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However, these processes are often carried out separately, making it difficult to achieve both objectives simultaneously. Herein, a polyethyleneimine (PEI)-induced simultaneous functionalization and defect engineering strategy is proposed, in which PEI is introduced during the synthesis of RHO-topology ZIF(Cu) to in situ generate structural defects through competitive coordination with Cu2+ centers. PEI enhanced the interfacial compatibility between the filler and the Pebax matrix through hydrogen-bonding interactions and introduced a facilitated transport effect. Meanwhile, defect engineering exposed additional Cu2+ Lewis acid sites capable of adsorbing CO2 and generated additional transport pathways. The synergy between amine functionalization and defect engineering resulted in a substantial enhancement in the separation performance of the MMMs. Under humid conditions, the MMM containing 5 wt % PEI-RHO ZIF(Cu) presented a CO2 permeability of 188.1 Barrer and a CO2\/N2 separation factor of 73.0, representing increases of 95.10% and 78.14%, respectively, relative to Pebax, and surpassing the 2008 Robeson upper bound. This integrated strategy, combining defect engineering with amine functionalization, provides a promising avenue for the development of high-efficiency CO2 capture MMMs.<\/jats:p>","DOI":"10.1021\/acsami.6c12606","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T10:50:03Z","timestamp":1788432603000},"page":"49164-49174","source":"Crossref","is-referenced-by-count":0,"title":["PEI-Induced Simultaneous Functionalization and Defect Engineering of RHO-Topology ZIF(Cu) for Enhanced CO2 Separation Performance in Mixed Matrix Membranes"],"prefix":"10.1021","volume":"18","author":[{"given":"Zikang","family":"Qin","sequence":"first","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min","family":"Deng","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Long","family":"Shi","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2743-758X","authenticated-orcid":true,"given":"Lu","family":"Yao","sequence":"additional","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]},{"name":"National Engineering Research Centre for Flue Gas Desulfurization , ,","place":["Chengdu, China, 610065"]},{"name":"Chengdu , ,","place":["China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3367-244X","authenticated-orcid":true,"given":"Lin","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]},{"name":"National Engineering Research Centre for Flue Gas Desulfurization , ,","place":["Chengdu, China, 610065"]},{"name":"Chengdu , ,","place":["China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1327-7159","authenticated-orcid":true,"given":"Wenju","family":"Jiang","sequence":"additional","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]},{"name":"National Engineering Research Centre for Flue Gas Desulfurization , ,","place":["Chengdu, China, 610065"]},{"name":"Chengdu , ,","place":["China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8515-6770","authenticated-orcid":true,"given":"Junfeng","family":"Zheng","sequence":"additional","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]},{"name":"National Engineering Research Centre for Flue Gas Desulfurization , ,","place":["Chengdu, China, 610065"]},{"name":"Chengdu , ,","place":["China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3558-5403","authenticated-orcid":true,"given":"Zhongde","family":"Dai","sequence":"additional","affiliation":[{"name":"College of Carbon Neutrality Future Technology, Sichuan University , ,","place":["Chengdu, China, 610065"]},{"name":"National Engineering Research Centre for Flue Gas Desulfurization , ,","place":["Chengdu, China, 610065"]},{"name":"Chengdu , ,","place":["China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,1]]},"reference":[{"issue":"27","key":"2026092321464303100_cit1","doi-asserted-by":"publisher","first-page":"22020","DOI":"10.1039\/d5ta02226f","article-title":"Pebax mixed matrix membranes based on novel HOF\/MOF nanofiller with simultaneous improvement in CO2 permeability and CO2\/N2 selectivity","volume":"13","author":"Qin","year":"2025","journal-title":"J. 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