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Leveraging the abundance and eco\u2010friendliness of cellulose\u2010based materials, GPEs were produced using methyl cellulose and incorporating various doping agents, either an ionic liquid (1\u2010Butyl\u20101\u2010methylpyrrolidinium bis(trifluoromethylsulfonyl)imide [Pyr14][TFSI]), its polymeric ionic liquid analogue (Poly(diallyldimethylammonium bis(trifluoromethylsulfonyl)imide) [PDADMA][TFSI]), or an anionically charged backbone polymeric ionic liquid (lithium poly[(4\u2010styrenesulfonyl)(trifluoromethyl(S\u2010trifluoromethylsulfonylimino) sulfonyl) imide] LiP[STFSI]). The ion dynamics and molecular interactions within the GPEs were thoroughly analyzed using Attenuated Total Reflectance Fourier\u2010Transform Infrared Spectroscopy (ATR\u2010FTIR), Heteronuclear Overhauser Enhancement Spectroscopy (HOESY), and Pulsed\u2010Field Gradient Nuclear Magnetic Resonance Diffusion (PFG\u2010NMR). Li<jats:sup>+<\/jats:sup> transference numbers (t<jats:sub>Li<\/jats:sub>+) were successfully calculated. Our study found that by combining slow\u2010diffusing polymeric ionic liquids (PILs) with fast\u2010diffusing lithium salt, we were able to achieve transference numbers comparable to those of liquid electrolytes, especially with the anionic PIL, LiP[STFSI]. This research highlights the influence of the polymer\u2032s nature on lithium\u2010ion transport within GPEs. Additionally, micro supercapacitor (MSC) devices assembled with these GPEs exhibited capacitive behavior. These findings suggest that further optimization of GPE composition could significantly improve their performance, thereby positioning them for application in sustainable and efficient energy storage systems.<\/jats:p>","DOI":"10.1002\/cssc.202401710","type":"journal-article","created":{"date-parts":[[2024,11,6]],"date-time":"2024-11-06T22:29:28Z","timestamp":1730932168000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Poly(Ionic) Liquid\u2010Enhanced Ion Dynamics in Cellulose\u2010Derived Gel Polymer Electrolytes"],"prefix":"10.1002","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1207-9452","authenticated-orcid":false,"given":"Tiago G.","family":"Paiva","sequence":"first","affiliation":[{"name":"I3N Cenimat Department of Materials Science (DCM) NOVA School of Science and Technology NOVA University of Lisbon  Caparica 2829-516 Portugal"},{"name":"Centro de Qu\u00edmica Estrutural Institute of Molecular Sciences and Departamento de Engenharia Qu\u00edmica Instituto Superior T\u00e9cnico, Universidade de Lisboa, Avenida Rovisco Pais  Lisboa 1049-001 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6301-8895","authenticated-orcid":false,"given":"Maykel","family":"Klem","sequence":"additional","affiliation":[{"name":"I3N Cenimat Department of Materials Science (DCM) NOVA School of Science and Technology NOVA University of Lisbon  Caparica 2829-516 Portugal"},{"name":"School of Technology and Sciences S\u00e3o Paulo State University (UNESP)  Presidente Prudente SP 19060-900 Brazil"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3560-4317","authenticated-orcid":false,"given":"Sara L.","family":"Silvestre","sequence":"additional","affiliation":[{"name":"I3N Cenimat Department of Materials Science (DCM) NOVA School of Science and Technology NOVA University of Lisbon  Caparica 2829-516 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4217-3842","authenticated-orcid":false,"given":"Jo\u00e3o","family":"Coelho","sequence":"additional","affiliation":[{"name":"I3N Cenimat Department of Materials Science (DCM) NOVA School of Science and Technology NOVA University of Lisbon  Caparica 2829-516 Portugal"},{"name":"Dpto. F\u00edsica de la Materia Condensada Instituto de Ciencia de Materiales de Sevilla (Universidad de Sevilla-CSIC  Avda. 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