Journal of Polymer & Composites Original Research
A Review of Modified Cellulose for Electrochemical Energy Storage with a Multiphysics Framework for Quaternized Bagasse Nanocellulose/Al₂O₃–PEO Composite Electrolytes in Solid-State Batteries
Abstract
A critical review of modified cellulose for electrochemical energy storage is integrated with a potassium-specific multiphysics framework using cellulose obtainable from India-relevant feedstocks, including sugarcane bagasse, cotton/cotton stalk, banana pseudostem, Hibiscus/kenaf-type biomass, and other agricultural residues. The framework addresses the coupled requirements of ambient-temperature ionic transport, K⁺ selectivity, and mechanical integrity in solid polymer electrolytes. A hierarchical QCNF@Al₂O₃/PEO₁₆–KTFSI₁ architecture is evaluated in which quaternized bagasse cellulose nanofibers provide percolated reinforcement and fixed cationic sites for partial TFSI⁻ immobilization, while low-loading Al₂O₃ acts primarily as an interfacial modifier. A literature-bounded reduced-order model couples Vogel–Tammann–Fulcher transport, composite crystallinity, fixed-charge-mediated transference enhancement, interfacial effects, filler tortuosity, and percolation reinforcement. The Pareto-knee composition, 4 wt% QCNF + 2 wt% Al₂O₃ at effective DS=0.30, gives nominal predictions of σ₂₅=7.33×10⁻⁵ S cm⁻¹, tK=0.391, σK,₂₅=2.86×10⁻⁵ S cm⁻¹, and G′₂₅=5.55 MPa. Relative to PEO₁₆–KTFSI₁, it increases total and K⁺-specific conductivity by 2.06 and 4.73 times, respectively, while reducing the concentration-polarization proxy by 64.3%. Monte Carlo propagation (20,000 realizations) provides uncertainty intervals for transport and modulus. Thickness-dependent resistance and thermal safety are treated as explicit validation variables: area-specific bulk resistance scales as L/σ, and TGA must confirm a decomposition onset well above the 25–55 °C operating window. The framework identifies a directly testable formulation and validation pathway combining structural characterization, EIS, transference-number measurement, rheology, K-metal symmetric cells, and Prussian-blue full cells.
Keywords
References (50)
- Wang T, Yu Q, Li Z, et al. The potential of solid-state potassium-ion batteries with polymer-based electrolytes. Carbon Energy. 2025;7:e670. doi:10.1002/cey2.670.
- Khudyshkina AD, Morozova PA, Butzelaar AJ, et al. Poly(ethylene oxide)-based electrolytes for solid-state potassium metal batteries with a Prussian Blue positive electrode. ACS Applied Polymer Materials. 2022;4:2734–2746. doi:10.1021/acsapm.2c00014.
- Khudyshkina AD, Rauska UC, Butzelaar AJ, et al. Impact of nano-sized inorganic fillers on PEO-based electrolytes for potassium batteries. Batteries & Supercaps. 2024;7:e202300404. doi:10.1002/batt.202300404.
- Zheng J, Schkeryantz L, Gourdin G, Qin L, Wu Y. Single potassium-ion conducting polymer electrolytes: Preparation, ionic conductivities, and electrochemical stability. ACS Applied Energy Materials. 2021;4:4156–4164. doi:10.1021/acsaem.1c00483.
- Mönich C, Andersson R, Hernández G, Mindemark J, Schönhoff M. Seeing the unseen: Mg²⁺, Na⁺, and K⁺ transference numbers in post-Li battery electrolytes by electrophoretic nuclear magnetic resonance. Journal of the American Chemical Society. 2024;146:11105–11114. doi:10.1021/jacs.3c12272.
- Prado-Martínez C, Sutton P, Mombrini I, et al. Cellulose nanofiber-reinforced solid polymer electrolytes with high ionic conductivity for lithium batteries. Journal of Materials Chemistry A. 2023;11:9521–9529. doi:10.1039/D3TA00380A.
