@Article{jpm.2026.087360,
AUTHOR = {Ruoxi Zhang, Rongzu Sun, Wei Zhou, Zhen Chen},
TITLE = {Segmental Dynamics, Ion-Associated Relaxation, and Ion Transport in Cellulose-Based Gel Polymer Electrolytes Revealed by Broadband Dielectric Spectroscopy},
JOURNAL = {Journal of Polymer Materials},
VOLUME = {},
YEAR = {},
NUMBER = {},
PAGES = {{pages}},
URL = {http://www.techscience.com/jpm/online/detail/28400},
ISSN = {0976-3449},
ABSTRACT = {Cellulose-based gel polymer electrolytes (GPEs) are promising sustainable candidates for next-generation lithium batteries; however, the relationship between polymer dynamics and ion transport remains insufficiently understood. In this study, cellulose-based GPEs with varying lithium salt concentrations and crosslinking densities were systematically investigated using broadband dielectric spectroscopy, complemented by structural and thermal characterizations. Three dielectric relaxations including a secondary <math id="mml-ieqn-1">	 
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</math> relaxation, a structural <math id="mml-ieqn-2">	 
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</math> relaxation arising from cooperative segmental motion of the cellulose network, and a slower near-Debye <math id="mml-ieqn-3">	 
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</math> relaxation were identified. Both the <math id="mml-ieqn-4">	 
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</math> and <math id="mml-ieqn-5">	 
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</math> processes follow Vogel–Fulcher–Tammann (VFT) behavior, indicating their strong coupling with the glassy dynamics of the polymer matrix. The <math id="mml-ieqn-6">	 
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</math> process is plausibly ascribed to orientational polarization of ion-associated species, such as transient ion pairs or small ionic aggregates coordinated with the cellulose network. The direct current conductivity of the samples was also found following VFT behavior. Notably, the conductivity relaxation time nearly coincides with the <math id="mml-ieqn-7">	 
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</math> relaxation time across the entire investigated temperature range for all compositions, suggesting that lithium-ion transport is predominantly governed by polymer segmental dynamics. The dielectric glass transition temperature and fragility index, derived from VFT analysis, exhibit marked dependencies on salt concentration and crosslinking density, whereas the calorimetric glass transition temperature remains virtually invariant. This work unveils a strongly coupled ion-transport mechanism and provides fundamental insights into the intricate interplay among polymer dynamics, ionic association, and charge transport in cellulose-based GPEs.},
DOI = {10.32604/jpm.2026.087360}
}