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Amine\u2010functionalized sorbents (AFS) achieve high selectivity via strong chemisorption, but suffer from kinetic limitations, pore blocking, and degradation under humid, high\u2010temperature. Hydrogen\u2010bonded organic frameworks (HOFs), enabling rapid and selective transport through ordered supramolecular pores without strong binding, although their weak intermolecular interactions and structural fragility pose challenges. Our review, critically compare AFS and HOF\u2010based membranes, elucidating how chemical functionality, pore architecture, and framework stability govern CO\n                    <jats:sub>2<\/jats:sub>\n                    transport. AFS deliver CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivities up to \u223c800 at low partial pressures but exhibit limited permeance and durability. In contrast, HOF\u2010based mixed\u2010matrix membranes decouple selectivity from chemisorption, achieving permeabilities exceeding 750 Barrer with CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivity \u223c60, and up to 7,000\u20138,400 Barrer with sustained performance over 400\u2009h. Cross\u2010linked HOF\u2010derived carbon reach CO\n                    <jats:sub>2<\/jats:sub>\n                    \/CH\n                    <jats:sub>4<\/jats:sub>\n                    selectivity of 192 with significantly enhanced permeability. Emerging strategies, including hydrogen bonding, charge\u2010assisted\u2010interactions, and post\u2010synthetic cross\u2010linking, that overcome intrinsic limitations of HOFs. Hybrid AFS\u2013HOF membranes, integrating strong binding sites with well\u2010defined transport channels, are identified as a promising route toward scalable, defect\u2010tolerant separations. Collectively, this review establishes molecular\u2010level\u2010design principles and outlines pathway for translating supramolecular membrane into industrially viable CO\n                    <jats:sub>2<\/jats:sub>\n                    capture technologies.\n                  <\/jats:p>","DOI":"10.1002\/cssc.70927","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T09:48:58Z","timestamp":1785923338000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular and Supramolecular Pathways for CO\n                    <sub>2<\/sub>\n                    Separation Membranes: Amine\u2010Functionalized Silica and Hydrogen\u2010Bonded Organic Frameworks"],"prefix":"10.1002","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-7112-4922","authenticated-orcid":false,"given":"Amjad","family":"Ali","sequence":"first","affiliation":[{"name":"Co\u2010Innovation Center of Efficient 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