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One such strategy is to employ the combination of a CO<jats:sub>2<\/jats:sub>\u2010selective membrane coupled with a CO<jats:sub>2<\/jats:sub> capture solvent acting as a draw solution. Here, the interactions between a leading water\u2010lean carbon\u2010capture solvent, a polyether ether ketone (PEEK)\u2010ionene membrane, CO<jats:sub>2<\/jats:sub>, and combinations were probed using advanced NMR techniques coupled with advanced simulations. We identify the speciation and dynamics of the solvent, membrane, and CO<jats:sub>2<\/jats:sub>, presenting spectroscopic evidence of CO<jats:sub>2<\/jats:sub> diffusion through benzylic regions within the PEEK\u2010ionene membrane, not spaces in the ionic lattice as expected. Our results demonstrate that water\u2010lean capture solvents provide a thermodynamic and kinetic funnel to draw CO<jats:sub>2<\/jats:sub> from the air through the membrane and into the bulk solvent, thus enhancing the performance of the membrane. The reaction between the carbon\u2010capture solvent and CO<jats:sub>2<\/jats:sub> produces carbamic acid, disrupting interactions between the imidazolium (Im<jats:sup>+<\/jats:sup>) cations and the bistriflimide anions within the PEEK\u2010ionene membrane, thereby creating structural changes through which CO<jats:sub>2<\/jats:sub> can diffuse more readily. Consequently, this restructuring results in CO<jats:sub>2<\/jats:sub> diffusion at the interface that is faster than CO<jats:sub>2<\/jats:sub> diffusion in the bulk carbon\u2010capture solvent.<\/jats:p>","DOI":"10.1002\/cssc.202300157","type":"journal-article","created":{"date-parts":[[2023,5,24]],"date-time":"2023-05-24T10:18:20Z","timestamp":1684923500000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Enhancing CO<sub>2<\/sub> Transport Across a PEEK\u2010Ionene Membrane and Water\u2010Lean Solvent Interface"],"prefix":"10.1002","volume":"16","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3644-5514","authenticated-orcid":false,"given":"Eric D.","family":"Walter","sequence":"first","affiliation":[{"name":"Pacific Northwest National Laboratory  Battelle Blvd 99352 Richland WA USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7530-2378","authenticated-orcid":false,"given":"Difan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Pacific Northwest National Laboratory  Battelle Blvd 99352 Richland WA USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7417-0991","authenticated-orcid":false,"given":"Ying","family":"Chen","sequence":"additional","affiliation":[{"name":"Pacific Northwest National Laboratory  Battelle Blvd 99352 Richland WA USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3535-1818","authenticated-orcid":false,"given":"Kee","family":"Sung Han","sequence":"additional","affiliation":[{"name":"Pacific Northwest National Laboratory  Battelle Blvd 99352 Richland WA USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4599-3208","authenticated-orcid":false,"given":"J. 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