Bioinspired Hierarchical Hydrogel Electrolyte for Ultralong-Life Flexible Zinc-Ion Batteries
Corresponding Author: Pengcheng Du
Nano-Micro Letters,
Vol. 18 (2026), Article Number: 399
Abstract
Hydrogel electrolytes are pivotal for flexible zinc-ion batteries (ZIBs) yet suffer from an intrinsic trade-off between mechanical robustness and ionic conductivity. Herein, drawing inspiration from the “adhesion-conduction” architecture of spider webs, we developed a hierarchical hydrogel electrolyte (MTP) by incorporating tannic acid (TA)-modified MXene nanosheets (MT) into a polyacrylamide (PAM) skeleton to construct uniform 3D ion-conductive pathways. This bioinspired hierarchy serves a dual function: The PAM framework ensures mechanical integrity, while the MT network creates directed low-resistance channels for Zn2+ transport. Specifically, the dense array of polar groups on MXene and phenolic hydroxyls on TA act as “sticky sites”, which accelerate desolvation kinetics and homogenize Zn2+ flux. Consequently, the MTP electrolyte achieves an impressive ionic conductivity of 27.69 mS cm−1 and a high Zn2+ transference number of 0.833. Enabled by this design, Zn//Zn symmetric cells demonstrate an ultralong lifespan of 4600 h (> 6 months) at 0.5 mA cm−2/0.5 mAh cm−2. Furthermore, Zn//Z-VO full cells exhibit outstanding cyclability, retaining 74.5% capacity after 2000 cycles at 2 A g−1 and maintaining durable operation for over 10,000 cycles at 5 A g−1. This work successfully translates a biological blueprint into a practical strategy for resolving the kinetic and stability challenges in high-performance flexible ZIBs.
Highlights:
1 Drawing inspiration from the “adhesion-conduction” architecture of spider webs, a hierarchical hydrogel electrolyte (MTP) is developed with uniform 3D ion-conductive pathways.
2 Specific “sticky sites” on the MXene/tannic acid network facilitate superior electrochemical properties, including a high Zn2+ transference number of 0.833 and ionic conductivity of 27.69 mS cm−1.
3 This strategy enables stable Zn anodes with an impressive lifespan of 4600 h (>6 months) and empowers flexible full cells with outstanding cyclability over 10,000 cycles.
Keywords
Download Citation
Endnote/Zotero/Mendeley (RIS)BibTeX
- X. Wu, Y. Chen, B. Tang, Q. Yan, D. Wu et al., CeOx-integrated dual site enhanced urea electrosynthesis from nitrate and carbon dioxide. Nat. Commun. 16(1), 8785 (2025). https://doi.org/10.1038/s41467-025-63839-8
- L.-L. Zhao, J.-Y. Wang, Y.-M. Wu, P.-F. Wang, Z.-L. Liu et al., Unlocking the multidimensional application and optimization mechanism of MOFs materials in aqueous zinc ion batteries. J. Energy Chem. 111, 249–273 (2025). https://doi.org/10.1016/j.jechem.2025.07.063
- Y. Yang, S. Bremner, C. Menictas, M. Kay, Modelling and optimal energy management for battery energy storage systems in renewable energy systems: a review. Renew. Sustain. Energy Rev. 167c, 112671 (2022). https://doi.org/10.1016/j.rser.2022.112671
- Z. Zhang, Y. Mu, L. Xiao, H. Hu, T. Xue et al., Hydrogel electrolytes for zinc-ion batteries: materials design, functional strategies, and future perspectives. Nano-Micro Lett. 18(1), 139 (2026). https://doi.org/10.1007/s40820-025-01993-w
- Y. Zhu, G. Liang, X. Cui, X. Liu, H. Zhong et al., Engineering hosts for Zn anodes in aqueous Zn-ion batteries. Energy Environ. Sci. 17(2), 369–385 (2024). https://doi.org/10.1039/D3EE03584K
- R. Wang, W. Chen, C. Zhang, R. Zhao, X. Wang, Electrochemically active Mn2+ enabling high-performance aqueous zinc ion batteries. Energy Fuels 38(14), 13436–13443 (2024). https://doi.org/10.1021/acs.energyfuels.4c02624
- D. Wu, H. Wang, Y. Nie, H. Wan, S. Liu et al., When covalent organic frameworks meet metals: from opportunities toward applications. Prog. Mater. Sci. 155, 101538 (2026). https://doi.org/10.1016/j.pmatsci.2025.101538
- J. Zhu, X. Ge, Z. Peng, L. Pan, Z. Peng et al., Interfacial regulation for zinc metal anode of aqueous zinc-ion battery. Green Energy Environ. 10(4), 689–708 (2025). https://doi.org/10.1016/j.gee.2024.11.001
- H. Yan, S. Li, J. Zhong, B. Li, An electrochemical perspective of aqueous zinc metal anode. Nano-Micro Lett. 16(1), 15 (2023). https://doi.org/10.1007/s40820-023-01227-x
- G. Zhang, Y. Chen, L. Fu, L. Zheng, K. Fan et al., Regulating the solvation sheath of zinc ions by supramolecular coordination chemistry toward ultrastable zinc anodes. SmartMat 5(3), e1216 (2024). https://doi.org/10.1002/smm2.1216
- X. Lu, L. Chen, W. Li, X. Zhang, W. Chi et al., Accelerating desolvation and constructing dual-storage channels for Zn2+ by ligand field engineering of polar organic molecules for high-performance zinc-ion batteries. Adv. Funct. Mater. 36(2), e13457 (2026). https://doi.org/10.1002/adfm.202513457
- W. Chen, Z. Xie, H. Chen, X. Wang, Low-cost aqueous electrolyte with MBA additives for uniform and stable zinc deposition. ACS Appl. Mater. Interfaces 16(23), 30580–30588 (2024). https://doi.org/10.1021/acsami.4c05430
