Rational development of high-performance and cost-effective electrocatalysts for the oxygen evolution reaction (OER) is of particular importance for renewable energy conversion and storage technologies. Herein, we developed a facile and easily scalable hard-template strategy to fabricate hierarchical Ni/Ni_0.2Mo_0.8N nanosheets (~4.37 nm in thickness) in situ coupled with N-doped carbon (Ni/Ni_0.2Mo_0.8N@N-C) as an efficient electrocatalyst for the OER. The elaborate construction of Ni/Ni_0.2Mo_0.8N can validly regulate the electronic structure, increase the number of active sites, and facilitate diffusion kinetics. Benefiting from the coupling effect between hierarchical Ni/Ni_0.2Mo_0.8N and the N-carbon matrix, the resultant Ni/Ni_0.2Mo_0.8N@N-C exhibits excellent OER performance in alkaline media, including a low overpotential of 260 mV at 10 mA cm⁻², a small Tafel slope of 46 mV dec⁻¹, as well as remarkable stability for long-term electrolysis operation, significantly exceeding the findings for most previously reported OER electrocatalysts. Theoretical studies demonstrate that incorporation of Ni into Ni_0.2Mo_0.8N can effectively optimize water adsorption energy and enhance electronic states density near the Fermi level, which is conducive to accelerating the OER process. This work underlines a rational and new perspective for designing inexpensive and robust Mott-Schottky electrocatalysts toward OER for energy storage and conversion devices.

合理开发用于氧气析出反应（OER）的高性能且具有成本效益的电催化剂对于可再生能源转化和存储技术尤为重要。本文中，我们开发了一种简便且易于扩展的硬模板策略，以在原位与掺N的碳（Ni / Ni _0.2 Mo _0.8 N @ NC）耦合地制造分层的Ni / Ni _0.2 Mo _0.8 N纳米片（厚度约4.37 nm ）。作为OER的高效电催化剂。Ni / Ni _0.2 Mo _0.8的精细构造N可以有效地调节电子结构，增加活性位点的数量，并促进扩散动力学。得益于分层Ni / Ni _0.2 Mo _0.8 N与N-碳基体之间的耦合效应，所得的Ni / Ni _0.2 Mo _0.8 N @ NC在碱性介质中表现出出色的OER性能，包括在10 mA下的低过电势为260 mV厘米^-2，46毫伏分解的小塔菲尔斜率^-1，以及用于长期电解操作显着的稳定性，显著超过了大多数的发现以前报道OER电催化剂。理论研究表明Ni掺入Ni _0.2 Mo _0.8氮可以有效地优化水的吸附能并提高费米能级附近的电子态密度，这有利于加速OER过程。这项工作为设计面向储能和转换装置的OER的廉价且坚固的Mott-Schottky电催化剂奠定了合理和崭新的视角。