Volume 11 Issue 2
May  2026
Turn off MathJax
Article Contents
Aoxue Lang, Zhiying Liang, Wu Yang, Ziyu Guo, Kasim Ocakoglu, Emmanuel Iwuoha, Ruidong Xia, Xinwen Peng. Multiscale dual-network cellulose hydrogel electrolytes for dendrite-free Zn anode[J]. Journal of Bioresources and Bioproducts, 2026, 11(2): 100232. doi: 10.1016/j.jobab.2026.100232
Citation: Aoxue Lang, Zhiying Liang, Wu Yang, Ziyu Guo, Kasim Ocakoglu, Emmanuel Iwuoha, Ruidong Xia, Xinwen Peng. Multiscale dual-network cellulose hydrogel electrolytes for dendrite-free Zn anode[J]. Journal of Bioresources and Bioproducts, 2026, 11(2): 100232. doi: 10.1016/j.jobab.2026.100232

Multiscale dual-network cellulose hydrogel electrolytes for dendrite-free Zn anode

doi: 10.1016/j.jobab.2026.100232
Funds:

We are grateful for the financial support by National Natural Science Foundation of China (No. 32401519, No 32471811, and No 32201499), Guangdong Basic and Applied Basic Research Foundation (No. 2023B1515040013, No 2025A1515011107, and No 2024A1515011229), National Key Research and Development Project (No. 2023YFE0109600), Guangzhou Key Research and Development Program (No. 2023B03J1330), State Key Laboratory of Advanced Papermaking and Paper-based Materials (No. 2024C04), and Guangzhou Basic and Applied Basic Research Foundation (No. 2024A04J3413 and No 2024A04J3704).

  • Received Date: 2025-09-03
  • Accepted Date: 2025-12-20
  • Rev Recd Date: 2025-11-24
  • Available Online: 2026-05-07
  • Publish Date: 2026-01-12
  • Aqueous zinc-ion batteries (AZIBs) have emerged as promising energy storage systems owing to their high safety, low cost, and environmental friendliness. However, their practical application faces critical challenges, including the formation of Zn dendrites and the occurrence of parasitic side reactions. These phenomena not only hinder ion transport kinetics but also cause rapid capacity decay and potential battery failure. To address these limitations, we developed a sustainable double-crosslinked cellulose hydrogel electrolyte by integrating micron-sized cellulose and cellulose nanofibers (CNFs). The hydrogel electrolyte, constructed from cellulose components with distinct size scales, exhibits a well-organized hierarchical porous network structure, which significantly facilitates the migration of zinc ions. Specifically, nanocellulose serves as a reinforcing filler that enhances the mechanical strength of the dual-network electrolyte, thereby inhibiting Zn dendrite growth. Additionally, abundant carboxyl polar functional groups were also introduced as high-affinity Zn2+ binding sites to mitigate side reactions. Consequently, the assembled Zn//Zn symmetric cells with this electrolyte demonstrate superior cycling stability exceeding 1100 h at current density of 0.5 mA/cm2, along with a high-capacity retention of 79.9% after 1000 cycles in the Zn//V2O5 battery. Furthermore, this cellulose hydrogel electrolyte is easily accessible and biodegradable, paving the way for the scalable production of high-performance and environmentally friendly energy storage devices.

     

