP–CoP/NF affords a remarkable hydrogen evolution performance in terms of high activity, enhanced kinetics, and outstanding durability in an alkaline electrolyte, superior to most of the Co (or Ni)-phosphide-based catalysts reported previously. Density functional theory calculations demonstrate that there is an interfacial effect between NiCoP and CoP, which allows a preferable hydrogen adsorption and thus contributes to the significantly enhanced performance. Furthermore, an electrolyzer employing NiCoP–CoP/NF as the cathode and RuO2/NF as the anode (NiCoP–CoP/NF||RuO2/NF) exhibits excellent water-splitting activity and outstanding durability, which is comparable to that of the benchmark Pt–C/NF||RuO2/NF electrolyzer.

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The decomposition of water into hydrogen and oxygen is an effective method to generate new energy. How to develop highly efficient catalysts with low cost for the hydrolysis of water is a huge challenge. Herein, heterogeneous CDs/NiCo2S4/Ni3S2 nanorods were constructed on nickel foam (CDs/NiCo2S4/Ni3S2/NF) by Co ion exchange on carbon dots (CDs) and sulfur codoped nickel foam (NF). The designed CDs/NiCo2S4/Ni3S2/NF as a self-standing electrocatalyst shows excellent electrocatalytic properties. In the hydrogen evolution reaction process, the current density can reach 10 mA cm–2 only with the overpotential of 0.127 V. During the oxygen evolution reaction process, overpotential of 0.116 V is enough to achieve the same current density. Meanwhile, the CDs/NiCo2S4/Ni3S2/NF electrode can serve as both anode and cathode in alkaline electrolyte, and overpotential of 1.50 V can drive the overall water splitting with superior durability. Such excellent properties are mainly due to (1) a large number of exposed active sites provided by carbon dots modified transition metal chalcogenide (NiCo2S4 and Ni3S2), (2) the changed electronic structure caused by the incorporation of carbon dots and Co ions and the synergistic effect between NiCo2S4 and Ni3S2, (3) the accelerated electron transfer and mass transfer processes owing to the hierarchical structure formed by 3D nickel foam and one-dimensional CDs/NiCo2S4/Ni3S2/NF nanorods. This study can facilitate with the production of efficient and non-noble metal catalysts for overall water splitting.

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