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Melamine incorporation partially reduced the accessible surface area and pore volume of the framework while preserving its crystallinity and structural stability. Despite the decrease in porosity, the modified MIL-101(Cr)-MEL exhibited enhanced CO2 adsorption performance at low pressures and elevated temperatures compared with pristine MIL-101(Cr). At 60 \u00b0C and 1 bar, the CO2 uptake of MIL-101(Cr)-MEL was more than twice that of the pristine material, while the working capacity in the 0.08\u20130.14 bar range increased fourfold. IAST calculations revealed significantly enhanced CO2\/N2 selectivity at low pressures, reaching selectivity values close to 90 below 0.05 bar. Dynamic breakthrough experiments under both dry and humid CO2\/N2 gas streams further confirmed the preferential CO2 adsorption of MIL-101(Cr)-MEL, with only a 13.4% reduction in CO2 adsorption capacity under humid conditions. The modified material also exhibited higher isosteric enthalpies of adsorption at low CO2 coverage, indicating enhanced CO2 affinity relative to pristine MIL-101(Cr). However, the moderate \u2212\u0394Hads values suggest that adsorption is governed by reversible non-covalent CO2-melamine interactions rather than by the formation of strongly bound CO2-amine adducts, providing an effective balance between CO2 affinity and regenerability. DRIFTS analyses confirmed reversible CO2 adsorption without evidence of carbonate or carbamate formation, supporting a mechanism dominated by moderate-strength non-covalent interactions. Overall, these results demonstrate that melamine functionalization provides a simple and effective strategy to enhance low-pressure CO2 capture performance under thermally demanding conditions.<\/jats:p>","DOI":"10.1021\/acsomega.6c07336","type":"journal-article","created":{"date-parts":[[2026,9,15]],"date-time":"2026-09-15T20:02:43Z","timestamp":1789502563000},"page":"57925-57934","source":"Crossref","is-referenced-by-count":0,"title":["Melamine-Modified\nMIL-101(Cr) with Enhanced CO2 Affinity for Low-Pressure\nCapture"],"prefix":"10.1021","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6223-1718","authenticated-orcid":true,"given":"Andre\u0301s","family":"Lancheros","sequence":"first","affiliation":[{"name":"Pontificia Universidad Cato\u0301lica de Chile . , ,","place":["Santiago, Chile, 7820436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Claudio","family":"Contreras-Di\u0301az","sequence":"additional","affiliation":[{"name":"Pontificia Universidad Cato\u0301lica de Chile . , ,","place":["Santiago, Chile, 7820436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0973-9453","authenticated-orcid":true,"given":"Esteban","family":"Camu\u0301","sequence":"additional","affiliation":[{"name":"Pontificia Universidad Cato\u0301lica de Chile . , ,","place":["Santiago, Chile, 7820436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thiago C.","family":"dos Santos","sequence":"additional","affiliation":[{"name":"Universidade Federal do Rio de Janeiro , , , ,","place":["Rio de Janeiro, Rio de Janeiro, Brazil, 21941-901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9736-9661","authenticated-orcid":true,"given":"Ce\u0301lia M.","family":"Ronconi","sequence":"additional","affiliation":[{"name":"Universidade Federal Fluminense , , , ,","place":["Nitero\u0301i, Rio de Janeiro, Brazil, 24220-900"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ne\u0301stor","family":"Escalona","sequence":"additional","affiliation":[{"name":"Pontificia Universidad Cato\u0301lica de Chile . , ,","place":["Santiago, Chile, 7820436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9955-8394","authenticated-orcid":true,"given":"E\u0301lodie","family":"Blanco","sequence":"additional","affiliation":[{"name":"Pontificia Universidad Cato\u0301lica de Chile . , ,","place":["Santiago, Chile, 7820436"]},{"name":"Pontificia Universidad Cato\u0301lica de Chile , , ,","place":["Santiago, Chile, 7820436"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,15]]},"reference":[{"issue":"4","key":"2026092911113288300_cit1","doi-asserted-by":"publisher","first-page":"66","DOI":"10.3390\/environments10040066","article-title":"The\nRising Threat of Atmospheric CO2: A Review on the Causes,\nImpacts, and Mitigation Strategies","volume":"10","author":"Nunes","year":"2023","journal-title":"Environments"},{"issue":"13","key":"2026092911113288300_cit2","doi-asserted-by":"publisher","first-page":"6767","DOI":"10.3390\/ijerph18136767","article-title":"Analysis of\nthe Emergent Climate\nChange Mitigation Technologies","volume":"18","author":"Panepinto","year":"2021","journal-title":"Int. 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