  • loading
  • [1]
    Cao, J., Zhang, D.D., Zhang, X.Y., Zeng, Z.Y., Qin, J.Q., Huang, Y.H., 2022. Strategies of regulating Zn2+ solvation structures for dendrite-free and side reaction-suppressed zinc-ion batteries. Energy Environ. Sci. 15, 499–528.
    [2]
    Cao, M.Y., Zhu, J.Q., Miao, G.H., Sha, J., Li, D.Q., Li, J., Wang, C., Li, C.H., Zhang, J.K., Xu, Y.L., Chen, S., Xu, F., 2025. Ambient-dried nanocellulose composite aerogels for enhanced hydrovoltaic electricity generation. Adv. Funct. Mater. 35, 2418823.
    [3]
    Chen, M.F., Chen, J.Z., Zhou, W.J., Xu, J.L., Wong, C.P., 2019. High-performance flexible and self-healable quasi-solid-state zinc-ion hybrid supercapacitor based on borax-crosslinked polyvinyl alcohol/nanocellulose hydrogel electrolyte. J. Mater. Chem. A 7, 26524–26532.
    [4]
    Chen, K., Huang, J., Yuan, J.L., Qin, S.D., Huang, P.F., Wan, C., You, Y., Guo, Y.L., Xu, Q.Q., Xie, H.B., 2023. Molecularly engineered cellulose hydrogel electrolyte for highly stable zinc ion hybrid capacitors. Energy Stor. Mater. 63, 102963.
    [5]
    Deka, M., Longkumar, Y., Boruah, B., Sarmah, H., Konwar, M., Borthakur, L.J., 2024. Borax cross-linked guar gum hydrogel-based self healing polymer electrolytes filled with ceramic nanofibers towards high-performance green energy storage applications. React. Funct. Polym. 195, 105822.
    [6]
    Ding, Y., Pang, Z.Q., Lan, K., Yao, Y., Panzarasa, G., Xu, L., Lo Ricco, M., Rammer, D.R., Zhu, J.Y., Hu, M., Pan, X.J., Li, T., Burgert, I., Hu, L.B., 2023. Emerging engineered wood for building applications. Chem. Rev. 123, 1843–1888.
    [7]
    Dong, Q., Zhang, X., Qian, J., He, S.M., Mao, Y.M., Brozena, A.H., Zhang, Y., Pollard, T.P., Borodin, O.A., Wang, Y.B., Chava, B.S., Das, S., Zavalij, P., Segre, C.U., Zhu, D.Y., Xu, L., Liang, Y.L., Yao, Y., Briber, R.M., Li, T., Hu, L.B., 2022. A cellulose-derived supramolecule for fast ion transport. Sci. Adv. 8, eadd2031.
    [8]
    Du, Y.X., Li, Y., Xu, B.B., Liu, T.X., Liu, X.Q., Ma, F.Y., Gu, X.X., Lai, C., 2022. Electrolyte salts and additives regulation enables high performance aqueous zinc ion batteries: A mini review. Small 18, 2104640.
    [9]
    Fang, Y., Xie, X.S., Zhang, B.Y., Chai, Y.Z., Lu, B.G., Liu, M.K., Zhou, J., Liang, S.Q., 2022. Regulating zinc deposition behaviors by the conditioner of PAN separator for zinc-ion batteries. Adv. Funct. Mater. 32, 2109671.
    [10]
    Ge, H.Y., Xie, X., Xie, X.S., Zhang, B.Y., Li, S.L., Liang, S.Q., Lu, B.G., Zhou, J., 2024. Critical challenges and solutions: Quasi-solid-state electrolytes for zinc-based batteries. Energy Environ. Sci. 17, 3270–3306.
    [11]
    Gea, S., Reynolds, C.T., Roohpour, N., Wirjosentono, B., Soykeabkaew, N., Bilotti, E., Peijs, T., 2011. Investigation into the structural, morphological, mechanical and thermal behaviour of bacterial cellulose after a two-step purification process. Bioresour. Technol. 102, 9105–9110.
    [12]
    Gomez Vazquez, D., Tabor, J., Pollard, T.P., Borodin, O., Lukatskaya, M.R., 2025. Measuring Zn transference with precision: Insights for dendrite-free zinc metal anodes. Adv. Mater. 37, e02245.
    [13]
    Guo, J., Wang, Y.J., Li, S.H., Qin, Y.Y., Meng, Y.S., Jiang, L.T., Huang, H., Shen, L.D., 2023. Chitosan hydrogel polyelectrolyte-modified cotton pad as dendrite-inhibiting separators for stable zinc anodes in aqueous zinc-ion batteries. J. Power Sources 580, 233392.
    [14]
    Jiang, C.G., Zhou, C.Y., Tang, W., Chen, G.H., Yin, S.N., Xie, W.Y., Wu, D.F., 2023. Crosslinking of bacterial cellulose toward fabricating ultrastretchable hydrogels for multiple sensing with high sensitivity. ACS Sustain. Chem. Eng. 11, 11548–11558.
