Phenolic Resin‐type Microporous Organic Polymers for High‐Performance Carbon Dioxide Adsorption

Abstract Three new types of Si‐centered porous organic polymer (Si‐POPs) were successfully prepared using phenolic resin‐type chemistry to form C−C bonds. This new family of microporous Si‐POPs manifests as uniform, microporous, spherical particles with a high specific surface area. Notably, Si‐POPs were engineered to possess varying numbers of hydroxyl (−OH) groups by altering the monomer in the synthetic process. Among these materials, the variant with the highest number of hydroxyl groups exhibited ultra‐high CO 2 adsorption capacity, reaching up to 4.3 mmol g −1 at 273 K and 1.0 bar, which surpasses the performance of most porous polymers. Furthermore, Si‐POPs also demonstrated remarkable selectivity adsorption for carbon dioxide over nitrogen (17–50, IAST at 273 K and 1.0 bar). This study not only highlighted the superior CO 2 adsorption properties of Si‐POPs but also explored their potential application in selective gas adsorption.