Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, PR China; Beijing Key Laboratory of Chemical Power Source and Green Catalysis, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, PR China.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, PR China; Beijing Key Laboratory of Chemical Power Source and Green Catalysis, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, PR China.
J Colloid Interface Sci. 2023 Oct 15;648:701-708. doi: 10.1016/j.jcis.2023.05.205. Epub 2023 Jun 8.
Transition metal oxides have been extensively investigated for oxygen evolution reaction (OER). While the introduction of oxygen vacancies (V) was found to be an effective way to enhance the electrical conductivity and the OER electrocatalytic activity of transition metal oxides, the oxygen vacancies are easily damaged during the long-term catalytic process, resulting in rapid decay of the electrocatalytic activity. Herein, we proposed the strategy of dual-defect engineering to enhance the catalytic activity and stability of NiFeO by filling the oxygen vacancies of NiFeO with phosphorus atoms. The filled P atoms could form coordination with iron and nickel ions to compensate the coordination number and optimize the local electronic structure, which not only enhances the electrical conductivity but also improves the intrinsic activity of the electrocatalyst. Meanwhile, the filling of P atoms could stabilize the V and thus improving the cycling stability of the material. The theoretical calculation further demonstrates that the improvement in conductivity and intermediate binding by P refilling remarkably contributes to enhancing the OER activity of NiFeO-V-P. Benefiting from the synergistic effect of filled P atoms and V, the derived NiFeO-V-P exhibits fascinating activity with ultra-low OER overpotentials of 234 and 306 mV at 10 and 200 mA cm, together with the good durability for 120 h at relatively high current density of 100 mA cm. This work sheds light on the design of high-performance transition metal oxide catalysts through defect regulation in the future.
过渡金属氧化物在析氧反应（OER）中得到了广泛的研究。虽然氧空位（V）的引入被发现是提高过渡金属氧化物电导率和 OER 电催化活性的有效方法，但氧空位在长期催化过程中很容易被破坏，导致电催化活性迅速衰减。在此，我们提出了通过用磷原子填充 NiFeO 的氧空位来增强 NiFeO 催化活性和稳定性的双缺陷工程策略。填充的 P 原子可以与铁和镍离子形成配位，以补偿配位数并优化局部电子结构，这不仅提高了电导率，而且提高了电催化剂的本征活性。同时，填充的 P 原子可以稳定 V，从而提高材料的循环稳定性。理论计算进一步表明，通过 P 原子的填充来提高电导率和中间结合能显著有助于提高 NiFeO-V-P 的 OER 活性。受益于填充 P 原子和 V 的协同效应，所得到的 NiFeO-V-P 在 10 和 200 mA cm 时，具有超低的 OER 过电位，分别为 234 和 306 mV，并且在相对较高的电流密度 100 mA cm 时具有良好的耐久性，可稳定运行 120 小时。这项工作为通过缺陷调节设计高性能过渡金属氧化物催化剂提供了思路。
