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An innovative design of a molecularly imprinted phase-change microcapsule (MIM) system for bifunctional applications in waste heat recovery and targeted pollutant removal was reported in this work. This molecularly imprinted system was successfully constructed by encapsulating n-eicosane with a SiO2 base shell through emulsion-templated interfacial polycondensation and then coating a molecularly imprinted polymeric layer with bisphenol A (BPA) as a template molecule through surface free-radical polymerization. The morphology, microstructure, and chemical structure of the resultant molecularly imprinted phase-change microcapsules (MIMs) were characterized, and their phase-change behavior, thermal energy-storage performance, and selective adsorption capability were investigated intensively. The MIMs developed in this study achieved an outstanding latent heat-storage capability with a high capacity more than 165 J/g and also showed an excellent phase-change reliability with a very small fluctuation in phase-change temperatures and enthalpies after 500 thermal cycles. Moreover, the MIMs also presented a high thermal stability over 200 °C and good shape stability up to 120 °C. Most of all, an effective specific recognition capability and high recognition efficiency were achieved for the MIMs due to the formation of BPA-molecular imprinting sites on their surface. As a result, the MIMs exhibited good adsorption selectivity toward the BPA molecules and satisfactory reusability for targeted removal of BPA with a removal efficiency of 61.7% after 10 cycles of the rebinding–elution procedure. In view of a smart combination of thermal energy-storage and selective adsorption functions, the MIMs developed in this study demonstrate a great potential in applications for waste heat recovery and targeted pollutant removal of industrial and domestic wastewaters.

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