- Kim GT, Antonelli C, Iojoiu C, et al. Nanocrystalline cellulose reinforced poly(ethylene oxide) electrolytes for lithium-metal batteries with excellent cycling stability. Frontiers in Energy Research. 2023;11:1325612. doi:10.3389/fenrg.2023.1325612.
- Ji C, Wu S, Tang F, Yu Y, Hung F, Wei Q. Cationic cellulose nanofiber solid electrolytes: A pathway to high lithium-ion migration and polysulfide adsorption for lithium-sulfur batteries. Carbohydrate Polymers. 2024;335:122075. doi:10.1016/j.carbpol.2024.122075.
- Atifi S, Miao C, Mirvakili MN, Hamad WY. On the ionic conductivity and mechanical behavior of cellulose-based electrolytes: Applications for rechargeable batteries. Colloids and Surfaces A: Physicochemical and Engineering Aspects. 2024;686:133322. doi:10.1016/j.colsurfa.2024.133322.
- Alokika, Anu, Kumar A, Kumar V, Singh B. Cellulosic and hemicellulosic fractions of sugarcane bagasse: Potential, challenges and future perspective. International Journal of Biological Macromolecules. 2021;169:564–582. doi:10.1016/j.ijbiomac.2020.12.175.
- Abolore RS, Jaiswal S, Jaiswal AK. Green and sustainable pretreatment methods for cellulose extraction from lignocellulosic biomass and its applications: A review. Carbohydrate Polymer Technologies and Applications. 2024;7:100396. doi:10.1016/j.carpta.2023.100396.
- Cao K, Ma J, Yue Z, Li H, Fan Y, Liu H. Status and challenges of solid-state electrolytes for potassium batteries. Small. 2026;22(12):e2500762. doi:10.1002/smll.202500762.
- Sun J, Du Y, Liu Y, et al. Recent advances in potassium metal batteries: Electrodes, interfaces and electrolytes. Chemical Society Reviews. 2025;54:2543–2594. doi:10.1039/D4CS00845F.
- Zhu X, Ali RN, Song M, Tang Y, Fan Z. Recent advances in polymers for potassium ion batteries. Polymers. 2022;14(24):5538. doi:10.3390/polym14245538.
- Johansson IL, Kolesnikov TI, Khudyshkina A, et al. Polycarbonate-based polymer electrolytes for potassium batteries. Solid State Ionics. 2025;432:117069. doi:10.1016/j.ssi.2025.117069.
- Gong X, Wang J, Zhong L, et al. Recent advances on cellulose-based solid polymer electrolytes. Industrial Chemistry & Materials. 2025;3:31–48. doi:10.1039/D4IM00066H.
- Zhang J, Liu J, Xu Z, Cao D, Chen K. Enabling sustainable future energy storage with cellulose-based solid-state electrolytes: A review. Materials Today Energy. 2025;54:102091. doi:10.1016/j.mtener.2025.102091.
- Wu H, Wang J, Zhao Y, et al. A branched cellulose-reinforced composite polymer electrolyte with upgraded ionic conductivity for anode-stabilized solid-state Li-metal batteries. Sustainable Energy & Fuels. 2019;3:2642–2656. doi:10.1039/C9SE00361D.
- Li J, Hu Z, Zhang S, et al. Molecular engineering of renewable cellulose biopolymers for solid-state battery electrolytes. Nature Sustainability. 2024;7:1481–1491. doi:10.1038/s41893-024-01414-7.
- Mahmud MA, Anannya FR. Sugarcane bagasse—A source of cellulosic fiber for diverse applications. Heliyon. 2021;7(8):e07771. doi:10.1016/j.heliyon.2021.e07771.
- Konde KS, Nagarajan S, Kumar V, Patil SV, Ranade VV. Sugarcane bagasse-based biorefineries in India: Potential and challenges. Sustainable Energy & Fuels. 2021;5:52–78. doi:10.1039/D0SE01332C.
