Exploring earth‐abundant bifunctional electrocatalysts with high efficiency for water electrolysis is extremely demanding and challenging. Herein, density functional theory (DFT) predictions reveal that coupling Ni with Ni₃C can not only facilitate the oxygen evolution reaction (OER) kinetics, but also optimize the hydrogen adsorption and water adsorption energies. Experimentally, a facile strategy is designed to in situ fabricate Ni₃C nanosheets on carbon cloth (CC), and simultaneously couple with Ni nanoparticles, resulting in the formation of an integrated heterostructure catalyst (Ni–Ni₃C/CC). Benefiting from the superior intrinsic activity as well as the abundant active sites, the Ni–Ni₃C/CC electrode demonstrates excellent bifunctional electrocatalytic activities toward the OER and hydrogen evolution reaction (HER), which are superior to all the documented Ni₃C‐based electrocatalysts in alkaline electrolytes. Specifically, the Ni–Ni₃C/CC catalyst exhibits the low overpotentials of only 299 mV at the current density of 20 mA cm⁻² for the OER and 98 mV at 10 mA cm⁻² for the HER in 1 m KOH. Furthermore, the bifunctional Ni–Ni₃C/CC catalyst can propel water electrolysis with excellent activity and nearly 100% faradic efficiency. This work highlights an easy approach for designing and constructing advanced nickel carbide‐based catalysts with high activity based on the theoretical predictions.

中文翻译：

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Ni纳米粒子与Ni3 C纳米片的协同耦合，可实现高效的总水分解。

探索高效的富含土的双功能电催化剂以进行水电解是一项极为艰巨和艰巨的任务。在此，密度泛函理论（DFT）的预测表明，Ni与Ni ₃ C的偶联不仅可以促进氧释放反应（OER）动力学，而且还可以优化氢吸附和水吸附能。实验上，设计了一种简便的策略来在碳布（CC）上原位制备Ni ₃ C纳米片，并同时与Ni纳米粒子偶联，从而形成集成的异质结构催化剂（Ni–Ni ₃ C / CC）。受益于出色的固有活性以及丰富的活性位点，Ni-Ni ₃C / CC电极对OER和析氢反应（HER）表现出出色的双功能电催化活性，这优于碱性电解质中所有已记录的Ni ₃ C基电催化剂。具体而言，Ni-Ni ₃ C / CC催化剂在1 m KOH中的OER电流密度为20 mA cm ^-2时表现出只有299 mV的低过电势，而在10 mA cm ^-2的电流密度下则为98 mV 。此外，双功能Ni–Ni ₃C / CC催化剂可以以优异的活性和接近100％的法拉第效率推动水电解。这项工作强调了基于理论预测设计和构建具有高活性的高级碳化镍基催化剂的简便方法。