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The incorporation of ILs into MOFs cages has led to the development of a novel type of solid electrolytes (ILs@MOF), characterized by exceptional thermal stability and high conductivity for large ionic species. In this study, an efficient capillary method was employed to introduce a classical protic IL, [Dema][TfO], into ZIF\u20108 pores, consisting of sodalite\u2010type cages (Zn(MeIm)\n                    <jats:sub>2<\/jats:sub>\n                    ). Our investigation focuses on the influence of varying ILs content on the free (pore) volume, thermal stability, microstructure, and ionic conductivity. The uptake of [Dema][TfO] results in a ZIF\u20108 cage expansion, accompanied by a decrease of the decomposition temperature. Upon infiltration of [Dema][TfO] into the ZIF\u20108 pores, the preexisting hydrogen bonds within the IL are broken due to confinement effects. Notably, when ZIF\u20108 pores are entirely saturated with [Dema][TfO], the composite material exhibits an ionic conductivity of 1.09(6) mS\u00b7cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    (at 160\u00b0C under anhydrous conditions) with an activation energy of 0.45(3) eV, which is better than other ILs@MOF conductive composites. These findings reveal ILs@MOF hybrid composites are versatile systems to compose protic conductors, attributable to their elevated ionic conductivity.\n                  <\/jats:p>","DOI":"10.1002\/smll.76019","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T16:48:30Z","timestamp":1790527710000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["The Host\u2010Guest Assemblies of Metal\u2013Organic Frameworks and Protic Ionic Liquids With ZIF\u20108 and [Dema][TfO] \u2013 Structural Response and Ionic Conductivity"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-4807-9451","authenticated-orcid":false,"given":"Wen","family":"Yang","sequence":"first","affiliation":[{"name":"Institute of Energy Technologies (IET\u20104) Forschungszentrum J\u00fclich GmbH  J\u00fclich Germany"},{"name":"Faculty of Mathematics, Computer Science and Natural Sciences RWTH Aachen 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