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Here, we program a permeation inversion in CO2\/H2 transport by constructing a nanoconfined ionic liquid membrane through the synergistic engineering of graphene oxide nanosheets and ionic liquids. A substrate-assisted size-selection strategy enables the preferential incorporation of large nanosheets, which form ordered laminates, while short-chain CO2-philic ionic liquids are precisely confined within the interlayer galleries. The resulting membrane exhibits inverted transport behavior, achieving an ultrahigh CO2 permeance of 358.2 GPU and a mixed-gas CO2\/H2 selectivity of 201.9 under a 10:90 CO2\/H2 feed\u2500surpassing the upper bounds of conventional polymeric and mixed-matrix membranes. Scalability is demonstrated using a five-cell module, in which CO2 flux increases linearly without selectivity loss. Molecular dynamics simulations and spectroscopic studies reveal that the nanoconfined ionic liquid phase creates a continuous, high-solubility pathway for CO2, whereas H2 is largely excluded from the graphene oxide interfaces. This study establishes nanosheet\u2013ionic liquid synergy as a programmable design platform to engineer permeation inversion, offering a scalable route to advanced CO2\/H2 separation membranes.<\/jats:p>","DOI":"10.1021\/acsnano.6c07156","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T18:04:37Z","timestamp":1784657077000},"page":"21327-21336","source":"Crossref","is-referenced-by-count":0,"title":["Programming\nPermeation Inversion in Nanoconfined Ionic\nLiquid Membranes for Ultra-Selective CO2\/H2 Separation"],"prefix":"10.1021","volume":"20","author":[{"given":"Yue","family":"Qiu","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyue","family":"Pi","sequence":"additional","affiliation":[{"name":"Renmin University of China , , , ,","place":["Beijing, China, 100872"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lin","family":"Zhao","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Dong","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junfeng","family":"Lu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yumiao","family":"Lu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2214-8781","authenticated-orcid":true,"given":"Yanlei","family":"Wang","sequence":"additional","affiliation":[{"name":"Renmin University of China , , , ,","place":["Beijing, China, 100872"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1291-2771","authenticated-orcid":true,"given":"Hongyan","family":"He","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,21]]},"reference":[{"key":"2026080409271544700_cit1","doi-asserted-by":"publisher","first-page":"1065","DOI":"10.1126\/science.aaf1835","article-title":"Selective conversion of syngas to\nlight olefins","volume":"351","author":"Jiao","year":"2016","journal-title":"Science"},{"key":"2026080409271544700_cit2","doi-asserted-by":"publisher","first-page":"12119","DOI":"10.1021\/acsnano.1c03492","article-title":"Scalable polymeric\nfew-nanometer organosilica membranes with hydrothermal stability for\nselective hydrogen separation","volume":"15","author":"Zhu","year":"2021","journal-title":"ACS Nano"},{"key":"2026080409271544700_cit3","doi-asserted-by":"publisher","first-page":"14379","DOI":"10.1021\/acsnano.2c04670","article-title":"Facile ionization of\nthe nanochannels of lamellar membranes for stable ionic liquid immobilization\nand efficient CO2 separation","volume":"16","author":"Jia","year":"2022","journal-title":"ACS\nNano"},{"key":"2026080409271544700_cit4","doi-asserted-by":"publisher","first-page":"1073","DOI":"10.1021\/accountsmr.2c00143","article-title":"Gas separation membranes with atom-thick nanopores:\nThe potential of nanoporous single-layer graphene","volume":"3","author":"Villalobos","year":"2022","journal-title":"Acc. 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Colloid Interface Sci."},{"key":"2026080409271544700_cit19","doi-asserted-by":"publisher","first-page":"1855","DOI":"10.1063\/1.1635356","article-title":"Structure of ionic\nliquids of 1-alkyl-3-methylimidazolium\ncations: a systematic computer simulation study","volume":"120","author":"Urahata","year":"2004","journal-title":"J. Chem. Phys."