{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T14:26:50Z","timestamp":1785421610133,"version":"3.56.0"},"reference-count":33,"publisher":"MDPI AG","issue":"12","license":[{"start":{"date-parts":[[2026,6,13]],"date-time":"2026-06-13T00:00:00Z","timestamp":1781308800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100013209","name":"Hellenic Foundation for Research and Innovation","doi-asserted-by":"crossref","award":["16103"],"award-info":[{"award-number":["16103"]}],"id":[{"id":"10.13039\/501100013209","id-type":"DOI","asserted-by":"crossref"}]},{"award":["16103"],"award-info":[{"award-number":["16103"]}],"id":[{"id":"https:\/\/ror.org\/05v75r592","id-type":"ROR","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Materials"],"abstract":"<jats:p>Hydrogen (H2), produced from syngas and the Water\u2013Gas Shift reaction, plays a vital role as both an energy carrier and an essential industrial feedstock. This preliminary study examines the effect of incorporating ionic liquids into PLA membranes for the separation of hydrogen (H2) from carbon dioxide (CO2), aiming to provide a more energy-efficient alternative to the conventional Pressure Swing Adsorption process. Specifically, neat PLA and composite membranes containing cholinium-based ionic liquids at concentrations of 3% and 10% were fabricated. Their thermal properties and microstructural characteristics were systematically analyzed, alongside their gas separation performance. The most promising membrane was further evaluated under humid conditions to assess the impact of water presence. The PLA membrane incorporating 3% cholinium glycinate ionic liquid demonstrated the best performance, achieving a hydrogen permeability of 111 Barrer and an H2\/CO2 selectivity of 8.2, surpassing the Robeson Upper Bound reported in 2008. However, the presence of water led to a decline in separation performance, indicating that effective water removal is necessary prior to membrane application in hydrogen purification.<\/jats:p>","DOI":"10.3390\/ma19122567","type":"journal-article","created":{"date-parts":[[2026,6,15]],"date-time":"2026-06-15T03:01:27Z","timestamp":1781492487000},"page":"2567","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Tailoring PLA-Based Composite Membranes with Ionic Liquids for Efficient H2\/CO2 Separation in Reforming Processes"],"prefix":"10.3390","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8538-9523","authenticated-orcid":false,"given":"Dionysios","family":"Vroulias","sequence":"first","affiliation":[{"name":"Institute of Chemical Engineering Sciences (ICE-HT), Foundation for Research and Technology\u2014Hellas (FORTH), Stadiou St., GR 265 04 Patras, Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Athina","family":"Nikolopoulou","sequence":"additional","affiliation":[{"name":"Institute of Chemical Engineering Sciences (ICE-HT), Foundation for Research and Technology\u2014Hellas (FORTH), Stadiou St., GR 265 04 Patras, Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8765-5354","authenticated-orcid":false,"given":"Theophilos","family":"Ioannides","sequence":"additional","affiliation":[{"name":"Institute of Chemical Engineering Sciences (ICE-HT), Foundation for Research and Technology\u2014Hellas (FORTH), Stadiou St., GR 265 04 Patras, Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9029-4994","authenticated-orcid":false,"given":"Vassilios","family":"Dracopoulos","sequence":"additional","affiliation":[{"name":"Institute of Chemical Engineering Sciences (ICE-HT), Foundation for Research and Technology\u2014Hellas (FORTH), Stadiou St., GR 265 04 Patras, Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2026,6,13]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"1026","DOI":"10.1016\/j.ijhydene.2025.01.033","article-title":"Hydrogen as an alternative fuel: A comprehensive review of challenges and opportunities in production, storage, and transportation","volume":"102","author":"Hossain","year":"2025","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"100460","DOI":"10.1016\/j.nxener.2025.100460","article-title":"Review on hydrogen fuel cells as an alternative fuel","volume":"9","author":"Sethia","year":"2025","journal-title":"Next Energy"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"651","DOI":"10.1016\/B978-0-443-15740-0.00158-0","article-title":"Comparative Analysis of Natural Gas Reforming Techniques for Syngas Production","volume":"2","author":"Lak","year":"2025","journal-title":"Compr. Methanol Sci."