- Y. Lv, C. Huang, M. Zhao, M. Fang, Q. Dong et al., Synergistic anion–cation chemistry enables highly stable Zn metal anodes. J. Am. Chem. Soc. 147(10), 8523–8533 (2025). https://doi.org/10.1021/jacs.4c16932
- J. Zhang, Z. Liu, M. Li, Y. Shi, H. Li et al., Synchronized regulating Zn2+ depositing/stripping processes to achieve ultra-stable aqueous zinc metal batteries. Energy Storage Mater. 81, 104451 (2025). https://doi.org/10.1016/j.ensm.2025.104451
- Z. Yan, F. Luo, S. Yang, Q. Wu, J. Zhang et al., Polydentate ligand-induced surface reconstruction of MIL-88A reinforced gel electrolytes for highly reversible zinc batteries via ion rectification and charge redistribution. Adv. Funct. Mater. 36(3), e14679 (2026). https://doi.org/10.1002/adfm.202514679
- Y. Yang, Q. He, C. Hu, X. Xie, S. Liang et al., Electron-initiated self-growth in situ hydrogel electrolyte with gradient protection interface enables stable zinc metal batteries. ACS Nano 19(23), 21717–21728 (2025). https://doi.org/10.1021/acsnano.5c04942
- R. Li, L. Zhang, X. Wang, F. Wu, L. Li et al., A stretchable and self-healing polymer-in-salt all-solid electrolyte for wearable zinc-ion batteries. Nano Res. 18(8), 94907536 (2025). https://doi.org/10.26599/nr.2025.94907536
- X. Hui, Z. Zhan, Z. Zhang, J. Yu, P. Jiang et al., Missing-linker defect functionalized metal-organic frameworks accelerating zinc ion conduction for ultrastable all-solid-state zinc metal batteries. ACS Nano 18(36), 25237–25248 (2024). https://doi.org/10.1021/acsnano.4c07907
- Y. Yang, C. Huang, H. Li, Z. Teng, H. Zhang et al., Study of a novel supramolecular hydrogel electrolyte for aqueous zinc ion batteries. J. Mater. Chem. C 11(28), 9559–9569 (2023). https://doi.org/10.1039/d3tc01284k
- D. Li, L. Cao, T. Deng, S. Liu, C. Wang, Design of a solid electrolyte interphase for aqueous Zn batteries. Angew. Chem. Int. Ed. 60(23), 13035–13041 (2021). https://doi.org/10.1002/anie.202103390
- D. Wang, D. Zhao, L. Chang, Y. Zhang, W. Wang et al., Interface engineering of electron-ion dual transmission channels for ultra-long lifespan quasi-solid zinc-ion batteries. Energy Storage Mater. 74, 103903 (2025). https://doi.org/10.1016/j.ensm.2024.103903
- H. Xia, W. Zhang, C. Miao, H. Chen, C. Yi et al., Ultra-thin amphiphilic hydrogel electrolyte for flexible zinc-ion paper batteries. Energy Environ. Sci. 17(18), 6507–6520 (2024). https://doi.org/10.1039/D4EE01993H
- W. Zeng, S. Zhang, J. Lan, Y. Lv, G. Zhu et al., Double network gel electrolyte with high ionic conductivity and mechanical strength for Zinc-ion batteries. ACS Nano 18(38), 26391–26400 (2024). https://doi.org/10.1021/acsnano.4c09879
- Y. Mao, H. Ren, J. Zhang, T. Luo, N. Liu et al., Modifying hydrogel electrolyte to induce Zinc deposition for dendrite-free Zinc metal anode. Electrochim. Acta 393, 139094 (2021). https://doi.org/10.1016/j.electacta.2021.139094
- P. Xu, Q. Zhang, X. Chen, J. Liu, N. Zhao et al., Multifunctional double-network hydrogel with enhanced interface engineering for high-performance flexible Zinc-air batteries. Chem. Eng. J. 522, 167206 (2025). https://doi.org/10.1016/j.cej.2025.167206
- Y. An, C. Shu, Y. Liu, Y. Xu, L. Kang et al., Modulating the hydrogen bond for a stable Zinc anode with a wide temperature range via the sucrose and polyacrylamide synergistic effect. ACS Nano 19(11), 11146–11163 (2025). https://doi.org/10.1021/acsnano.4c18178
- Q. He, Y. Zhong, J. Li, S. Chai, Y. Yang et al., Constructing kosmotropic salt-compatible PVA hydrogels for stable Zinc anodes via strong hydrogen bonds preshielding effect. Adv. Energy Mater. 14(23), 2400170 (2024). https://doi.org/10.1002/aenm.202400170
- C. Yang, P. Woottapanit, S. Geng, R. Chanajaree, Y. Shen et al., A multifunctional quasi-solid-state polymer electrolyte with highly selective ion highways for practical Zinc ion batteries. Nat. Commun. 16, 183 (2025). https://doi.org/10.1038/s41467-024-55656-2
- M. Sun, G. Ji, M. Li, J. Zheng, A robust hydrogel electrolyte with ultrahigh ion transference number derived from Zincophilic “chain-gear” network structure for dendrite-free aqueous Zinc ion battery. Adv. Funct. Mater. 34(37), 2402004 (2024). https://doi.org/10.1002/adfm.202402004
- J. Wang, X. Zou, L. Song, Y. Hou, J. Lu et al., A bio-inspired multifunctional interface layer for high performance Zinc-ion batteries via novel in situ electropolymerization. J. Mater. Chem. A 11(44), 23973–23983 (2023). https://doi.org/10.1039/D3TA04886A
- S. Yang, Q. Wu, Y. Li, F. Luo, J. Zhang et al., A bio-inspired multifunctional hydrogel network with toughly interfacial chemistry for dendrite-free flexible Zinc ion battery. Angew. Chem. Int. Ed. 63(44), e202409160 (2024). https://doi.org/10.1002/anie.202409160
- Q. Wang, J. Huang, L. Qi, M. Li, S. Wang et al., A bioinspired gradient hydrogel electrolyte network with optimized interfacial chemistry toward robust aqueous Zinc-ion batteries. ACS Nano 19(29), 26770–26781 (2025). https://doi.org/10.1021/acsnano.5c06914
