Elucidating and regulating dynamic catalyst reconstruction are crucial for various electrocatalytic reactions. Here, we applied model fittings with operando characterizations to quantify the reconstruction activity (i.e., ability to reconstruct) of layered Co(OH)₂ toward the oxygen evolution reaction (OER). By modulating the intercalation species into Co(OH)₂, we governed distinct reconstruction thermodynamics and kinetics, with diverse mass changes and heterogeneous Co oxidation during the OER. We further established a volcano-type relationship between reconstruction activity and OER activity and identified that a moderate reconstruction activity, achieved by dual-anion intercalation, favored a high OER activity. This might result from its proper basal spacing that regulated the coupled ion (de)intercalation–electron transfer for reconstruction, leading to optimal Co for binding OER intermediates. The optimally reconstructed Co(OH)_1.26Cl_0.08(CO₃)_0.33·0.84 H₂O delivered 1 A cm^–2 at 1.78 V for anion-exchange membrane water electrolysis. This work laid the foundation for modulating reconstruction activities to benefit electrocatalysis.

中文翻译：

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调节钴电极的重构活性以优化水氧化


阐明和调节动态催化剂重构对于各种电催化反应至关重要。在这里，我们应用了具有原位表征的模型拟合来量化层状 Co（OH）₂ 对析氧反应 （OER） 的重建活性（即重建能力）。通过将嵌入物质调节到 Co（OH）₂ 中，我们控制了不同的重建热力学和动力学，在 OER 期间具有不同的质量变化和异质 Co 氧化。我们进一步建立了重建活动和 OER 活动之间的火山型关系，并确定通过双阴离子嵌入实现的适度重建活动有利于高 OER 活性。这可能是由于其适当的基底间距调节了耦合离子（去）插层-电子转移以进行重建，从而产生了结合 OER 中间体的最佳 Co。最佳重构的 Co（OH）_1.26Cl_0.08（CO₃）_0.33·0.84 H₂O 在 1.78 V 下提供 1 A cm^–2 用于阴离子交换膜水电解。这项工作为调节重建活动以利于电催化奠定了基础。