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Mixed matrix membranes (MMMs) integrate the advantages of polymer matrices and inorganic fillers, making them promising materials for high-performance carbon capture. However, their practical separation performance is often severely limited by poor interfacial compatibility. To address this challenge, we designed and fabricated a series of chemically bonded MMMs. Graphitic carbon nitride (g-C3N4) served as a solid-state cross-linker, with its amino groups reacting with the benzyl bromide moieties of the brominated polyimide (PI-Br) matrix through nucleophilic substitution. This interfacial chemical bonding improved polymer\u2013filler compatibility and introduced interfacial cross-linking constraints, thereby regulating polymer chain packing. Comprehensive characterization Fourier-transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS) indicated that the organic\u2013inorganic interfacial interactions effectively minimized nonselective interfacial defects and promoted efficient gas transport. Among the investigated membranes, PI-Br-4-3% demonstrated the most favorable separation capability, with CO2 permeability and CO2\/CH4 selectivity reaching 335.38 Barrer and 47.03, respectively. Furthermore, the cross-linked MMM demonstrated remarkable stability under varying pressure and temperature conditions, providing solid empirical evidence for its potential application in industrial natural gas purification.<\/jats:p>","DOI":"10.1021\/acsami.6c15654","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T15:01:48Z","timestamp":1791385308000},"page":"56673-56685","source":"Crossref","is-referenced-by-count":0,"title":["Preparation of Mixed Matrix Membranes Using Graphitic Carbon Nitride as Solid Cross-Linking Agent for CO2 Separation"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0678-3937","authenticated-orcid":true,"given":"Jiayou","family":"Liao","sequence":"first","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]},{"name":"Shanxi Research Institute of Huairou Laboratory , ,","place":["China, 030032"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min","family":"Wen","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhe","family":"Meng","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyue","family":"Meng","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-2991-6154","authenticated-orcid":true,"given":"Xianjie","family":"Meng","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4919-4048","authenticated-orcid":true,"given":"Xianmei","family":"Xie","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-8197-9155","authenticated-orcid":true,"given":"ChengYun","family":"Gao","sequence":"additional","affiliation":[{"name":"Taiyuan University of Science and Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xia","family":"An","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2628-0376","authenticated-orcid":true,"given":"Jinping","family":"Li","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]},{"name":"Shanxi Research Institute of Huairou Laboratory , ,","place":["China, 030032"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4997-2148","authenticated-orcid":true,"given":"Xu","family":"Wu","sequence":"additional","affiliation":[{"name":"Taiyuan University of Technology , , ,","place":["Taiyuan, China, 030024"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,7]]},"reference":[{"issue":"7600","key":"2026102108075045100_cit1","doi-asserted-by":"publisher","first-page":"435","DOI":"10.1038\/532435a","article-title":"Seven Chemical Separations to Change the World","volume":"532","author":"Sholl","year":"2016","journal-title":"Nature"},{"issue":"3","key":"2026102108075045100_cit2","doi-asserted-by":"publisher","first-page":"419","DOI":"10.1016\/j.pecs.2012.01.004","article-title":"Recent Developments in Membrane-Based Technologies for CO2 Capture","volume":"38","author":"Luis","year":"2012","journal-title":"Prog. 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