},{"key":"2026080409271544700_cit20","doi-asserted-by":"publisher","first-page":"59","DOI":"10.1016\/j.seppur.2017.03.031","article-title":"CO2\/N2 separation using alumina\nsupported membranes based on new functionalized ionic liquids","volume":"182","author":"Sa\u0301nchez Fuentes","year":"2017","journal-title":"Sep. Purif. 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Sci."},{"key":"2026080409271544700_cit26","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2024.130891","article-title":"Grafted graphene oxide membrane confining ionic liquid\nfor high efficiency CO2\/H2 separation","volume":"360","author":"Qiu","year":"2025","journal-title":"Sep. Purif. Technol."},{"key":"2026080409271544700_cit27","doi-asserted-by":"publisher","DOI":"10.1002\/smll.201904145","article-title":"CO2-philic separation membrane: deep eutectic\nsolvent filled graphene oxide nanoslits","volume":"15","author":"Lin","year":"2019","journal-title":"Small"},{"key":"2026080409271544700_cit28","doi-asserted-by":"publisher","first-page":"6531","DOI":"10.1021\/acs.iecr.2c00748","article-title":"Surface functionalities\nof graphene oxide with varying flake size","volume":"61","author":"Khine","year":"2022","journal-title":"Ind.\nEng. Chem. Res."},{"key":"2026080409271544700_cit29","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aaz9184","article-title":"Realizing\nsmall-flake\ngraphene oxide membranes for ultrafast size-dependent organic solvent\nnanofiltration","volume":"6","author":"Nie","year":"2020","journal-title":"Sci. Adv."},{"key":"2026080409271544700_cit30","doi-asserted-by":"publisher","first-page":"7725","DOI":"10.1021\/acs.jpclett.9b03082","article-title":"Understanding\ngas transport behavior\nthrough few-layer graphene oxide membranes controlled by tortuosity\nand interlayer spacing","volume":"10","author":"Roh","year":"2019","journal-title":"J. Phys. Chem. Lett."},{"key":"2026080409271544700_cit31","doi-asserted-by":"publisher","first-page":"44460","DOI":"10.1021\/acsami.1c13169","article-title":"Effects of\nionic liquid nanoconfinement on the CO2\/CH4 separation\nin poly(vinylidene fluoride)\/1-ethyl-3-methylimidazolium thiocyanate\nmembranes","volume":"13","author":"Rahmani","year":"2021","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026080409271544700_cit32","doi-asserted-by":"publisher","first-page":"201","DOI":"10.1016\/j.memsci.2011.11.037","article-title":"CO2\/N2 separations using nanoporous\nalumina-supported ionic liquid\nmembranes: Effect of the support on separation performance","volume":"390","author":"Close","year":"2012","journal-title":"J. Membr. Sci."},{"key":"2026080409271544700_cit33","doi-asserted-by":"publisher","first-page":"457","DOI":"10.1038\/nature06016","article-title":"Preparation\nand\ncharacterization of graphene oxide paper","volume":"448","author":"Dikin","year":"2007","journal-title":"Nature"},{"key":"2026080409271544700_cit34","doi-asserted-by":"publisher","first-page":"13024","DOI":"10.1002\/anie.201305630","article-title":"Solvation of carbon\ndioxide in [C4mim][BF4] and [C4mim][PF6] ionic liquids revealed by high-pressure NMR spectroscopy","volume":"52","author":"Corvo","year":"2013","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026080409271544700_cit35","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcou.2023.102555","article-title":"Breaking boundaries\nin CO2 capture: Ionic liquid-based membrane separation\nfor post-combustion applications","volume":"75","author":"Mulk","year":"2023","journal-title":"J. CO2 Util."},{"key":"2026080409271544700_cit36","doi-asserted-by":"publisher","DOI":"10.1016\/j.ces.2023.119393","article-title":"Preparation\nof two-dimensional nanoconfined ionic liquid membrane and its molecular\nmechanism of CO2 separation","volume":"283","author":"Dong","year":"2024","journal-title":"Chem.\nEng. Sci."