- Y. Guo, Z. Chang, B. Li, Z.-L. Zhao, H.-P. Zhao et al., Functional gradient effects on the energy absorption of spider orb webs. Appl. Phys. Lett. 113(10), 103701 (2018). https://doi.org/10.1063/1.5039710
- Y. Liu, G. Tian, Y. Du, P. Shi, N. Li et al., Highly stretchable, low-hysteresis, and adhesive TA@MXene-composited organohydrogels for durable wearable sensors. Adv. Funct. Mater. 34(30), 2315813 (2024). https://doi.org/10.1002/adfm.202315813
- Y. Du, Y. Chen, M. Yang, S. Zou, X. Song et al., Poly(3, 4-ethylenedioxythiophene)–polystyrenesulfonate-added layered vanadium oxide cathode for high-performance zinc-ion batteries. ACS Appl. Energy Mater. 4(12), 14582–14589 (2021). https://doi.org/10.1021/acsaem.1c03209
- Q. Ma, A. Ma, S. Lv, B. Qin, Y. Xu et al., Regulating zinc ion transport behavior and solvated structure towards stable aqueous Zn metal batteries. J. Energy Chem. 93, 609–626 (2024). https://doi.org/10.1016/j.jechem.2024.02.016
- Y. Zhuang, Y. Liang, W. Zhang, Y. Sun, Z. Wang et al., Rational electrolyte structure engineering for highly reversible zinc metal anode in aqueous batteries. Nano-Micro Lett. 18(1), 102 (2026). https://doi.org/10.1007/s40820-025-01950-7
- X. Wu, Q. Yan, H. Wang, D. Wu, H. Zhou et al., Heterostructured catalytic materials as advanced electrocatalysts: classification, synthesis, characterization, and application. Adv. Funct. Mater. 34(42), 2404535 (2024). https://doi.org/10.1002/adfm.202404535
- J. Li, H. Zhang, Z. Liu, H. Du, H. Wan et al., Boosting dendrite-free zinc anode with strongly polar functional group terminated hydrogel electrolyte for high-safe aqueous zinc-ion batteries. Adv. Funct. Mater. 35(2), 2412865 (2025). https://doi.org/10.1002/adfm.202412865
- J. Cui, J. Wu, A. Feng, Y. Yu, L. Mi et al., Low infrared emissivity and oxidation stability of Ti3C2Tx MXene-based composite with tannic acid. Chem. Eng. J. 493, 152289 (2024). https://doi.org/10.1016/j.cej.2024.152289
- R.A. Soomro, P. Zhang, B. Fan, Y. Wei, B. Xu, Progression in the oxidation stability of MXenes. Nano-Micro Lett. 15(1), 108 (2023). https://doi.org/10.1007/s40820-023-01069-7
- W. Liu, S. Kang, Q. Zhang, S. Chen, Q. Yang et al., Self-assembly fabrication of chitosan-tannic acid/MXene composite film with excellent antibacterial and antioxidant properties for fruit preservation. Food Chem. 410, 135405 (2023). https://doi.org/10.1016/j.foodchem.2023.135405
- P. Zheng, X. Zhang, M. Yan, Y. Ma, Y. Jiang et al., The eruption of carbon chains in the oxidation of 2D Tin+1Cn (n = 1, 2, 3) MXenes. Appl. Surf. Sci. 550, 149310 (2021). https://doi.org/10.1016/j.apsusc.2021.149310
- M. Lai, C. Zhao, D. Wang, R. Gao, P. Cai et al., Significantly enhanced oxidation resistance and electrochemical performance of hydrothermal Ti3C2Tx MXene and tannic acid composite for high-performance flexible supercapacitors. ACS Appl. Mater. Interfaces 16(41), 55555–55568 (2024). https://doi.org/10.1021/acsami.4c13838
- Y. Zhang, L. Li, Y. Cao, Y. Yang, W. Wang et al., High-strength, low infrared-emission nonmetallic films for highly efficient Joule/solar heating, electromagnetic interference shielding and thermal camouflage. Mater. Horiz. 10(1), 235–247 (2023). https://doi.org/10.1039/D2MH01073A
- X. Li, Y. Li, R. Wang, D. Wang, F. Ran, Ion confinement effect enabled by carboxymethyl cellulose/tannic acid hybrid hydrogel electrolyte toward stable zinc anode. Chem. Eng. J. 496, 153865 (2024). https://doi.org/10.1016/j.cej.2024.153865
- L. Liu, C. Ge, Y. Zhang, W. Ma, X. Su et al., Tannic acid-modified silver nanops for enhancing anti-biofilm activities and modulating biofilm formation. Biomater. Sci. 8(17), 4852–4860 (2020). https://doi.org/10.1039/d0bm00648c
- H. Dou, X. Wu, M. Xu, R. Feng, Q. Ma et al., Steric-hindrance effect tuned ion solvation enabling high performance aqueous zinc ion batteries. Angew. Chem. Int. Ed. 63(21), e202401974 (2024). https://doi.org/10.1002/anie.202401974
- Z. Shen, Y. Liu, Z. Li, Z. Tang, J. Pu et al., Highly-entangled hydrogel electrolyte for fast charging/discharging properties in aqueous zinc ion batteries. Adv. Funct. Mater. 35(21), 2406620 (2025). https://doi.org/10.1002/adfm.202406620
- H.-W. Park, N.-G. Jang, H.-S. Seo, K. Kwon, S. Shin, Facile synthesis of self-adhesion and ion-conducting 2-acrylamido-2-methylpropane sulfonic acid/tannic acid hydrogels using electron beam irradiation. Polymers 15(18), 3836 (2023). https://doi.org/10.3390/polym15183836
- G.R. Bhimanapati, Z. Lin, V. Meunier, Y. Jung, J. Cha et al., Recent advances in two-dimensional materials beyond graphene. ACS Nano 9(12), 11509–11539 (2015). https://doi.org/10.1021/acsnano.5b05556
- H. Chen, X. Chen, C. Rong, X. Ma, B. Zhang et al., Layered structured MXene/PVA conductive hydrogels with excellent mechanical properties for flexible strain and temperature sensing. Small 21(39), e06824 (2025). https://doi.org/10.1002/smll.202506824
- Y. Zhao, K. Feng, Y. Yu, In situ preparation of zincophilic covalent-organic frameworks with low surface work function and high rigidity to stabilize zinc metal anodes. J. Energy Chem. 102, 524–533 (2025). https://doi.org/10.1016/j.jechem.2024.11.019
