Thanks to tunable physical and chemical properties, two-dimensional (2D) materials have received intensive interest, endowing their excellent electrocatalytic performances for applications in energy conversion. However, their catalytic activities are largely determined by poor adsorption energy and limited active edge sites. Herein, a one-step electrochemical exfoliation strategy was developed to fabricate 2D Ni-doped MoS₂ nanosheets (Ni-EX-MoS₂) with a lateral size of ∼500 nm and thickness of ∼3.5 nm. Profiting from high electrical conductivity and abundant exposing active sites, Ni-EX-MoS₂ catalyst displayed an admirable performance for electrochemical hydrogen evolution reaction (HER) with a low overpotential of 145 mV at 10 mA/cm² as well as a small Tafel slope of 89 mV/dec in alkaline media, which are superior to those of the most reported MoS₂-based electrocatalysts. The formed Ni species with tuning electronic structure played a crucial role as primary active center of Ni-EX-MoS₂, as well as the forming stable 1T/2H phase MoS₂ interface demonstrated a synergistic effect on electrocatalytic HER performance. Further, Ni-EX-MoS₂ was employed as a cathode electrode for alkaline Zn-H₂O battery, which displayed a high power density of 3.3 mW/cm² with excellent stability. This work will provide a simple and effective guideline for design of electrochemically exfoliated transition metal-doped MoS₂ nanosheets to inspire their practical applications in energy catalytic and storage.

由于可调节的物理和化学性质，二维（2D）材料受到了广泛的关注，赋予其在能量转换应用中优异的电催化性能。然而，它们的催化活性很大程度上取决于较差的吸附能和有限的活性边缘位点。在此，我们开发了一种一步电化学剥离策略来制备横向尺寸约为 500 nm、厚度约为 3.5 nm 的二维 Ni 掺杂 MoS ₂纳米片 (Ni-EX-MoS _{2 )。}得益于高导电性和丰富的暴露活性位点，Ni-EX-MoS _{2催化剂在 10 mA/cm} ²下具有 145 mV 的低过电势，在电化学析氢反应 (HER) 中表现出令人赞叹的性能以及在碱性介质中 89 mV/dec 的小 Tafel 斜率，优于报道最多的基于 MoS ₂的电催化剂。_{形成的具有调谐电子结构的Ni作为Ni-EX-MoS 2}的主要活性中心起着至关重要的作用，并且形成稳定的1T/2H相MoS ₂界面对电催化HER性能具有协同作用。此外，Ni-EX-MoS ₂被用作碱性Zn-H ₂ O电池的阴极电极，其显示出3.3 mW/cm ²的高功率密度和优异的稳定性。这项工作将为电化学剥离过渡金属掺杂 MoS _{2的设计提供简单有效的指导。}纳米片以激发其在能量催化和存储中的实际应用。