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"118985","DOI":"10.1016\/j.seppur.2021.118985","article-title":"Highly efficient CO removal by active cuprous-based ternary deep eutectic solvents [HDEEA][Cl] + CuCl + EG","volume":"274","author":"Cui","year":"2021","journal-title":"Sep. Purif. Technol."},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"100415","DOI":"10.1016\/j.nxener.2025.100415","article-title":"A comprehensive review of carbon capture: From conventional to emerging electrochemical technologies","volume":"9","author":"Hadi","year":"2025","journal-title":"Next Energy"},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"115868","DOI":"10.1016\/j.rser.2025.115868","article-title":"Polymeric membranes for sustainable gas separation: A comprehensive review with challenges, innovations and future perspectives","volume":"219","author":"Borah","year":"2025","journal-title":"Renew. Sustain. Energy Rev."},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"4729","DOI":"10.1016\/j.polymer.2013.05.075","article-title":"Energy-efficient polymeric gas separation membranes for a sustainable future: A review","volume":"54","author":"Sanders","year":"2013","journal-title":"Polymer"},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"117701","DOI":"10.1016\/j.memsci.2019.117701","article-title":"Hydrogen selective palladium-alumina composite membranes prepared by Atomic Layer Deposition","volume":"596","author":"Weber","year":"2020","journal-title":"J. Membr. Sci."},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"390","DOI":"10.1016\/j.memsci.2008.04.030","article-title":"The upper bound revisited","volume":"320","author":"Robeson","year":"2008","journal-title":"J. Membr. Sci."},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"22138","DOI":"10.1016\/j.ijhydene.2017.04.060","article-title":"New PEEK-WC and PLA membranes for H2 separation","volume":"42","author":"Iulianelli","year":"2017","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"15861","DOI":"10.1039\/D1TA03656D","article-title":"A review of the thermophysical properties and potential of ionic liquids for thermal applications","volume":"9","author":"Fabre","year":"2021","journal-title":"J. Mater. Chem. A"},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"1074","DOI":"10.1002\/pi.70017","article-title":"Rheological and tribological behavior of new 3D-printed poly(lactic acid) modified by ionic liquid","volume":"74","author":"Pamies","year":"2025","journal-title":"Polym. Int."},{"key":"ref_13","doi-asserted-by":"crossref","unstructured":"Schmitz, D.P., Lins, L., Silva, J.M.F.d., Soares, B.G., and Livi, S. (2025). Dual Role of Ionic Liquids as Plasticizer and Co-Foaming Agent of Polylactide Matrix. Polymers, 17.","DOI":"10.3390\/polym17222967"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"172552","DOI":"10.1016\/j.cej.2026.172552","article-title":"Terminal-carboxyl-engineered 3D PLA nanochannels via ionic liquid templating for high osmotic energy conversion","volume":"528","author":"Chang","year":"2026","journal-title":"Chem. Eng. J."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"121878","DOI":"10.1016\/j.memsci.2023.121878","article-title":"Gas dehumidification over supported nicotine-based ionic liquid membranes: Effect of alkyl chain length and ether group presence","volume":"684","author":"Vroulias","year":"2023","journal-title":"J. Membr. Sci."},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"8976","DOI":"10.1021\/acs.iecr.6c00160","article-title":"Water Vapor Separation from Gas Streams Using Nicotine-Based Ionic-Liquid Membranes","volume":"65","author":"Vroulias","year":"2026","journal-title":"Ind. Eng. Chem. Res."},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"7053","DOI":"10.1021\/acs.chemrev.6b00461","article-title":"Vibrational Spectroscopy of Ionic Liquids","volume":"117","author":"Paschoal","year":"2017","journal-title":"Chem. Rev."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"927","DOI":"10.1177\/0892705711423291","article-title":"Comparison of injection moulded, natural fibre-reinforced composites with PP and PLA as matrices","volume":"25","author":"Mofokeng","year":"2011","journal-title":"J. Thermoplast. Compos. Mater."},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"2952","DOI":"10.1039\/D5SU00108K","article-title":"CO2 capture by carboxylate ionic liquids: Fine-tuning the performance by altering hydrogen bonding motifs","volume":"3","author":"Yousefe","year":"2025","journal-title":"RSC Sustain."},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"98","DOI":"10.1016\/j.jiec.2017.05.022","article-title":"Synthesis, characterization, and CO2 separation performance of polyether sulfone\/[EMIM][Tf2N] ionic liquid-polymeric membranes (ILPMs)","volume":"54","author":"Mannan","year":"2017","journal-title":"J. Ind. Eng. Chem."