Sluggish reaction kinetics of oxygen evolution reaction (OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_2−xNi_xO₄ (0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic (FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni³⁺ increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_1.6Ni_0.4O₄ shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe₂O₄ and unactivated ZnFe_1.6Ni_0.4O₄, and even superior to the benchmark IrO₂ under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe₂O₄. We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.

由于多步质子耦合电子转移和自旋收缩导致析氧反应（OER）反应动力学缓慢，限制了大多数报道的催化剂的整体效率。在此，我们使用模拟的ZnFe _{2− x} Ni _x O ₄ (0 ≤ x ≤ 0.4)尖晶石氧化物，旨在通过结合铁磁(FM)有序通道的构建和高活性重构物种的生成来开发更好的OER电催化剂。对称性破缺的 Fe-O-Ni 结构的数量与 FM 有序电子转移通道的形成有关。^{同时，随着Ni 3+}的数量增加，形成更多的配体孔，有利于重定向表面重建。电活化的ZnFe _1.6 Ni _0.4 O ₄显示出最高的比活度，分别比ZnFe ₂ O ₄和未活化的ZnFe _1.6 Ni _0.4 O ₄高13倍和2.5倍，甚至在过电位下优于基准IrO ₂ 350毫伏。施加外磁场可以使电子自旋更加排列，活性可进一步提高至ZnFe ₂ O _4的39倍。我们提出，FM/顺磁界面处有趣的FM交换场相互作用可以将FM有序通道穿透到重建的羟基氧化物层中，从而激活羟基氧化物层作为自旋过滤器，以加速自旋选择性电子转移。这项工作为开发用于水氧化和其他自旋禁止反应的高效自旋电子催化剂提供了新的指导。