- Evans J, Vincent CA, Bruce PG. Electrochemical measurement of transference numbers in polymer electrolytes. Polymer. 1987;28(13):2324–2328. doi:10.1016/0032-3861(87)90394-6.
- Bruce PG, Evans J, Vincent CA. Conductivity and transference number measurements on polymer electrolytes. Solid State Ionics. 1988;28–30:918–922. doi:10.1016/0167-2738(88)90304-9.
- Klemm D, Heublein B, Fink HP, Bohn A. Cellulose: Fascinating biopolymer and sustainable raw material. Angewandte Chemie International Edition. 2005;44:3358–3393. doi:10.1002/anie.200460587.
- Habibi Y, Lucia LA, Rojas OJ. Cellulose nanocrystals: Chemistry, self-assembly, and applications. Chemical Reviews. 2010;110:3479–3500. doi:10.1021/cr900339w.
- Moon RJ, Martini A, Nairn J, Simonsen J, Youngblood J. Cellulose nanomaterials review: Structure, properties and nanocomposites. Chemical Society Reviews. 2011;40:3941–3994. doi:10.1039/C0CS00108B.
- Isogai A, Saito T, Fukuzumi H. TEMPO-oxidized cellulose nanofibers. Nanoscale. 2011;3:71–85. doi:10.1039/C0NR00583E.
- Thomas B, Raj MC, B AK, et al. Nanocellulose, a versatile green platform: From biosources to materials and their applications. Chemical Reviews. 2018;118:11575–11625. doi:10.1021/acs.chemrev.7b00627.
- Chen C, Hu L. Nanocellulose toward advanced energy storage devices: Structure and electrochemistry. Accounts of Chemical Research. 2018;51:3154–3165. doi:10.1021/acs.accounts.8b00391.
- Nargatti KI, Subhedar AR, Ahankari SS, Grace AN, Dufresne A. Nanocellulose-based aerogel electrodes for supercapacitors: A review. Carbohydrate Polymers. 2022;297:120039. doi:10.1016/j.carbpol.2022.120039.
- Choudhary NN, Singh S, Bhardwaj S, et al. Recent advancements in nanocellulose-based supercapacitors for energy storage devices: A review. Carbohydrate Polymer Technologies and Applications. 2024:100416. doi:10.1016/j.carpta.2023.100416.
- Wang Y, Xu T, Liu K, et al. Nanocellulose-based advanced materials for flexible supercapacitor electrodes. Industrial Crops and Products. 2023;204(B):117378. doi:10.1016/j.indcrop.2023.117378.
- Rath PC, Patra J, Huang HT, Bresser D, Wu TY, Chang JK. Carbonaceous anodes derived from sugarcane bagasse for sodium-ion batteries. ChemSusChem. 2019;12:2302–2309. doi:10.1002/cssc.201900319.
- Choudhary N, Tomar A, Singh S, Chandra R, Maji PK. Fabrication of a symmetric supercapacitor device using MnO₂/cellulose nanocrystals/graphite electrodes via sputtering for energy storage. Nanoscale. 2025;17:1289–1307. doi:10.1039/D4NR03476G.
- Rajivgandhi P, Thirumal V, Sekar A, Kim J. Sustainable sugarcane bagasse-derived activated carbon for high-performance symmetric supercapacitor device applications. Nanomaterials. 2025;15(13):1028. doi:10.3390/nano15131028.
- Abdelfadeel MA, Al Kiey SA, Hesemann P, et al. From sugarcane bagasse pulp into electroactive materials: Carboxymethyl cellulose/reduced graphene oxide/nickel oxide composites as high-performance supercapacitor components. International Journal of Biological Macromolecules. 2025;316(2):144703. doi:10.1016/j.ijbiomac.2025.144703.
