Abstract
We explore the thermal oxidation of hyper-cross-linked polymers to enhance their hydrophilicity and efficacy in atmospheric water harvesting. Comprehensive chemical and physical characterizations are used to confirm the successful incorporation of polar oxygen moieties and the preservation of porosity upon thermal treatment. Newly introduced oxygen-based functional groups significantly improve water sorption properties, increasing total water uptake capacities by up to 400% and shifting water uptake onsets to significantly lower relative humidity. We also investigate the regeneration of oxidized hyper-cross-linked polymers after water sorption to probe their potential for multiple water harvesting cycles and reuse. Our findings outline a simple and cost-effective postsynthetic modification route for optimizing porous organic polymers for more sustainable and efficient atmospheric water harvesting.