    [15]
    Jin, H.T., Zhang, T.Y., Tian, Z.W., Jiang, S.H., 2024. Study on capacitive performance of bamboo-derived thick carbon electrodes using one-step activation method. J. Forestry Engineer. 9, 103–109.
    [16]
    Li, Q., Yan, B.X., Wang, D.H., Yang, Q., Huang, Z.D., Fan, J., Dai, M., Chen, W.S., Zhi, C.Y., 2022. Mechanistic study of interfacial modification for stable Zn anode based on a thin separator. Small 18, 2201045.
    [17]
    Li, C.Y., Wang, J.L., Zhang, D.T., Li, M.P., Chen, H., Yi, W.H., Ren, X.Y., Liu, B., Lu, X.F., Liu, M.C., 2024a. In-situ physical/chemical cross-linked hydrogel electrolyte achieving ultra-stable zinc anode-electrolyte interface towards dendrite-free zinc ion battery. J. Energy Chem. 97, 342–351.
    [18]
    Li, X.Y., Li, Y., Wang, R., Wang, D.H., Ran, F., 2024b Ion confinement effect enabled by carboxymethyl cellulose/tannic acid hybrid hydrogel electrolyte toward stable zinc anode. Chem. Eng. J. 496, 153865.
    [19]
    Li, Y., Yang, S., You, Y., Li, Y.Q., Zhang, Y.H., Wu, Q., Li, S.Z., Xu, Q.Q., Huang, J., Xie, H.B., 2024c. Cellulose nanocrystals built multiscale hydrogel electrolyte for highly reversible all-flexible zinc ion batteries. Chem. Eng. J. 496, 154357.
    [20]
    Liang, Y.X., Qiu, M.J., Sun, P., Mai, W.J., 2023. Comprehensive review of electrolyte modification strategies for stabilizing Zn metal anodes. Adv. Funct. Mater. 33, 2304878.
    [21]
    Lin, Y., Huang, J., Wang, S.J., Qi, L.H., Chen, W.M., Yu, L., Chen, C.J., 2025. Stretchable, adhesive, anti-freezing hydrogel electrolytes with dual-functional water regulation enabled by amide group–salt–water interactions for all-climate zinc-ion batteries. Adv. Mater. 37, e09975.
    [22]
    Liu, H.Y., Wang, J.G., You, Z.Y., Wei, C.G., Kang, F.Y., Wei, B.Q., 2021. Rechargeable aqueous zinc-ion batteries: Mechanism, design strategies and future perspectives. Mater. Today 42, 73–98.
    [23]
    Liu, Y., Chen, Y.A., Qi, H.S., 2022. Recyclable cellulose nanofibers reinforced poly (vinyl alcohol) films with high mechanical strength and water resistance. Carbohydr. Polym. 293, 119729.
    [24]
    Liu, Y., Wu, Y.K., Zhou, X.M., Mo, Y., Zheng, Y., Yuan, G.H., Yang, M.S., 2025. All-cellulose-based flexible zinc-ion battery enabled by waste pomelo peel. J. Colloid Interface Sci. 678, 497–505.
    [25]
    Lv, Y.Q., Xiao, Y., Ma, L.T., Zhi, C.Y., Chen, S.M., 2022. Recent advances in electrolytes for “beyond aqueous” zinc-ion batteries. Adv. Mater. 34, 2106409.
    [26]
    Lv, L., Hui, B., Zhang, X.H., Zou, Y.H., Yang, D.J., 2023. Lamellar agarose/graphene oxide gel polymer electrolyte network for all-solid-state supercapacitor. Chem. Eng. J. 452, 139443.
    [27]
    Manzano-Agugliaro, F., Alcayde, A., Montoya, F.G., Zapata-Sierra, A., Gil, C., 2013. Scientific production of renewable energies worldwide: An overview. Renew. Sustain. Energy Rev. 18, 134–143.
    [28]
    Peng, H.L., Wang, D.D., Zhang, F.L., Yang, L.S., Jiang, X.L., Zhang, K.Y., Qian, Z., Yang, J., 2024. Improvements and challenges of hydrogel polymer electrolytes for advanced zinc anodes in aqueous zinc-ion batteries. ACS Nano 18, 21779–21803.
    [29]
    Quan, Y.H., Zhou, W.J., Wu, T., Chen, M.F., Han, X., Tian, Q.H., Xu, J.L., Chen, J.Z., 2022. Sorbitol-modified cellulose hydrogel electrolyte derived from wheat straws towards high-performance environmentally adaptive flexible zinc-ion batteries. Chem. Eng. J. 446, 137056.
    [30]
    Saito, T., Kimura, S., Nishiyama, Y., Isogai, A., 2007. Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. Biomacromolecules 8(8), 2485–2491.
    [31]
