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Covalent organic frameworks (COFs)-based nanoreactors have attracted broad interest in many fields due to their void-confinement effects. However, the inherent drawback of conventional nanoreactors is the lack of internal active sites, which limits their widespread utilization. Herein, we report the construction of hierarchical COF (EB-TFP) nanoreactor with pre-synthesized polyoxometalates (POM, [PV2W10O40]5– (PV2W10)) clusters encapsulated inside of COF (POM@COF). PV2W10@EB-TFP anchors nucleophilic-group (Br– ions) and PV2W10 anion cluster within the COF framework via electrostatic interactions, which not only simplifies the reaction system but also enhances catalytic efficiency. The reaction performance of the PV2W10@EB-TFP nanoreactor can be tuned to achieve excellent catalytic activity in CO2 cycloaddition reaction (CCR) for ~ 97.63% conversion and ~ 100% selectivity under visible light irradiation. A mechanistic study based on density functional theory (DFT) calculations and in-situ characterization was also carried out. In summary, we have reported a method for achieving the uniform dispersion of POM single clusters into COF nanoreactor, demonstrating the potential of POM@COF nanoreactor for synergistic photothermal catalytic CO2 cycloaddition.
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