- Kumar V, Chakraborty P, Janghu P, et al. Potential of banana-based cellulose materials for advanced applications: A review on properties and technical challenges. Carbohydrate Polymer Technologies and Applications. 2023;6:100366. doi:10.1016/j.carpta.2023.100366.
- Nascimento REA, Carvalheira M, Crespo JG, Neves LA. Extraction and characterization of cellulose obtained from banana plant pseudostem. Clean Technologies. 2023;5:1028–1043. doi:10.3390/cleantechnol5030052.
- Cheng J, Hu SC, Sun GT, Kang K, Zhu MQ, Geng ZC. Comparison of activated carbons prepared by one-step and two-step chemical activation processes based on cotton stalk for supercapacitor applications. Energy. 2021;215(B):119144. doi:10.1016/j.energy.2020.119144.
- Tian J, Zhang T, Talifu D, Abulizi A, Ji Y. Porous carbon materials derived from waste cotton stalk with ultra-high surface area for high-performance supercapacitors. Materials Research Bulletin. 2021;143:111457. doi:10.1016/j.materresbull.2021.111457.
- Song D, Liu W, Liu C, Li H. Recent progress of bacterial cellulose-based separator platforms for lithium-ion and lithium-sulfur batteries. International Journal of Biological Macromolecules. 2024;274(2):133419. doi:10.1016/j.ijbiomac.2024.133419.
- Hassoun J, Kimura K, Tominaga Y. Cellulose-based electrolytes in rechargeable Zn-battery: An overview. Advanced Sustainable Systems. 2025. doi:10.1002/adsu.202500287.
- Lv P, Lu X, Wang L, Feng W. Nanocellulose-based functional materials: From chiral photonics to soft actuator and energy storage. Advanced Functional Materials. 2021;31:2104991. doi:10.1002/adfm.202104991.
- Du K, Teng Y, Zhang S, Tam KC. Recent progress on solid-state electrolytes based on nanocellulose: Structures, applications, and challenges. Materials Today Energy. 2025;51:101891. doi:10.1016/j.mtener.2025.101891.
- Safavi-Mirmahalleh SA, Eliseeva SN, Moghaddam AR, Roghani-Mamaqani H, Salami-Kalajahi M. Evaluation of crosslinked cellulose-based solid and gel polymer electrolytes in lithium-ion batteries. International Journal of Biological Macromolecules. 2025;327(2):147508. doi:10.1016/j.ijbiomac.2025.147508.
- Tang Z, Lin X, Yu M, Mondal AK, Wu H. Recent advances in TEMPO-oxidized cellulose nanofibers: Oxidation mechanism, characterization, properties and applications. International Journal of Biological Macromolecules. 2024;259(1):129081. doi:10.1016/j.ijbiomac.2023.129081.
- Cardenas-Riojas AA, Gualdron-Plata AP, Pastor E, Martins VL, Baena-Moncada AM. Electrochemical performance of electrochemical capacitors prepared with activated carbons from sugarcane bagasse. New Journal of Chemistry. 2026;50:3933–3946. doi:10.1039/D5NJ04251H.
- Shi L, Xiao T, Wang X, Huang L, Wu L, Shi H. Recent advances in sustainable cellulose-based supercapacitors: Diverse applications, crucial challenges, and coping strategies. Carbohydrate Polymers. 2026;371:124478. doi:10.1016/j.carbpol.2025.124478.
- Chen Z, Zheng H, Yi J, et al. Advanced cellulose-based materials for flexible energy storage systems. Resources Chemicals and Materials. 2025;4(3):100120. doi:10.1016/j.recm.2025.100120.
- Zhang Z, Cui K, Zhang J, Xu Y, Xu F. Cellulose-based solid-state electrolytes for solid-state lithium metal batteries: Advances in functionalization strategies and interfacial engineering. Advanced Energy Materials. 2026;16(9):e04386. doi:10.1002/aenm.202504386.