- D. Wang, F. Zhu, J. Luan, P. Xu, Y. Wei et al., Cooperative solvation-interface engineering via cell membrane-inspired hydrated nanodomains for high-mass-loading zinc-ion batteries. Adv. Funct. Mater. 36(27), e17438 (2026). https://doi.org/10.1002/adfm.202517438
- Q. Wang, B. Xu, Z. Jiang, M. Li, J. Zhang et al., Modulating zincophile property and solvation structure via molecular isomerism engineering for enhanced Zn anode stabilization. Adv. Funct. Mater. 36(28), e30054 (2026). https://doi.org/10.1002/adfm.202530054
- H. Peng, D. Wang, X. Wang, W. Miao, J. Zeng et al., Coupling solvation structure regulation and interface engineering via reverse micelle strategy toward highly stable Zn metal anode. Adv. Funct. Mater. 35(12), 2417695 (2025). https://doi.org/10.1002/adfm.202417695
- W. Hu, Y. Zhang, J. Ju, Y. Wang, Z. Zhang et al., Nanofiber-reinforced composite gel enabling high ionic conductivity and ultralong cycle life for Zn ion batteries. Small 20(5), e2305140 (2024). https://doi.org/10.1002/smll.202305140
- W. Chen, X. Li, Z. Du, Z. Ma, Y. Zuo et al., Revealing the alkali ions effects in potential shift and Zn dendrites suppression via electrolyte concentration regulation in aqueous zinc ion batteries. Chem. Eng. J. 493, 152647 (2024). https://doi.org/10.1016/j.cej.2024.152647
- R. Han, Y. Meng, X. Zhao, Y. Wang, M. Tang et al., Polyphosphonitrile derivative-based gel electrolytes for all-climate zinc metal batteries operating from -70 °C to +80 °C, Energy Environ. Sci. 18(11), 5482–5491 (2025). https://doi.org/10.1039/D5EE01478F
- H. Li, W. Li, P. Zhou, X. Chen, B. Shang et al., Overpotential engineering enables dendrite-free zinc anode for high-performance zinc-ion batteries. J. Colloid Interface Sci. 681, 159–168 (2025). https://doi.org/10.1016/j.jcis.2024.11.182
- Z. Hu, Z. Han, H. Liu, X. Jiang, K. Bai et al., Mechanically strong and tough ionic liquid gel electrolyte for four-electron zinc-iodine batteries. J. Am. Chem. Soc. 147(50), 46632–46641 (2025). https://doi.org/10.1021/jacs.5c18431
- Y. Wang, W. Yan, X. Zhu, J. Li, Z. Li et al., Boosting performance of quasi-solid-state zinc ion batteries via zincophilic solubilization. Angew. Chem. Int. Ed. 64(35), e202508556 (2025). https://doi.org/10.1002/anie.202508556
- S. Lee, I.K. Han, N.G. Jeon, Y. Lee, H.B. Son et al., Promoting homogeneous zinc-ion transfer through preferential ion coordination effect in gel electrolyte for stable zinc metal batteries. Adv. Sci. 10(34), 2304915 (2023). https://doi.org/10.1002/advs.202304915
- C. Wang, Z. Gong, J.A. Yuwono, Q. Meng, Y. Lyu et al., Ligand-channel-induced ion liberation in crowded zwitterionic hydrogel electrolyte for efficient zinc metal batteries. Nat. Commun. 16, 11069 (2025). https://doi.org/10.1038/s41467-025-66041-y
- G. Liu, S. Zhang, R. Wang, H. Zeng, R. Liu et al., Inhibiting proton corrosion and hydrogen evolution reaction on the surface of zinc anodes by hierarchical structure hydrogel to realize long-life aqueous zinc metal batteries. Adv. Energy Mater. 16(1), e03823 (2026). https://doi.org/10.1002/aenm.202503823
- Y. Lei, F. Liu, L. Chen, M. Xu, Y. Hu et al., Polyanionic hydrogel electrolytes to regulate ion transport behavior in long cycle life zinc-ion batteries. Nano Energy 143, 111284 (2025). https://doi.org/10.1016/j.nanoen.2025.111284
- W. Zhang, F. Guo, H. Mi, Z.-S. Wu, C. Ji et al., Kinetics-boosted effect enabled by zwitterionic hydrogel electrolyte for highly reversible zinc anode in zinc-ion hybrid micro-supercapacitors. Adv. Energy Mater. 12(40), 2202219 (2022). https://doi.org/10.1002/aenm.202202219
- S. Zhang, H. Ao, J. Dong, D. Wang, C. Wang et al., Dipole moment dictates the preferential immobilization in gel electrolytes for ah-level aqueous zinc-metal batteries. Angew. Chem. Int. Ed. Engl. 64(2), e202414702 (2025). https://doi.org/10.1002/anie.202414702
- Y. Xiong, H. Cheng, Y. Jiang, Z. Fan, X. Li et al., A novel water-reducer-based hydrogel electrolyte for robust and flexible Zn-I2 battery. Energy Storage Mater. 74, 103981 (2025). https://doi.org/10.1016/j.ensm.2024.103981
- Z. Wang, R. Xue, H. Zhang, Y. Zhang, X. Tang et al., A hydrogel electrolyte toward a flexible zinc-ion battery and multifunctional health monitoring electronics. ACS Nano 18(10), 7596–7609 (2024). https://doi.org/10.1021/acsnano.4c00085
- X. Bai, Y. Nan, K. Yang, B. Deng, J. Shao et al., Zn ionophores to suppress hydrogen evolution and promote uniform Zn deposition in aqueous Zn batteries. Adv. Funct. Mater. 33(42), 2307595 (2023). https://doi.org/10.1002/adfm.202307595
- X. Liu, Y. Guo, F. Ning, Y. Liu, S. Shi et al., Fundamental understanding of hydrogen evolution reaction on zinc anode surface: a first-principles study. Nano-Micro Lett. 16(1), 111 (2024). https://doi.org/10.1007/s40820-024-01337-0
- G. Ma, W. Yuan, X. Li, T. Bi, L. Niu et al., Organic cations texture zinc metal anodes for deep cycling aqueous zinc batteries. Adv. Mater. 36(35), 2408287 (2024). https://doi.org/10.1002/adma.202408287