    Shao, W., Wu, J.M., Liu, H., Ye, S., Jiang, L., Liu, X.F., 2017. Novel bioactive surface functionalization of bacterial cellulose membrane. Carbohydr. Polym. 178, 270–276.
    [32]
    Su, Y., Wang, X.L., Zhou, S., Zou, X.Q., Sun, H.Z., Liu, D.T., Zhu, G.S., 2022. A specific free-volume network as synergistic zinc–ion–conductor interface towards stable zinc anode. Energy Stor. Mater. 53, 909–916.
    [33]
    Sun, C., Wu, C.P., Gu, X.X., Wang, C., Wang, Q.H., 2021. Interface engineering via Ti3C2Tx MXene electrolyte additive toward dendrite-free zinc deposition. Nanomicro Lett. 13, 89.
    [34]
    Takeno, H., Inoguchi, H., Hsieh, W.C., 2020. Mechanical and structural properties of cellulose nanofiber/poly(vinyl alcohol) hydrogels cross-linked by a freezing/thawing method and borax. Cellulose 27, 4373–4387.
    [35]
    Tang, Y., Liu, C.X., Zhu, H.R., Xie, X.S., Gao, J.W., Deng, C.B., Han, M.M., Liang, S.Q., Zhou, J., 2020. Ion-confinement effect enabled by gel electrolyte for highly reversible dendrite-free zinc metal anode. Energy Stor. Mater. 27, 109–116.
    [36]
    Tanpichai, S., Phoothong, F., Boonmahitthisud, A., 2022. Superabsorbent cellulose-based hydrogels cross-liked with borax. Sci. Rep. 12, 8920.
    [37]
    Tian, C., Wang, J.L., Sun, R.X., Ali, T., Wang, H.F., Xie, B.B., Zhong, Y.J., Hu, Y., 2023. Improved interfacial ion migration and deposition through the chain-liquid synergistic effect by a carboxylated hydrogel electrolyte for stable zinc metal anodes. Angew. Chem. Int. Ed. 62, e202310970.
    [38]
    Wan, X.J., Xie, Q.R., Song, H.Q., Li, C.M., Wang, J.W., 2022. Borax-crosslinked hydrogel electrolyte membranes for quasi-solid state aqueous energy storage devices. J. Membr. Sci. 655, 120606.
    [39]
    Wang, Y.B., Li, Q., Hong, H., Yang, S., Zhang, R., Wang, X.Q., Jin, X., Xiong, B., Bai, S.C., Zhi, C.Y., 2023. Lean-water hydrogel electrolyte for zinc ion batteries. Nat. Commun. 14, 3890.
    [40]
    Wu, M.L., Zhang, Y., Xu, L., Yang, C.P., Hong, M., Cui, M.J., Clifford, B.C., He, S.M., Jing, S.S., Yao, Y., Hu, L.B., 2022. A sustainable chitosan-zinc electrolyte for high-rate zinc-metal batteries. Matter 5, 3402–3416.
    [41]
    Xu, L., Meng, T.T., Zheng, X.Y., Li, T.Y., Brozena, A.H., Mao, Y.M., Zhang, Q., Clifford, B.C., Rao, J.C., Hu, L.B., 2023. Nanocellulose-carboxymethylcellulose electrolyte for stable, high-rate zinc-ion batteries. Adv. Funct. Mater. 33, 2302098.
    [42]
    Xu, J.H., Zou, Y.J., Chen, H., Wan, Z.M., Takagi, A., Wang, Z.G., Yu, J., Liu, L., Lu, Y., Fan, Y.M., Rojas, O.J., 2025. Magnetoresponsive cellulose nanofiber hydrogels: Dynamic structuring, selective light transmission, and information encoding. ACS Nano 19(14), 14063–14072.
    [43]
    Yan, D., Li, H.B., Yang, A.M., Wang, M.L., Nie, K.Q., Lv, X.X., Deng, J.J., 2025. Ultrafast synthesis of vanadium-based oxides with crystalline-amorphous heterostructure for advanced aqueous zinc-ion batteries. Chem. Eng. J. 504, 158966.
    [44]
    Yang, W., Yang, W., Zeng, J.M., Chen, Y.L., Huang, Y.F., Liu, J., Gan, J.Y., Li, T.Z., Zhang, H., Zhong, L.X., Peng, X.W., 2024. Biopolymer-based gel electrolytes for electrochemical energy storage: Advances and prospects. Prog. Mater. Sci. 144, 101264.
    [45]
    Yang, W., Yang, W., Huang, Y.F., Wu, Y.R., Ma, X.Y., Dong, L.B., Peng, X.W., 2025a. Stable Zn anodes enabled by all-cellulose separators with synergistic hydroxyl and carboxyl chemistry. Energy Stor. Mater. 80, 104436.
    [46]
    Yang, W., Zeng, J.M., Lang, A.X., Zhou, K.Y., Yang, W., Peng, X.W., 2025b Biomass-based separators for aqueous zinc-ion batteries: Advantages, strategies, and perspectives. J. Mater. Chem. A 13, 31978–32003.
    [47]
