近日，中国科学院上海应用物理研究所李炯团队揭示了非晶氧化物的非常规两步结构重构克服电催化剂的活性-稳定性权衡。2025年8月6日出版的《美国化学会杂志》发表了这项成果。

通过结构重构活化氧化催化剂中的晶格氧是优化氧化还原体系催化性能的关键。然而，在电化学O₂演化过程中，电化学重构之前的结构转变及其对结构不均匀性的影响一直没有得到充分的了解。

研究组通过自发和电化学体重构激活了w掺杂Co-Fe无定形氧化物的晶格氧。化学态演化研究表明，重构的活性γ-层状双氢氧化物（LDH）具有局部结构不均匀的特点，促进了活性非键氧态的形成，实现了Co³⁺催化的O₂演化。该催化剂在1 A cm^-2下的电池电压为1.69 V，在阴离子交换膜水电解槽中稳定运行600 h。

利用原位光谱技术，研究组在重建过程中建立了Co离子氧化态、相结构和晶格氧活化之间的动态相关性。值得注意的是，研究组提供了控制催化剂活性和稳定性的电位依赖机制转变的第一个实验证据。这些发现加深了他们对电催化剂结构-性能关系的理解，并强调了化学状态演化在催化过程中的关键作用。

附：英文原文

Title: Overcoming the Activity-Stability Trade-Off in Electrocatalysts via Unconventional Two-Step Structural Reconstructions of Amorphous Oxides

Author: Guichen Gao, Guangshe Li, Taotao Huang, Jiawei Wan, Zhibin Geng, Haitong Tang, Xu Zhao, Shilong Fu, Luyi Sun, Jiong Li, Liping Li

Issue&Volume: August 5, 2025

Abstract: The activation of lattice oxygen in oxide catalysts via structural reconstruction is critical for optimizing the catalytic performance in oxidation–reduction systems. However, in electrochemical O2 evolution, the structural transformations preceding electrochemical reconstruction and their impact on the resulting structural inhomogeneity have long remained insufficiently understood. Here, we activate the lattice oxygen of the W-doped Co–Fe amorphous oxide through spontaneous and electrochemical bulk reconstructions. Chemical state evolution studies reveal that the reconstructed active γ-layered double hydroxide (LDH), characterized by local structural inhomogeneity, promotes the formation of reactive nonbonding oxygen states, achieving Co3+-catalyzed O2 evolution. The catalyst demonstrates a cell voltage of 1.69 V at 1 A cm–2 with stable operation for 600 h in anion-exchange membrane water electrolyzers. Using in situ spectroscopic techniques, we establish dynamic correlations among Co ion oxidation states, phase structure, and lattice oxygen activation during reconstruction. Notably, we provide the first experimental evidence of a potential-dependent mechanistic transition governing both the activity and the stability of the catalyst. These findings deepen our understanding of structure-performance relationships in electrocatalysts and highlight the pivotal role of the chemical state evolution in catalytic processes.

DOI: 10.1021/jacs.5c04970

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c04970