- F. Tao, Y. Ren, L.-E. Mo, Y. Wang, Y. Huang et al., Exposing Zn(002) texture with sucralose additive for stable and dendrite-free aqueous zinc-ion batteries. Nano-Micro Lett. 18(1), 107 (2026). https://doi.org/10.1007/s40820-025-01954-3
- D. Kundu, B.D. Adams, V. Duffort, S.H. Vajargah, L.F. Nazar, A high-capacity and long-life aqueous rechargeable zinc battery using a metal oxide intercalation cathode. Nat. Energy 1, 16119 (2016). https://doi.org/10.1038/nenergy.2016.119
- Z. Xie, Y. Qu, F. Kong, R. Zhao, X. Wang, Stable vacancy-rich sodium vanadate as a cathode for high-performance aqueous zinc-ion batteries. Nanomaterials 15(12), 940 (2025). https://doi.org/10.3390/nano15120940
- L. Hu, P.L. Chee, S. Sugiarto, Y. Yu, C. Shi et al., Hydrogel-based flexible electronics. Adv. Mater. 35(14), 2205326 (2023). https://doi.org/10.1002/adma.202205326
- W. Wang, H. Zhou, Z. Xu, Z. Li, L. Zhang et al., Flexible conformally bioadhesive MXene hydrogel electronics for machine learning-facilitated human-interactive sensing. Adv. Mater. 36(31), 2401035 (2024). https://doi.org/10.1002/adma.202401035
References
X. Wu, Y. Chen, B. Tang, Q. Yan, D. Wu et al., CeOx-integrated dual site enhanced urea electrosynthesis from nitrate and carbon dioxide. Nat. Commun. 16(1), 8785 (2025). https://doi.org/10.1038/s41467-025-63839-8
L.-L. Zhao, J.-Y. Wang, Y.-M. Wu, P.-F. Wang, Z.-L. Liu et al., Unlocking the multidimensional application and optimization mechanism of MOFs materials in aqueous zinc ion batteries. J. Energy Chem. 111, 249–273 (2025). https://doi.org/10.1016/j.jechem.2025.07.063
Y. Yang, S. Bremner, C. Menictas, M. Kay, Modelling and optimal energy management for battery energy storage systems in renewable energy systems: a review. Renew. Sustain. Energy Rev. 167c, 112671 (2022). https://doi.org/10.1016/j.rser.2022.112671
Z. Zhang, Y. Mu, L. Xiao, H. Hu, T. Xue et al., Hydrogel electrolytes for zinc-ion batteries: materials design, functional strategies, and future perspectives. Nano-Micro Lett. 18(1), 139 (2026). https://doi.org/10.1007/s40820-025-01993-w
Y. Zhu, G. Liang, X. Cui, X. Liu, H. Zhong et al., Engineering hosts for Zn anodes in aqueous Zn-ion batteries. Energy Environ. Sci. 17(2), 369–385 (2024). https://doi.org/10.1039/D3EE03584K
R. Wang, W. Chen, C. Zhang, R. Zhao, X. Wang, Electrochemically active Mn2+ enabling high-performance aqueous zinc ion batteries. Energy Fuels 38(14), 13436–13443 (2024). https://doi.org/10.1021/acs.energyfuels.4c02624
D. Wu, H. Wang, Y. Nie, H. Wan, S. Liu et al., When covalent organic frameworks meet metals: from opportunities toward applications. Prog. Mater. Sci. 155, 101538 (2026). https://doi.org/10.1016/j.pmatsci.2025.101538
J. Zhu, X. Ge, Z. Peng, L. Pan, Z. Peng et al., Interfacial regulation for zinc metal anode of aqueous zinc-ion battery. Green Energy Environ. 10(4), 689–708 (2025). https://doi.org/10.1016/j.gee.2024.11.001
H. Yan, S. Li, J. Zhong, B. Li, An electrochemical perspective of aqueous zinc metal anode. Nano-Micro Lett. 16(1), 15 (2023). https://doi.org/10.1007/s40820-023-01227-x
G. Zhang, Y. Chen, L. Fu, L. Zheng, K. Fan et al., Regulating the solvation sheath of zinc ions by supramolecular coordination chemistry toward ultrastable zinc anodes. SmartMat 5(3), e1216 (2024). https://doi.org/10.1002/smm2.1216
X. Lu, L. Chen, W. Li, X. Zhang, W. Chi et al., Accelerating desolvation and constructing dual-storage channels for Zn2+ by ligand field engineering of polar organic molecules for high-performance zinc-ion batteries. Adv. Funct. Mater. 36(2), e13457 (2026). https://doi.org/10.1002/adfm.202513457
W. Chen, Z. Xie, H. Chen, X. Wang, Low-cost aqueous electrolyte with MBA additives for uniform and stable zinc deposition. ACS Appl. Mater. Interfaces 16(23), 30580–30588 (2024). https://doi.org/10.1021/acsami.4c05430
Y. Lv, C. Huang, M. Zhao, M. Fang, Q. Dong et al., Synergistic anion–cation chemistry enables highly stable Zn metal anodes. J. Am. Chem. Soc. 147(10), 8523–8533 (2025). https://doi.org/10.1021/jacs.4c16932
J. Zhang, Z. Liu, M. Li, Y. Shi, H. Li et al., Synchronized regulating Zn2+ depositing/stripping processes to achieve ultra-stable aqueous zinc metal batteries. Energy Storage Mater. 81, 104451 (2025). https://doi.org/10.1016/j.ensm.2025.104451
Z. Yan, F. Luo, S. Yang, Q. Wu, J. Zhang et al., Polydentate ligand-induced surface reconstruction of MIL-88A reinforced gel electrolytes for highly reversible zinc batteries via ion rectification and charge redistribution. Adv. Funct. Mater. 36(3), e14679 (2026). https://doi.org/10.1002/adfm.202514679
Y. Yang, Q. He, C. Hu, X. Xie, S. Liang et al., Electron-initiated self-growth in situ hydrogel electrolyte with gradient protection interface enables stable zinc metal batteries. ACS Nano 19(23), 21717–21728 (2025). https://doi.org/10.1021/acsnano.5c04942
