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By spanning a broad frequency range from 30\u00a0kHz using FFC NMR to high-field NMR (500\u2013800\u00a0MHz), we reveal distinct relaxation mechanisms governing ion dynamics in ionogels with and without lithium salts. Our results highlight the role of hBN in modulating molecular rotation and translational motion, significantly affecting 1H and 19F relaxation profiles. The presence of Li+ alters the dynamic behavior in ionogels, enhancing anion mobility at the interface. Notably, 7Li relaxation reveals strong interactions with the hBN surface that cannot be detected by diffusion NMR. These findings underscore the importance of spanning a broad frequency range in NMR studies of ionogels and provide critical insights into optimizing their design as novel electrolytes.<\/jats:p>","DOI":"10.1063\/5.0271227","type":"journal-article","created":{"date-parts":[[2025,6,6]],"date-time":"2025-06-06T09:54:27Z","timestamp":1749203667000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":1,"title":["Ion dynamics in hexagonal boron nitride ionogel electrolytes"],"prefix":"10.1063","volume":"162","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9212-5334","authenticated-orcid":false,"given":"Giselle","family":"de Araujo Lima e Souza","sequence":"first","affiliation":[{"name":"Department of Physics, Hunter College, CUNY 1 , New York, New York 10065,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-4137-6585","authenticated-orcid":false,"given":"Moises","family":"Acero","sequence":"additional","affiliation":[{"name":"Department of Physics, Hunter College, CUNY 1 , New York, New York 10065,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-2538-3405","authenticated-orcid":false,"given":"Emilia","family":"Pelegano-Titmuss","sequence":"additional","affiliation":[{"name":"Department of Physics, Hunter College, CUNY 1 , New York, New York 10065,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4210-0531","authenticated-orcid":false,"given":"Phillip","family":"Stallworth","sequence":"additional","affiliation":[{"name":"Department of Physics, Hunter College, CUNY 1 , New York, New York 10065,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-5013-2550","authenticated-orcid":false,"given":"Cory M.","family":"Thomas","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Northwestern University 2 , Evanston, Illinois 60208,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4120-1426","authenticated-orcid":false,"given":"Mark C.","family":"Hersam","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Northwestern University 2 , Evanston, Illinois 60208,","place":["USA"]},{"name":"Department of Chemistry, Northwestern University 3 , Evanston, Illinois 60208,","place":["USA"]},{"name":"Department of Electrical and Computer Engineering, Northwestern University 4 , Evanston, Illinois 60208,","place":["USA"]}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6450-3019","authenticated-orcid":false,"given":"Pedro Jos\u00e9","family":"Oliveira Sebasti\u00e3o","sequence":"additional","affiliation":[{"name":"CeFEMA and Department of Physics, Instituto Superior T\u00e9cnico, Universidade de Lisboa 5 , Lisboa,","place":["Portugal"]}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5497-5274","authenticated-orcid":false,"given":"Steven","family":"Greenbaum","sequence":"additional","affiliation":[{"name":"Department of Physics, Hunter College, CUNY 1 , New York, New York 10065,","place":["USA"]}]}],"member":"317","published-online":{"date-parts":[[2025,6,6]]},"reference":[{"key":"2025061010113422600_c1","doi-asserted-by":"publisher","first-page":"188","DOI":"10.1016\/j.coelec.2020.01.015","article-title":"Recent advances in solid-state polymer electrolytes and innovative ionic liquids based polymer electrolyte systems","volume":"21","year":"2020","journal-title":"Curr. 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