},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"243","DOI":"10.1016\/S0376-7388(01)00446-X","article-title":"Gas permeation properties of poly(lactic acid)","volume":"190","author":"Lehermeier","year":"2001","journal-title":"J. Membr. Sci."},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"166","DOI":"10.1016\/j.memsci.2006.08.021","article-title":"Gas permeation properties of poly(lactic acid) revisited","volume":"285","author":"Bao","year":"2006","journal-title":"J. Membr. Sci."},{"key":"ref_23","doi-asserted-by":"crossref","unstructured":"Yampolskii, Y., Pinnau, I., and Freeman, B. (2006). Transport of gases and vapors in glassy and rubbery polymers. Materials Science of Membranes for Gas and Vapor Separation, John Wiley & Sons Ltd.. [1st ed.].","DOI":"10.1002\/047002903X"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"286","DOI":"10.1016\/j.memsci.2014.11.037","article-title":"Gas transport properties of reverse-selective poly(ether-b-amide6)\/[Emim][BF4] gel membranes for CO2\/light gases separation","volume":"476","author":"Rabiee","year":"2015","journal-title":"J. Membr. Sci."},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"947","DOI":"10.1021\/acsmacrolett.5b00512","article-title":"Fine-Tuned Intrinsically Ultramicroporous Polymers Redefine the Permeability\/Selectivity Upper Bounds of Membrane-Based Air and Hydrogen Separations","volume":"4","author":"Swaidan","year":"2015","journal-title":"ACS Macro Lett."},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"165326","DOI":"10.1016\/j.cej.2025.165326","article-title":"Efficient electrochemical hydrogen compression based on high-crystallinity polymeric membrane electrolytes","volume":"519","author":"Ngo","year":"2025","journal-title":"Chem. Eng. J."},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"165","DOI":"10.1016\/0376-7388(91)80060-J","article-title":"Correlation of separation factor versus permeability for polymeric membranes","volume":"62","author":"Robeson","year":"1991","journal-title":"J. Membr. Sci."},{"key":"ref_28","unstructured":"Thornton, A.W., Freeman, B.D., and Robeson, L.M. (2026, May 02). Polymer Gas Separation Membrane Database. Available online: https:\/\/research.csiro.au\/virtualscreening\/membrane-database-polymer-gas-separation-membranes\/."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"227","DOI":"10.1016\/j.memsci.2014.08.022","article-title":"Facilitated separation of CO2 and SO2 through supported liquid membranes using carboxylate-based ionic liquids","volume":"471","author":"Huang","year":"2014","journal-title":"J. Membr. Sci."},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"1481","DOI":"10.1126\/science.156.3781.1481","article-title":"Carbon Dioxide-Oxygen Separation: Facilitated Transport of Carbon Dioxide across a Liquid Film","volume":"156","author":"Ward","year":"1967","journal-title":"Science"},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"134082","DOI":"10.1016\/j.biortech.2026.134082","article-title":"Functional Bioplastics from Agricultural Wastes: Precursor Engineering, Composite Strategies, and Sustainable Packaging Performance","volume":"446","author":"Khamis","year":"2026","journal-title":"Bioresour. Technol."},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"742847","DOI":"10.1016\/j.aquaculture.2025.742847","article-title":"Harvesting of Microalga Coelastrella Sp. CHZ by Flocculation with Ionic Liquid Choline-Alanine","volume":"609","author":"Xie","year":"2025","journal-title":"Aquaculture"},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"102121","DOI":"10.1016\/j.jcou.2022.102121","article-title":"Fabrication, Characterization and Optimization of Industrial Alpha Alumina Powders Based Ceramic Membrane Supports and Its Applicative Potential for CO2\/N2 Separation","volume":"63","author":"Sharma","year":"2022","journal-title":"J. CO2 Util."}],"container-title":["Materials"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/1996-1944\/19\/12\/2567\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,6,19]],"date-time":"2026-06-19T04:41:22Z","timestamp":1781844082000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/1996-1944\/19\/12\/2567"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,6,13]]},"references-count":33,"journal-issue":{"issue":"12","published-online":{"date-parts":[[2026,6]]}},"alternative-id":["ma19122567"],"URL":"https:\/\/doi.org\/10.3390\/ma19122567","relation":{},"ISSN":["1996-1944"],"issn-type":[{"value":"1996-1944","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,6,13]]}}}