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High crystallinity\u2014an often\u2010overlooked aspect in PHI frameworks\u2014is identified as a key factor governing CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption capacity in microporous structures. Thermogravimetric analysis and manometric studies reveal a CO\n                    <jats:sub>2<\/jats:sub>\n                    uptake of \u22483.8\u2009mmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , at 1\u2009bar and 25\u2009\u00b0C, surpassing most reported PHI\u2010based adsorbents under similar conditions. Exchanging Na\n                    <jats:sup>+<\/jats:sup>\n                    with K\n                    <jats:sup>+<\/jats:sup>\n                    or Rb\n                    <jats:sup>+<\/jats:sup>\n                    preserves CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption performance, whereas Cs\n                    <jats:sup>+<\/jats:sup>\n                    incorporation induces structural distortion, greatly reducing CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption capacity in PHI. These materials exhibit excellent cyclic stability (20 cycles) without degradation and CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption capacity loss. Notably, at flue gas\u2010relevant temperature (100\u2009\u00b0C), NaPHI attains a CO\n                    <jats:sub>2<\/jats:sub>\n                    capacity of 2.1\u2009mmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , doubling the performance of benchmark Zeolite 13X (1.1\u2009mmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). Ideal Adsorbed Solution Theory confirms remarkable CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivity (\u22483.8\u2009mmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    vs typical N\n                    <jats:sub>2<\/jats:sub>\n                    adsorption of 0.3\u2009mmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), a critical property for postcombustion CO\n                    <jats:sub>2<\/jats:sub>\n                    capture. These findings position PHI\u2010based materials as a disruptive platform for CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption, offering 1) straightforward synthesis from readily available precursors, 2) promising scalability, and 3) outstanding performance.\n                  <\/jats:p>","DOI":"10.1002\/cssc.202500775","type":"journal-article","created":{"date-parts":[[2025,6,19]],"date-time":"2025-06-19T09:35:02Z","timestamp":1750325702000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Crystallinity\u2010Enhanced CO\n                    <sub>2<\/sub>\n                    Adsorption by Sodium Poly(Heptazine Imide) Frameworks"],"prefix":"10.1002","volume":"18","author":[{"given":"Pedro","family":"Ouro","sequence":"first","affiliation":[{"name":"Department of Chemistry CICECO \u2013 Aveiro Institute of Materials University of Aveiro Campus Universit\u00e1rio de Santiago 3810\u2010193 Aveiro Portugal"},{"name":"Department of Chemical and Environmental Engineering University of Oviedo 33006 Oviedo Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"\u00c1lvaro","family":"Cuevas","sequence":"additional","affiliation":[{"name":"Department of Chemical and Environmental Engineering University of Oviedo 33006 Oviedo Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Johannes","family":"Liessem","sequence":"additional","affiliation":[{"name":"Institute of Electrochemistry Ulm University Albert\u2010Einstein\u2010Allee 47 89081 Ulm Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dariusz","family":"Mitoraj","sequence":"additional","affiliation":[{"name":"Institute of Electrochemistry Ulm University Albert\u2010Einstein\u2010Allee 47 89081 Ulm Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Radim","family":"Beranek","sequence":"additional","affiliation":[{"name":"Institute of Electrochemistry Ulm University Albert\u2010Einstein\u2010Allee 47 89081 Ulm Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Eva","family":"D\u00edaz","sequence":"additional","affiliation":[{"name":"Department of Chemical and Environmental Engineering University of Oviedo 33006 Oviedo Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Salvador","family":"Ord\u00f3\u00f1ez","sequence":"additional","affiliation":[{"name":"Department of Chemical and Environmental Engineering University of Oviedo 33006 Oviedo Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ildefonso","family":"Marin\u2010Montesinos","sequence":"additional","affiliation":[{"name":"Department of Chemistry CICECO \u2013 Aveiro Institute of Materials University of Aveiro Campus Universit\u00e1rio de Santiago 3810\u2010193 Aveiro 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