The exploration of high-efficiency bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has long been challenging. The rational design of a catalyst by constructing heterostructures and a doping element are possibly expected to achieve it. Herein, the utilization of flower-like Fe/C-doped-MoS2/Ni3S2-450 spherical structural materials for electrocatalytic HER and OER is introduced in this study. The carboxyferrocene-incorporated molybdenum sulfide/nickel sulfide (MoySx/NiS) nanostructures were prepared by solvothermal method. After annealing, the iron and carbon elements derived from ferrocenecarboxylic acid enhanced the electrical transport performance and provided rich electronic sites for HER and OER in alkaline media. Specifically, the optimized flower-like Fe/C-doped-MoS2/Ni3S2-450 exhibited efficient bifunctional performance in alkaline electrolyte, with low overpotentials of 188 and 270 mV required to deliver a current density of 10 mA cm−2 for HER and OER, respectively. This work provides valuable insights for the rational design of energy storage and conversion materials by the incorporation of transition metal and carbon elements into metal sulfide structures utilizing metallocene.

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The slow kinetics of the oxygen evolution reaction (OER) is one of the significant reasons limiting the development of electrochemical hydrolysis. Doping metallic elements and building layered structures have been considered effective strategies for improving the electrocatalytic performance of the materials. Herein, we report flower-like nanosheet arrays of Mn-doped-NiMoO4/NF (where NF is nickel foam) on nickel foam by a two-step hydrothermal method and a one-step calcination method. The doping manganese metal ion not only modulated the morphologies of the nickel nanosheet but also altered the electronic structure of the nickel center, which could be the result of superior electrocatalytic performance. The Mn-doped-NiMoO4/NF electrocatalysts obtained at the optimum reaction time and the optimum Mn doping showed excellent OER activity, requiring overpotentials of 236 mV and 309 mV to drive 10 mA cm−2 (62 mV lower than the pure NiMoO4/NF) and 50 mA cm−2 current densities, respectively. Furthermore, the high catalytic activity was maintained after continuous operation at a current density of 10 mA cm−2 of 76 h in 1 M KOH. This work provides a new method to construct a high-efficiency, low-cost, stable transition metal electrocatalyst for OER electrocatalysts by using a heteroatom doping strategy.

Schematic illustration of the proposed reaction mechanism based on the CDAC/W18O49 composite.

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