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Membranes with 20 wt% of poly(diallyldimethylammonium) bis(trifluoromethylsulfonyl)imide, poly[pyr\n                    <jats:sub>11<\/jats:sub>\n                    ][NTf\n                    <jats:sub>2<\/jats:sub>\n                    ], PIL and 80 wt% of 1\u2010ethyl\u20103\u2010methylimidazolium bis(trifluoromethylsulfonyl)imide, ([C\n                    <jats:sub>2<\/jats:sub>\n                    mim][NTf\n                    <jats:sub>2<\/jats:sub>\n                    ]), IL with varying filler loadings were evaluated for CO\n                    <jats:sub>2<\/jats:sub>\n                    separation performance, including gas permeance, permeability, diffusivity, solubility, and CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivity. Spray\u2010coating enabled the formation of ultrathin, selective layers, resulting in CO\n                    <jats:sub>2<\/jats:sub>\n                    permeances up to 27\u00a0GPU, approximately twice than without silica and up to ten times higher than solvent\u2010cast samples, while maintaining selectivity values, between 29 and 40. In contrast, solvent\u2010cast membranes exhibited lower CO\n                    <jats:sub>2<\/jats:sub>\n                    permeances (2\u20133\u00a0GPU) but benefited from uniform filler dispersion, achieving a 63% increase in CO\n                    <jats:sub>2<\/jats:sub>\n                    permeability at optimal SiIL loadings. Mixed\u2010gas experiments (15% CO\n                    <jats:sub>2<\/jats:sub>\n                    and 85% N\n                    <jats:sub>2<\/jats:sub>\n                    ) demonstrated that spray\u2010coated membranes retained most of their performance under competitive conditions, with CO\n                    <jats:sub>2<\/jats:sub>\n                    permeance losses of only 5%\u20139%, whereas solvent\u2010cast membranes showed more stable selectivity but lower overall flux. These results highlight that membrane fabrication methodology, rather than filler content alone, critically determines the membrane architecture and thus gas transport behavior. Overall, spray\u2010coating emerges as a highly effective approach to designing scalable, high\u2010performance MMMs for industrial CO\n                    <jats:sub>2<\/jats:sub>\n                    separation applications.\n                  <\/jats:p>","DOI":"10.1002\/cssc.70922","type":"journal-article","created":{"date-parts":[[2026,7,28]],"date-time":"2026-07-28T11:30:18Z","timestamp":1785238218000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Advancing Ionic Liquid\u2010Based Membrane Fabrication: Spray\u2010Coating as a Pathway for Mixed\u2010Matrix Membranes"],"prefix":"10.1002","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2640-8146","authenticated-orcid":false,"given":"Bruna F.","family":"Soares","sequence":"first","affiliation":[{"name":"Departamento de Engenharia Qu\u00edmica e Centro de Qu\u00edmica Estrutural Instituto Superior de Lisboa Universidade de Lisboa  Lisboa Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-2538-818X","authenticated-orcid":false,"given":"Francisco","family":"Cunha","sequence":"additional","affiliation":[{"name":"Departamento de Engenharia Qu\u00edmica e Centro de Qu\u00edmica Estrutural Instituto Superior de Lisboa Universidade de Lisboa  Lisboa Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-7699-140X","authenticated-orcid":false,"given":"Henrique","family":"Santos","sequence":"additional","affiliation":[{"name":"Departamento de Engenharia Qu\u00edmica e Centro de Qu\u00edmica Estrutural Instituto Superior de Lisboa Universidade de Lisboa  Lisboa Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Clara","family":"Parreir\u00e3o","sequence":"additional","affiliation":[{"name":"Departamento de Engenharia Qu\u00edmica e Centro de Qu\u00edmica Estrutural Instituto Superior de Lisboa Universidade de Lisboa  Lisboa Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5611-4080","authenticated-orcid":false,"given":"M\u00e1rcia C.","family":"Neves","sequence":"additional","affiliation":[{"name":"Department of Chemistry CICECO \u2010 Aveiro Institute of Materials University of Aveiro  Aveiro Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8895-0614","authenticated-orcid":false,"given":"Mara G.","family":"Freire","sequence":"additional","affiliation":[{"name":"Department of Chemistry CICECO \u2010 Aveiro Institute of Materials University of Aveiro  Aveiro Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8733-1958","authenticated-orcid":false,"given":"Isabel M.","family":"Marrucho","sequence":"additional","affiliation":[{"name":"Departamento de Engenharia Qu\u00edmica e Centro de Qu\u00edmica Estrutural Instituto Superior de Lisboa Universidade de Lisboa  Lisboa 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