R. Li, L. Zhang, X. Wang, F. Wu, L. Li et al., A stretchable and self-healing polymer-in-salt all-solid electrolyte for wearable zinc-ion batteries. Nano Res. 18(8), 94907536 (2025). https://doi.org/10.26599/nr.2025.94907536
X. Hui, Z. Zhan, Z. Zhang, J. Yu, P. Jiang et al., Missing-linker defect functionalized metal-organic frameworks accelerating zinc ion conduction for ultrastable all-solid-state zinc metal batteries. ACS Nano 18(36), 25237–25248 (2024). https://doi.org/10.1021/acsnano.4c07907
Y. Yang, C. Huang, H. Li, Z. Teng, H. Zhang et al., Study of a novel supramolecular hydrogel electrolyte for aqueous zinc ion batteries. J. Mater. Chem. C 11(28), 9559–9569 (2023). https://doi.org/10.1039/d3tc01284k
D. Li, L. Cao, T. Deng, S. Liu, C. Wang, Design of a solid electrolyte interphase for aqueous Zn batteries. Angew. Chem. Int. Ed. 60(23), 13035–13041 (2021). https://doi.org/10.1002/anie.202103390
D. Wang, D. Zhao, L. Chang, Y. Zhang, W. Wang et al., Interface engineering of electron-ion dual transmission channels for ultra-long lifespan quasi-solid zinc-ion batteries. Energy Storage Mater. 74, 103903 (2025). https://doi.org/10.1016/j.ensm.2024.103903
H. Xia, W. Zhang, C. Miao, H. Chen, C. Yi et al., Ultra-thin amphiphilic hydrogel electrolyte for flexible zinc-ion paper batteries. Energy Environ. Sci. 17(18), 6507–6520 (2024). https://doi.org/10.1039/D4EE01993H
W. Zeng, S. Zhang, J. Lan, Y. Lv, G. Zhu et al., Double network gel electrolyte with high ionic conductivity and mechanical strength for Zinc-ion batteries. ACS Nano 18(38), 26391–26400 (2024). https://doi.org/10.1021/acsnano.4c09879
Y. Mao, H. Ren, J. Zhang, T. Luo, N. Liu et al., Modifying hydrogel electrolyte to induce Zinc deposition for dendrite-free Zinc metal anode. Electrochim. Acta 393, 139094 (2021). https://doi.org/10.1016/j.electacta.2021.139094
P. Xu, Q. Zhang, X. Chen, J. Liu, N. Zhao et al., Multifunctional double-network hydrogel with enhanced interface engineering for high-performance flexible Zinc-air batteries. Chem. Eng. J. 522, 167206 (2025). https://doi.org/10.1016/j.cej.2025.167206
Y. An, C. Shu, Y. Liu, Y. Xu, L. Kang et al., Modulating the hydrogen bond for a stable Zinc anode with a wide temperature range via the sucrose and polyacrylamide synergistic effect. ACS Nano 19(11), 11146–11163 (2025). https://doi.org/10.1021/acsnano.4c18178
Q. He, Y. Zhong, J. Li, S. Chai, Y. Yang et al., Constructing kosmotropic salt-compatible PVA hydrogels for stable Zinc anodes via strong hydrogen bonds preshielding effect. Adv. Energy Mater. 14(23), 2400170 (2024). https://doi.org/10.1002/aenm.202400170
C. Yang, P. Woottapanit, S. Geng, R. Chanajaree, Y. Shen et al., A multifunctional quasi-solid-state polymer electrolyte with highly selective ion highways for practical Zinc ion batteries. Nat. Commun. 16, 183 (2025). https://doi.org/10.1038/s41467-024-55656-2
M. Sun, G. Ji, M. Li, J. Zheng, A robust hydrogel electrolyte with ultrahigh ion transference number derived from Zincophilic “chain-gear” network structure for dendrite-free aqueous Zinc ion battery. Adv. Funct. Mater. 34(37), 2402004 (2024). https://doi.org/10.1002/adfm.202402004
J. Wang, X. Zou, L. Song, Y. Hou, J. Lu et al., A bio-inspired multifunctional interface layer for high performance Zinc-ion batteries via novel in situ electropolymerization. J. Mater. Chem. A 11(44), 23973–23983 (2023). https://doi.org/10.1039/D3TA04886A
S. Yang, Q. Wu, Y. Li, F. Luo, J. Zhang et al., A bio-inspired multifunctional hydrogel network with toughly interfacial chemistry for dendrite-free flexible Zinc ion battery. Angew. Chem. Int. Ed. 63(44), e202409160 (2024). https://doi.org/10.1002/anie.202409160
Q. Wang, J. Huang, L. Qi, M. Li, S. Wang et al., A bioinspired gradient hydrogel electrolyte network with optimized interfacial chemistry toward robust aqueous Zinc-ion batteries. ACS Nano 19(29), 26770–26781 (2025). https://doi.org/10.1021/acsnano.5c06914
Y. Guo, Z. Chang, B. Li, Z.-L. Zhao, H.-P. Zhao et al., Functional gradient effects on the energy absorption of spider orb webs. Appl. Phys. Lett. 113(10), 103701 (2018). https://doi.org/10.1063/1.5039710
Y. Liu, G. Tian, Y. Du, P. Shi, N. Li et al., Highly stretchable, low-hysteresis, and adhesive TA@MXene-composited organohydrogels for durable wearable sensors. Adv. Funct. Mater. 34(30), 2315813 (2024). https://doi.org/10.1002/adfm.202315813
Y. Du, Y. Chen, M. Yang, S. Zou, X. Song et al., Poly(3, 4-ethylenedioxythiophene)–polystyrenesulfonate-added layered vanadium oxide cathode for high-performance zinc-ion batteries. ACS Appl. Energy Mater. 4(12), 14582–14589 (2021). https://doi.org/10.1021/acsaem.1c03209
Q. Ma, A. Ma, S. Lv, B. Qin, Y. Xu et al., Regulating zinc ion transport behavior and solvated structure towards stable aqueous Zn metal batteries. J. Energy Chem. 93, 609–626 (2024). https://doi.org/10.1016/j.jechem.2024.02.016
Y. Zhuang, Y. Liang, W. Zhang, Y. Sun, Z. Wang et al., Rational electrolyte structure engineering for highly reversible zinc metal anode in aqueous batteries. Nano-Micro Lett. 18(1), 102 (2026). https://doi.org/10.1007/s40820-025-01950-7
