Zhao Xu, Shao Yiqun, Cai Junjie, Yue Xin, Huang Shaoming
Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China.
School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China.
ACS Appl Mater Interfaces. 2025 Jun 25;17(25):36698-36705. doi: 10.1021/acsami.5c05725. Epub 2025 Jun 14.
Developing high-performance electrocatalysts for the oxygen evolution reaction (OER) in an acidic environment is crucial for practical application in proton exchange membrane water electrolyzers (PEMWE). Due to its favorable performance in an acidic environment, spinel-type CoO has drawn considerable attention, although it remains inferior to precious metal-based electrocatalysts. In this study, we demonstrate that the catalytic activity and stability of CoO can be enhanced by doping Zr into the octahedral interstices of CoO, which effectively triggers the fast lattice oxygen-mediated mechanism (LOM). Thus, as-fabricated Zr-doped CoO (ZrCoO) exhibits efficient activity and fast kinetics in an acidic OER. ZrCoO demonstrates excellent stability by maintaining a current density of 100 mA cm for 60 h. In addition, electrochemical tests and theoretical calculations prove that doping Zr into the lattice of CoO can enhance the hybridization of the Co d and O p orbitals. This significantly optimizes the adsorption of intermediates during the AEM pathway and further triggers the LOM pathway, ultimately facilitating the OER process.
开发用于酸性环境中析氧反应（OER）的高性能电催化剂对于质子交换膜水电解槽（PEMWE）的实际应用至关重要。由于其在酸性环境中的良好性能，尖晶石型CoO尽管仍不如贵金属基电催化剂，但已引起了相当大的关注。在本研究中，我们证明通过将Zr掺杂到CoO的八面体间隙中可以提高CoO的催化活性和稳定性，这有效地触发了快速的晶格氧介导机制（LOM）。因此，制备的Zr掺杂CoO（ZrCoO）在酸性OER中表现出高效的活性和快速的动力学。ZrCoO通过在60小时内保持100 mA cm的电流密度而表现出优异的稳定性。此外，电化学测试和理论计算证明，将Zr掺杂到CoO晶格中可以增强Co d和O p轨道的杂化。这显著优化了AEM途径中中间体的吸附，并进一步触发了LOM途径，最终促进了OER过程。
