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Effective CO<jats:sub>2<\/jats:sub> capture technologies are urgently needed, particularly for the selective removal of CO<jats:sub>2<\/jats:sub> from industrial gas streams, such as flue gas and biogas, which often contain impurities like N<jats:sub>2<\/jats:sub> and CH<jats:sub>4<\/jats:sub>. In this study, we report the design and synthesis of novel molecularly imprinted polymers (MIPs) using 4\u2010vinylpyridine (4VP) and methacrylic acid (MAA) as functional monomers, and thiophene (Th) and formaldehyde (HC) as molecular templates. The MIPs were specifically engineered to create selective molecular cavities within a nanoporous polymer matrix for the efficient capture of CO<jats:sub>2<\/jats:sub>. By adjusting the molar ratios of the template to functional monomers, we optimized the molecular imprinting process to enhance CO<jats:sub>2<\/jats:sub> selectivity over N<jats:sub>2<\/jats:sub> and CH<jats:sub>4<\/jats:sub>. The resulting MIPs exhibited outstanding performance, with a maximum CO<jats:sub>2<\/jats:sub>\/N<jats:sub>2<\/jats:sub> selectivity of 153 at 25\u2005bar and CO<jats:sub>2<\/jats:sub>\/CH<jats:sub>4<\/jats:sub> selectivity of 25.3 at 1\u2005bar, significantly surpassing previously reported porous polymers and metal\u2010organic frameworks (MOFs) under similar conditions. Furthermore, we conducted heat of adsorption studies, which revealed the strong and selective interaction of CO<jats:sub>2<\/jats:sub> with the imprinted cavities, confirming the superior adsorption properties of the synthesized MIPs. The study demonstrates that molecular imprinting can effectively enhance both CO<jats:sub>2<\/jats:sub> capture capacity and selectivity, providing a cost\u2010efficient and scalable solution for industrial CO<jats:sub>2<\/jats:sub> separation and purification processes.<\/jats:p>","DOI":"10.1002\/asia.202401205","type":"journal-article","created":{"date-parts":[[2024,11,18]],"date-time":"2024-11-18T02:54:24Z","timestamp":1731898464000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Molecular Imprinting as a Tool for Exceptionally Selective Gas Separation in Nanoporous Polymers"],"prefix":"10.1002","volume":"20","author":[{"given":"Jaewoo","family":"Park","sequence":"first","affiliation":[{"name":"Department of Chemistry Ulsan National Institute of Science and Technology  44191 Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minji","family":"Jung","sequence":"additional","affiliation":[{"name":"Department of Chemistry Ulsan National Institute of Science and Technology  44191 Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sally E. 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