    Yang, W., Zeng, J.M., Yang, W., Lang, A.X., Zhao, M., Zhong, L.X., Lu, J., Peng, X.W., 2025c. Regulating ion migration and deposition through a cellulose hydrogel electrolyte enabled by anion-reinforced effect for zinc-ion batteries. Adv. Funct. Mater. e07159.
    [48]
    Yin, J.Y., Feng, X., Gan, Z.H., Gao, Y., Cheng, Y.H., Xu, X., 2023. From anode to cell: Synergistic protection strategies and perspectives for stabilized Zn metal in mild aqueous electrolytes. Energy Stor. Mater. 54, 623–640.
    [49]
    Zeng, J.M., Yang, W., Yang, W., Zheng, Z.Y., Gan, J.Y., Wang, Q., Dong, L.B., Zhong, L.X., Xia, R.D., Iwuoha, E.I., Feleni, U., Admassie, S., Peng, X.W., 2024. Cellulose reinforced eutectogel electrolyte for flexible zinc-ion hybrid supercapacitors. ACS Appl. Energy Mater. 7, 6003–6012.
    [50]
    Zhang, Z.Y., Ding, T., Zhou, Q., Sun, Y.G., Qu, M., Zeng, Z.Y., Ju, Y.T., Li, L., Wang, K., Chi, F.D., 2021. A review of technologies and applications on versatile energy storage systems. Renew. Sustain. Energy Rev. 148, 111263.
    [51]
    Zhang, B.Y., Qin, L.P., Fang, Y., Chai, Y.Z., Xie, X.S., Lu, B.G., Liang, S.Q., Zhou, J., 2022. Tuning Zn2+ coordination tunnel by hierarchical gel electrolyte for dendrite-free zinc anode. Sci. Bull. 67, 955–962.
    [52]
    Zhang, H.D., Gan, X.T., Yan, Y.Y., Zhou, J.P., 2024a. A sustainable dual cross-linked cellulose hydrogel electrolyte for high-performance zinc-metal batteries. Nanomicro Lett. 16, 106.
    [53]
    Zhang, J.R., Lin, C.Y., Zeng, L.X., Lin, H., He, L.J., Xiao, F.Y., Luo, L.T., Xiong, P.X., Yang, X.H., Chen, Q.H., Qian, Q.R., 2024b A hydrogel electrolyte with high adaptability over a wide temperature range and mechanical stress for long-life flexible zinc-ion batteries. Small 20, 2312116.
    [54]
    Zhang, M.H., Li, J.H., Tang, Y.W., Wang, D.W., Hu, H.S., Liu, M.T., Xiao, B., Wang, P.F., 2024c. Selective Zn-ion channels enabled by a double-network protective layer for stable zinc anode. Energy Stor. Mater. 65, 103113.
    [55]
    Zhang, H.D., Gan, X.T., Gao, Y.J., Wu, H., Song, Z.P., Zhou, J.P., 2025. Carboxylic acid-functionalized cellulose hydrogel electrolyte for dual-interface stabilization in aqueous zinc-organic batteries. Adv. Mater. 37, 2411997.
    [56]
    Zheng, X.H., Ahmad, T., Chen, W., 2021. Challenges and strategies on Zn electrodeposition for stable Zn-ion batteries. Energy Stor. Mater. 39, 365–394.
    [57]
    Zheng, Z.H., Cheng, W.K., Jiang, G.Y., Li, X.N., Sun, J.S., Zhu, Y., Zhao, D.W., Yu, H.P., 2024. Ethanol vapor-induced synthesis of robust, high-efficiency zinc ion gel electrolytes for flexible Zn-ion batteries. Small Struct. 5, 2400180.
    [58]
    Zhou, M., Chen, Y., Fang, G.Z., Liang, S.Q., 2022. Electrolyte/electrode interfacial electrochemical behaviors and optimization strategies in aqueous zinc-ion batteries. Energy Stor. Mater. 45, 618–646.
    [59]
    Zhou, J., Ma, Y.F., Chen, J.Q., Cai, Z.Y., Qi, L.H., Cui, J.Y., Deng, S.L., Ouyang, W.G., Fang, Z.Q., Qiu, X.Q., Chen, C.J., 2025. Supramolecular scale hydrophilicity regulation enabling efficient dewatering and assembly of nanocellulose into dense and strong bulk materials as sustainable plastic substitutes. Adv. Mater. 37, 2415313.
    [60]
    Zhu, Y.X., Huang, Z.M., Zheng, M.T., Chen, H., Qian, S.S., Sun, C., Tian, Y.H., Wu, Z.Z., Lai, C., Zhang, S.Q., Zhong, Y.L., 2024. Scalable construction of multifunctional protection layer with low-cost water glass for robust and high-performance zinc anode. Adv. Funct. Mater. 34, 2306085.
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索

    Article Metrics

    Article views (5) PDF downloads(0) Cited by()
    Proportional views
    Related

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return