Development of high-efficiency and low-cost electrocatalyst for oxygen evolution reaction (OER) is very important for use at alkaline water electrolysis. Metal-organic frameworks (MOF) provide a rich platform for designing multi-functional materials due to their controllable composition and ultra-high surface area. Herein, we report our findings in the development of amorphous nickel–cobalt bimetal-organic framework nanosheets with crystalline motifs via a simple “ligands hybridization engineering” strategy. These complexes’ ligands contain inorganic ligands (H₂O and NO₃⁻) and organic ones, hexamethylenetetramine (HMT). Further, we investigated a series of mixed-metal with multi-ligands materials as OER catalysts to explore their possible advantages and features. It is found that the Ni doping is an effective approach for optimizing the electronic configuration, changing lattice ordering degree, and thus enhancing activities of HMT-based electrocatalysts. Also, the crystalline-amorphous boundaries of various HMT-based electrocatalyst can be easily controlled by simply changing amounts of Ni-precursor added. As a result, the optimized ultrathin (Co, 0.3Ni)-HMT nanosheets can reach a current density of 10 mA cm⁻² at low overpotential of 330 mV with a small Tafel slope of 66 mV dec⁻¹. Our findings show that the electronic structure changes induced by Ni doping, 2D nanosheet structure, and MOF frameworks with multi-ligands compositions play critical roles in the enhancement of the kinetically sluggish electrocatalytic OER. The present study emphasizes the importance of ligands and active metals via hybridization for exploring novel efficient electrocatalysts.

开发用于氧气析出反应（OER）的高效，低成本的电催化剂对于在碱性水电解中的应用非常重要。金属有机框架（MOF）由于其可控的成分和超高的表面积，为多功能材料的设计提供了一个丰富的平台。在这里，我们通过简单的“配体杂交工程”策略报告了我们在具有晶体图案的无定形镍钴双金属有机骨架纳米片的开发中所取得的发现。这些复合物的配体包含无机配体（H ₂ O和NO ₃ ^-）和有机亚甲基六亚甲基四胺（HMT）。此外，我们研究了多种混合金属与多配体材料作为OER催化剂，以探索其可能的优点和特征。发现Ni掺杂是用于优化电子构型，改变晶格有序度并因此增强HMT基电催化剂的活性的有效方法。而且，通过简单地改变Ni前体的添加量，可以容易地控制各种基于HMT的电催化剂的晶体-非晶边界。结果，经过优化的超薄（Co，0.3Ni）-HMT纳米片可以在330 mV的低过电势和66 mV dec ^-1的小Tafel斜率下达到10 mA cm ^-2的电流密度。我们的发现表明，由Ni掺杂，2D纳米片结构和具有多配体组成的MOF骨架引起的电子结构变化在增强动力学迟缓的电催化OER中起着关键作用。本研究强调了配体和活性金属通过杂交对探索新型有效电催化剂的重要性。