Despite the challenges associated with the synthesis of flexible metal‐covalent organic frameworks (MCOFs), these offer the unique advantage of maximizing the atomic utilization efficiency. However, the construction of flexible MCOFs with flexible building units or linkages has rarely been reported. In this study, novel flexible MCOFs are constructed using flexible building blocks and copper clusters with hydrazone linkages. The heterometallic frameworks (Cu, Co) are prepared through the hydrazone linkage coordination method and evaluated as catalysts for the oxygen evolution reaction (OER). Owing to the spatial separation and functional cooperation of the heterometallic MCOF catalysts, the as‐synthesized MCOFs exhibited outstanding catalytic activities with an overpotential of 268.8 mV at 10 mA cm–2 for the OER in 1 M KOH, which is superior to those of the reported covalent organic frameworks (COFs)‐based OER catalysts. Theoretical calculations further elucidated the synergistic effect of heterometallic active sites within the linkages and frameworks, contributing to the enhanced OER activity. This study thus introduces a novel approach to the fundamental design of flexible MCOF catalysts for the OER, emphasizing their enhanced atomic utilization efficiency.

中文翻译：

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具有铜簇的柔性腙连接金属共价有机框架用于高效电催化析氧反应


尽管柔性金属共价有机骨架（MCOF）的合成面临挑战，但它们提供了最大化原子利用效率的独特优势。然而，利用灵活的建筑单元或连接装置建造灵活的MCOF却鲜有报道。在这项研究中，新型柔性 MCOF 是使用柔性构件和带有腙键的铜簇构建的。通过腙键配位法制备异金属骨架（Cu、Co），并作为析氧反应（OER）催化剂进行评估。由于异金属MCOF催化剂的空间分离和功能配合，所合成的MCOF表现出出色的催化活性，在10 mA cm-2下在1 M KOH中的OER具有268.8 mV的过电势，优于传统的MCOF催化剂。报道了基于共价有机框架（COF）的OER催化剂。理论计算进一步阐明了连接和框架内异金属活性位点的协同效应，有助于增强OER活性。因此，本研究介绍了一种用于 OER 的柔性 MCOF 催化剂的基本设计的新方法，强调其增强的原子利用效率。