| Summary: | Novel covalent organic framework (COF) composites containing a bipyridine multimetal complex were designed and obtained via the coordination interaction between bipyridine groups and metal ions. The obtained Pt and polyoxometalate (POM)–loaded COF complex (POM–Pt@COF–TB) exhibited excellent oxidation of methane. In addition, the resultant Co/Fe–based COF composites achieved great performance in an electrocatalytic oxygen evolution reaction (OER). Compared with Co–modified COFs (Co@COF–TB), the optimized bimetallic modified COF composites (Co<sub>0.75</sub>Fe<sub>0.25</sub>@COF–TB) exhibited great performance for electrocatalytic OER activity, showing a lower overpotential of 331 mV at 10 mA cm<sup>−2</sup>. Meanwhile, Co<sub>0.75</sub>Fe<sub>0.25</sub>@COF–TB also possessed a great turnover frequency (TOF) value (0.119 s<sup>−1</sup>) at the overpotential of 330 mV, which exhibited high efficiency in the utilization of metal atoms and was better than that of many reported COF-based OER electrocatalysts. This work provides a new perspective for the future coordination of COFs with bimetallic or polymetallic ions, and broadens the application of COFs in methane conversion and electrocatalytic oxygen evolution.
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