近日，中国科学技术大学周敏团队研究了定向无定形到无定形的高效析氧重建。相关论文于2026年3月4日发表在《德国应用化学》杂志上。

为充分挖掘析氧反应的催化潜力，关键在于引导重构过程，使初始非晶态向性能更优的非晶态结构定向演化。

研究组通过单齿封端策略开发了一种非晶态钴配位聚合物预催化剂。原位同步辐射X射线衍射表明，CH₃CN配位破坏了长程拓扑有序性，同时保留了局域结构基元。所获得的亚稳态非晶结构与晶态对应物（-7.441 eV）相比，由于与配体的d-π*强相互作用（能垒低至-8.175 eV），可将自发表面重构引导为非晶态羟基氧化钴活性层。

这种独特的非晶-非晶转变有效激活了亚稳态框架中的晶格氧，使析氧反应路径从吸附质演化机制转变为晶格氧介导机制，从而提升了析氧反应的效率与稳定性。优化后的非晶态aCo在10 mA cm^-2电流密度下的过电位低至186 mV，远低于RuO₂（233 mV）和晶态cCo（308 mV），并在2 A cm^-2的高电流密度下表现出超过100小时的稳定性。该策略为设计下一代析氧反应电催化剂提供了定向表面诱导方法，并为理解晶格氧活性与结构长程无序性之间的关联奠定了理论基础。

附：英文原文

Title: Directed Amorphous-to-Amorphous Reconstruction Toward Efficient Oxygen Evolution

Author: Cheng-Long Peng, Hang Wang, Qian Wang, Hong-Jian Qi, Jian-Yong Zhang, Rui Zhang, He Lin, Wen Wen, Shuang Song, Na Zhang, Yong-Zheng Fang, Fang-Na Dai, Min Zhou

Issue&Volume: 2026-03-04

Abstract: To fully unlock catalytic potential in the oxygen evolution reaction (OER), it is essential to guide the reconstruction process, orienting the evolution from the initial amorphous state into a more potent amorphous structure. We develop an amorphous cobalt coordination polymer (aCo) pre-catalyst via monodentate end-capping. In-situ synchrotron radiation X-ray diffraction reveals that CH3CN coordination disrupts the long-range topological order while preserving local motifs. The obtained metastable amorphous structure redirect spontaneous surface reconstruction into an amorphous cobalt oxyhydroxide (a-CoOOH) active layer due to strong d–π* interactions with the lower energetic barrier (8.175 eV) compared to the crystalline phase on its counterpart (7.441 eV). The unique amorphous-to-amorphous transformation effectively activates lattice oxygen within the metastable framework, switching the OER pathways from the adsorbate evolution mechanism to a lattice oxygen-mediated mechanism and consequently enhancing OER efficiency and stability. The optimized amorphous aCo can achieve an overpotential of 186 mV at 10 mA cm2, much lower than those of RuO2 (233 mV) and crystalline cCo (308 mV), and it demonstrates stability of over 100 h at 2 A cm2. This strategy offers a directed surface-induced approach for designing next-generation OER electrocatalysts, providing fundamental insights into the correlation between lattice oxygen activity and structural long-range disorder.

DOI: 10.1002/anie.202524570

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202524570