X. Wu, Q. Yan, H. Wang, D. Wu, H. Zhou et al., Heterostructured catalytic materials as advanced electrocatalysts: classification, synthesis, characterization, and application. Adv. Funct. Mater. 34(42), 2404535 (2024). https://doi.org/10.1002/adfm.202404535
J. Li, H. Zhang, Z. Liu, H. Du, H. Wan et al., Boosting dendrite-free zinc anode with strongly polar functional group terminated hydrogel electrolyte for high-safe aqueous zinc-ion batteries. Adv. Funct. Mater. 35(2), 2412865 (2025). https://doi.org/10.1002/adfm.202412865
J. Cui, J. Wu, A. Feng, Y. Yu, L. Mi et al., Low infrared emissivity and oxidation stability of Ti3C2Tx MXene-based composite with tannic acid. Chem. Eng. J. 493, 152289 (2024). https://doi.org/10.1016/j.cej.2024.152289
R.A. Soomro, P. Zhang, B. Fan, Y. Wei, B. Xu, Progression in the oxidation stability of MXenes. Nano-Micro Lett. 15(1), 108 (2023). https://doi.org/10.1007/s40820-023-01069-7
W. Liu, S. Kang, Q. Zhang, S. Chen, Q. Yang et al., Self-assembly fabrication of chitosan-tannic acid/MXene composite film with excellent antibacterial and antioxidant properties for fruit preservation. Food Chem. 410, 135405 (2023). https://doi.org/10.1016/j.foodchem.2023.135405
P. Zheng, X. Zhang, M. Yan, Y. Ma, Y. Jiang et al., The eruption of carbon chains in the oxidation of 2D Tin+1Cn (n = 1, 2, 3) MXenes. Appl. Surf. Sci. 550, 149310 (2021). https://doi.org/10.1016/j.apsusc.2021.149310
M. Lai, C. Zhao, D. Wang, R. Gao, P. Cai et al., Significantly enhanced oxidation resistance and electrochemical performance of hydrothermal Ti3C2Tx MXene and tannic acid composite for high-performance flexible supercapacitors. ACS Appl. Mater. Interfaces 16(41), 55555–55568 (2024). https://doi.org/10.1021/acsami.4c13838
Y. Zhang, L. Li, Y. Cao, Y. Yang, W. Wang et al., High-strength, low infrared-emission nonmetallic films for highly efficient Joule/solar heating, electromagnetic interference shielding and thermal camouflage. Mater. Horiz. 10(1), 235–247 (2023). https://doi.org/10.1039/D2MH01073A
X. Li, Y. Li, R. Wang, D. Wang, F. Ran, Ion confinement effect enabled by carboxymethyl cellulose/tannic acid hybrid hydrogel electrolyte toward stable zinc anode. Chem. Eng. J. 496, 153865 (2024). https://doi.org/10.1016/j.cej.2024.153865
L. Liu, C. Ge, Y. Zhang, W. Ma, X. Su et al., Tannic acid-modified silver nanops for enhancing anti-biofilm activities and modulating biofilm formation. Biomater. Sci. 8(17), 4852–4860 (2020). https://doi.org/10.1039/d0bm00648c
H. Dou, X. Wu, M. Xu, R. Feng, Q. Ma et al., Steric-hindrance effect tuned ion solvation enabling high performance aqueous zinc ion batteries. Angew. Chem. Int. Ed. 63(21), e202401974 (2024). https://doi.org/10.1002/anie.202401974
Z. Shen, Y. Liu, Z. Li, Z. Tang, J. Pu et al., Highly-entangled hydrogel electrolyte for fast charging/discharging properties in aqueous zinc ion batteries. Adv. Funct. Mater. 35(21), 2406620 (2025). https://doi.org/10.1002/adfm.202406620
H.-W. Park, N.-G. Jang, H.-S. Seo, K. Kwon, S. Shin, Facile synthesis of self-adhesion and ion-conducting 2-acrylamido-2-methylpropane sulfonic acid/tannic acid hydrogels using electron beam irradiation. Polymers 15(18), 3836 (2023). https://doi.org/10.3390/polym15183836
G.R. Bhimanapati, Z. Lin, V. Meunier, Y. Jung, J. Cha et al., Recent advances in two-dimensional materials beyond graphene. ACS Nano 9(12), 11509–11539 (2015). https://doi.org/10.1021/acsnano.5b05556
H. Chen, X. Chen, C. Rong, X. Ma, B. Zhang et al., Layered structured MXene/PVA conductive hydrogels with excellent mechanical properties for flexible strain and temperature sensing. Small 21(39), e06824 (2025). https://doi.org/10.1002/smll.202506824
Y. Zhao, K. Feng, Y. Yu, In situ preparation of zincophilic covalent-organic frameworks with low surface work function and high rigidity to stabilize zinc metal anodes. J. Energy Chem. 102, 524–533 (2025). https://doi.org/10.1016/j.jechem.2024.11.019
D. Wang, F. Zhu, J. Luan, P. Xu, Y. Wei et al., Cooperative solvation-interface engineering via cell membrane-inspired hydrated nanodomains for high-mass-loading zinc-ion batteries. Adv. Funct. Mater. 36(27), e17438 (2026). https://doi.org/10.1002/adfm.202517438
Q. Wang, B. Xu, Z. Jiang, M. Li, J. Zhang et al., Modulating zincophile property and solvation structure via molecular isomerism engineering for enhanced Zn anode stabilization. Adv. Funct. Mater. 36(28), e30054 (2026). https://doi.org/10.1002/adfm.202530054
H. Peng, D. Wang, X. Wang, W. Miao, J. Zeng et al., Coupling solvation structure regulation and interface engineering via reverse micelle strategy toward highly stable Zn metal anode. Adv. Funct. Mater. 35(12), 2417695 (2025). https://doi.org/10.1002/adfm.202417695
W. Hu, Y. Zhang, J. Ju, Y. Wang, Z. Zhang et al., Nanofiber-reinforced composite gel enabling high ionic conductivity and ultralong cycle life for Zn ion batteries. Small 20(5), e2305140 (2024). https://doi.org/10.1002/smll.202305140
