Dynamic structural evolution of catalyst active sites is crucial to for transition metal-catalyzed oxygen evolution reaction (OER). Yet, the elucidation of their mechanism behind the compressive-strain-induced reconstruction during OER process remains enigmatic. Here, we construct a bowl-like cobalt-based metal-organic frameworks (BL-Co-MOFs) catalyst with compressive strain to investigate the effect of strain on the structural evolution process and the OER mechanism. techniques directly observe that compressive strain exists in the reconstruction of the potential-driven CoOOH-like active phase with contractile interatomic CoCo distance, promoting a direct OO radical coupling over the Co sites (Co−O−O−Co) during the OER process. This disrupts the constrains of the inherent linear scaling relationship and achieves the kinetic-faster oxide path mechanism (OPM) during OER process. Consequently, the BL-Co-MOFs exhibit a huge mass activity of 12516 A g and a large turnover frequency of 6888 h at a low overpotential of 275 mV (300 mA cm).

中文翻译：

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追踪压缩应变在水氧化反应中碗状 Co-MOF 结构演化中的作用


催化剂活性位点的动态结构演化对于过渡金属催化的析氧反应（OER）至关重要。然而，OER 过程中压缩应变诱导重建背后的机制的阐明仍然是个谜。在这里，我们构建了一种具有压缩应变的碗状钴基金属有机框架（BL-Co-MOF）催化剂，以研究应变对结构演化过程和OER机制的影响。技术直接观察到压缩应变存在于具有收缩原子间 CoCo 距离的电势驱动的 CoOOH 类活性相的重建中，促进了 OER 过程中 Co 位点 (Co−O−O−Co) 上的直接 OO 自由基耦合。这打破了固有的线性比例关系的限制，并在 OER 过程中实现了动力学更快的氧化物路径机制 (OPM)。因此，BL-Co-MOF 在 275mV (300mAcm) 的低过电位下表现出 12516A g 的巨大质量活性和 6888h 的大周转频率。