},{"key":"2026080409271544700_cit37","doi-asserted-by":"publisher","first-page":"168","DOI":"10.1016\/j.seppur.2019.04.018","article-title":"Poly(ionic liquid)-based engineered\nmixed matrix membranes for CO2\/H2 separation","volume":"222","author":"Nabais","year":"2019","journal-title":"Sep. Purif. Technol."},{"key":"2026080409271544700_cit38","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2022.121784","article-title":"Recent advances in\npoly(ionic liquids)\nmembranes for CO2 separation","volume":"299","author":"Zhang","year":"2022","journal-title":"Sep.\nPurif. Technol."},{"key":"2026080409271544700_cit39","doi-asserted-by":"publisher","first-page":"480","DOI":"10.1021\/je0256277","article-title":"Solubilities\nof oxygen and carbon\ndioxide in butyl methyl imidazolium tetrafluoroborate as a function\nof temperature and at pressures close to atmospheric pressure","volume":"48","author":"Husson-Borg","year":"2003","journal-title":"J. Chem. Eng. Data"},{"key":"2026080409271544700_cit40","doi-asserted-by":"publisher","first-page":"3859","DOI":"10.3390\/app10113859","article-title":"Water\nvapour promotes CO2 transport in poly(ionic liquid)\/ionic\nliquid-based thin-film composite membranes containing zinc salt for\nflue gas treatment","volume":"10","author":"Nikolaeva","year":"2020","journal-title":"Appl. Sci."},{"key":"2026080409271544700_cit41","doi-asserted-by":"publisher","first-page":"6","DOI":"10.3390\/membranes10010006","article-title":"Effect of humidity\non CO2\/N2 and CO2\/CH4 separation\nusing novel robust mixed matrix composite hollow fiber membranes:\nexperimental and model evaluation","volume":"10","author":"Casado-Coterillo","year":"2020","journal-title":"Membranes"},{"key":"2026080409271544700_cit42","doi-asserted-by":"publisher","first-page":"834","DOI":"10.1016\/j.gee.2024.07.010","article-title":"Superhydrophobic ceramic\nmembrane coupled with a biphasic solvent\nfor efficient CO2 capture","volume":"10","author":"Xue","year":"2025","journal-title":"Green\nEnergy Environ."},{"key":"2026080409271544700_cit43","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2020.118113","article-title":"CO2\/H2 separation through poly(ionic\nliquid)\u2013ionic liquid membranes: The effect of multicomponent\ngas mixtures, temperature and gas feed pressure","volume":"259","author":"Gouveia","year":"2021","journal-title":"Sep. Purif. Technol."},{"key":"2026080409271544700_cit44","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1006\/jcph.1995.1039","article-title":"Fast parallel\nalgorithms for short-range molecular dynamics","volume":"117","author":"Plimpton","year":"1995","journal-title":"J. Comput. Phys."},{"key":"2026080409271544700_cit45","doi-asserted-by":"publisher","DOI":"10.1016\/j.jil.2022.100043","article-title":"Molecular modelling of ionic liquids: General guidelines on fixed-charge\nforce fields for balanced descriptions","volume":"2","author":"Sun","year":"2022","journal-title":"J. Ion.\nLiq."},{"key":"2026080409271544700_cit46","doi-asserted-by":"publisher","first-page":"6131","DOI":"10.1021\/acs.jctc.7b00520","article-title":"Revisiting\nOPLS force field parameters for ionic liquid simulations","volume":"13","author":"Doherty","year":"2017","journal-title":"J. Chem. Theory Comput."},{"key":"2026080409271544700_cit47","doi-asserted-by":"publisher","first-page":"15","DOI":"10.1016\/0927-0256(96)00008-0","article-title":"Efficiency of ab-initio total energy\ncalculations for\nmetals and semiconductors using a plane-wave basis set","volume":"6","author":"Kresse","year":"1996","journal-title":"Comput. Mater. Sci."},{"key":"2026080409271544700_cit48","doi-asserted-by":"publisher","first-page":"11169","DOI":"10.1103\/PhysRevB.54.11169","article-title":"Efficient iterative schemes for ab-initio\ntotal-energy\ncalculations using a plane-wave basis set","volume":"54","author":"Kresse","year":"1996","journal-title":"Phys.\nRev. B"},{"key":"2026080409271544700_cit49","doi-asserted-by":"publisher","first-page":"17953","DOI":"10.1103\/PhysRevB.50.17953","article-title":"Projector\naugmented-wave method","volume":"50","author":"Blo\u0308chl","year":"1994","journal-title":"Phys. Rev. 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