W. Chen, X. Li, Z. Du, Z. Ma, Y. Zuo et al., Revealing the alkali ions effects in potential shift and Zn dendrites suppression via electrolyte concentration regulation in aqueous zinc ion batteries. Chem. Eng. J. 493, 152647 (2024). https://doi.org/10.1016/j.cej.2024.152647
R. Han, Y. Meng, X. Zhao, Y. Wang, M. Tang et al., Polyphosphonitrile derivative-based gel electrolytes for all-climate zinc metal batteries operating from -70 °C to +80 °C, Energy Environ. Sci. 18(11), 5482–5491 (2025). https://doi.org/10.1039/D5EE01478F
H. Li, W. Li, P. Zhou, X. Chen, B. Shang et al., Overpotential engineering enables dendrite-free zinc anode for high-performance zinc-ion batteries. J. Colloid Interface Sci. 681, 159–168 (2025). https://doi.org/10.1016/j.jcis.2024.11.182
Z. Hu, Z. Han, H. Liu, X. Jiang, K. Bai et al., Mechanically strong and tough ionic liquid gel electrolyte for four-electron zinc-iodine batteries. J. Am. Chem. Soc. 147(50), 46632–46641 (2025). https://doi.org/10.1021/jacs.5c18431
Y. Wang, W. Yan, X. Zhu, J. Li, Z. Li et al., Boosting performance of quasi-solid-state zinc ion batteries via zincophilic solubilization. Angew. Chem. Int. Ed. 64(35), e202508556 (2025). https://doi.org/10.1002/anie.202508556
S. Lee, I.K. Han, N.G. Jeon, Y. Lee, H.B. Son et al., Promoting homogeneous zinc-ion transfer through preferential ion coordination effect in gel electrolyte for stable zinc metal batteries. Adv. Sci. 10(34), 2304915 (2023). https://doi.org/10.1002/advs.202304915
C. Wang, Z. Gong, J.A. Yuwono, Q. Meng, Y. Lyu et al., Ligand-channel-induced ion liberation in crowded zwitterionic hydrogel electrolyte for efficient zinc metal batteries. Nat. Commun. 16, 11069 (2025). https://doi.org/10.1038/s41467-025-66041-y
G. Liu, S. Zhang, R. Wang, H. Zeng, R. Liu et al., Inhibiting proton corrosion and hydrogen evolution reaction on the surface of zinc anodes by hierarchical structure hydrogel to realize long-life aqueous zinc metal batteries. Adv. Energy Mater. 16(1), e03823 (2026). https://doi.org/10.1002/aenm.202503823
Y. Lei, F. Liu, L. Chen, M. Xu, Y. Hu et al., Polyanionic hydrogel electrolytes to regulate ion transport behavior in long cycle life zinc-ion batteries. Nano Energy 143, 111284 (2025). https://doi.org/10.1016/j.nanoen.2025.111284
W. Zhang, F. Guo, H. Mi, Z.-S. Wu, C. Ji et al., Kinetics-boosted effect enabled by zwitterionic hydrogel electrolyte for highly reversible zinc anode in zinc-ion hybrid micro-supercapacitors. Adv. Energy Mater. 12(40), 2202219 (2022). https://doi.org/10.1002/aenm.202202219
S. Zhang, H. Ao, J. Dong, D. Wang, C. Wang et al., Dipole moment dictates the preferential immobilization in gel electrolytes for ah-level aqueous zinc-metal batteries. Angew. Chem. Int. Ed. Engl. 64(2), e202414702 (2025). https://doi.org/10.1002/anie.202414702
Y. Xiong, H. Cheng, Y. Jiang, Z. Fan, X. Li et al., A novel water-reducer-based hydrogel electrolyte for robust and flexible Zn-I2 battery. Energy Storage Mater. 74, 103981 (2025). https://doi.org/10.1016/j.ensm.2024.103981
Z. Wang, R. Xue, H. Zhang, Y. Zhang, X. Tang et al., A hydrogel electrolyte toward a flexible zinc-ion battery and multifunctional health monitoring electronics. ACS Nano 18(10), 7596–7609 (2024). https://doi.org/10.1021/acsnano.4c00085
X. Bai, Y. Nan, K. Yang, B. Deng, J. Shao et al., Zn ionophores to suppress hydrogen evolution and promote uniform Zn deposition in aqueous Zn batteries. Adv. Funct. Mater. 33(42), 2307595 (2023). https://doi.org/10.1002/adfm.202307595
X. Liu, Y. Guo, F. Ning, Y. Liu, S. Shi et al., Fundamental understanding of hydrogen evolution reaction on zinc anode surface: a first-principles study. Nano-Micro Lett. 16(1), 111 (2024). https://doi.org/10.1007/s40820-024-01337-0
G. Ma, W. Yuan, X. Li, T. Bi, L. Niu et al., Organic cations texture zinc metal anodes for deep cycling aqueous zinc batteries. Adv. Mater. 36(35), 2408287 (2024). https://doi.org/10.1002/adma.202408287
F. Tao, Y. Ren, L.-E. Mo, Y. Wang, Y. Huang et al., Exposing Zn(002) texture with sucralose additive for stable and dendrite-free aqueous zinc-ion batteries. Nano-Micro Lett. 18(1), 107 (2026). https://doi.org/10.1007/s40820-025-01954-3
D. Kundu, B.D. Adams, V. Duffort, S.H. Vajargah, L.F. Nazar, A high-capacity and long-life aqueous rechargeable zinc battery using a metal oxide intercalation cathode. Nat. Energy 1, 16119 (2016). https://doi.org/10.1038/nenergy.2016.119
Z. Xie, Y. Qu, F. Kong, R. Zhao, X. Wang, Stable vacancy-rich sodium vanadate as a cathode for high-performance aqueous zinc-ion batteries. Nanomaterials 15(12), 940 (2025). https://doi.org/10.3390/nano15120940
L. Hu, P.L. Chee, S. Sugiarto, Y. Yu, C. Shi et al., Hydrogel-based flexible electronics. Adv. Mater. 35(14), 2205326 (2023). https://doi.org/10.1002/adma.202205326
W. Wang, H. Zhou, Z. Xu, Z. Li, L. Zhang et al., Flexible conformally bioadhesive MXene hydrogel electronics for machine learning-facilitated human-interactive sensing. Adv. Mater. 36(31), 2401035 (2024). https://doi.org/10.1002/adma.202401035