Abstract
Hydrogel electrolyte based secondary batteries are promising for wearable electronics, yet face challenges including limited mechanical resilience, and narrow temperature range. Herein, we report a robust deep-eutectic hydrogel electrolyte fabricated via synergistic interplay of dual nanophase separation, hydrated eutectic solvation, and hydrogen-bond networks. The interwoven nanophase separation architecture, integrating hydrophilic polyvinyl alcohol phases and hydrophobic polyacrylonitrile phases, realizes high fracture-strength (4.1 MPa) and toughness (13.66 MJ m−3). Meanwhile, deep-eutectic chemistry modulates Zn2+ solvation structures and leverages cyano-coordination channels of polyacrylonitrile to achieve high Zn2+ ionic conductivity (28.2 mS cm−1) and transference number (0.65) at 20 °C. Concurrently, abundant hydrogen bonds induced by multiple donor sites of hydrophilic phases, urethane, and Zn(ClO4)2 immobilize active H2O to ensure broad-temperature durability. This tripartite synergy directs planar Zn deposition along (002) planes and suppresses dendrite growth, enabling Zn||I2 batteries with a thinner-than-paper thickness (42 μm) and high flexibility. The assembled Zn||I2 batteries demonstrate high specific energy (108.99 Wh kg−1) and cycling stability (over 36,000 cycles under −40 to 80 °C). In this work, the convergence of molecule design, phase modulation, and process engineering establishes a feasible methodological framework for developing advanced flexible batteries that integrate high energy density and harsh environment tolerance.
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References
Lu, H. et al. A recyclable biomass electrolyte towards green zinc-ion batteries. Nat. Commun. 14, 4435 (2023).
Yang, C. et al. All-temperature zinc batteries with high-entropy aqueous electrolyte. Nat. Sustain. 6, 325–335 (2023).
Chen, W. et al. A manganese-hydrogen battery with potential for grid-scale energy storage. Nat. Energy 3, 428–435 (2018).
Niu, B. et al. Polymers for aqueous zinc-ion batteries: from fundamental to applications across core components. Adv. Energy Mater. 14, 2303967 (2024).
Qi, R. et al. Gel polymer electrolyte toward large-scale application of aqueous zinc batteries. Adv. Funct. Mater. 33, 2306052 (2023).
Yang, P. et al. Ionic selective separator design enables long-life zinc-iodine batteries via synergistic anode stabilization and polyiodide shuttle suppression. Adv. Funct. Mater. 34, 2410712 (2024).
Xiao, X. et al. Rational design of flexible Zn-based batteries for wearable electronic devices. ACS Nano 17, 1764–1802 (2023).
Wu, M. et al. Aqueous Zn-based rechargeable batteries: recent progress and future perspectives. InfoMat 4, e12265 (2021).
Lyu, Z. et al. Design and manufacture of 3D-printed batteries. Joule 5, 89–114 (2021).
Wang, Y. et al. Lean-water hydrogel electrolyte for zinc ion batteries. Nat. Commun. 14, 3890 (2023).
Luo, F. et al. Hydrogel electrolytes with an electron/ion dual regulation mechanism for highly reversible flexible zinc batteries. Energy Environ. Sci. 17, 8570–8581 (2024).
Feng, D., Jiao, Y. & Wu, P. Guiding Zn uniform deposition with polymer additives for long-lasting and highly utilized Zn metal anodes. Angew. Chem. Int. Ed. 62, e202314456 (2023).
Li, X., Wang, D. & Ran, F. Key approaches and challenges in fabricating advanced flexible zinc-ion batteries with functional hydrogel electrolytes. Energy Storage Mater. 56, 351–393 (2023).
Hong, Z., Ahmad, Z. & Viswanathan, V. Design principles for dendrite suppression with porous polymer/aqueous solution hybrid electrolyte for Zn metal anodes. ACS Energy Lett. 5, 2466–2474 (2020).
Li, C. et al. High-fluidity/high-strength dual-layer gel electrolytes enable ultra-flexible and dendrite-free fiber-shaped aqueous zinc metal battery. Adv. Mater. 36, 2313772 (2024).
Chen, Z. et al. Tough, anti-fatigue, self-adhesive, and anti-freezing hydrogel electrolytes for dendrite-free flexible zinc ion batteries and strain sensors. Adv. Funct. Mater. 34, 2314864 (2024).
Tang, C. et al. A new polyvinyl alcohol lithium chloride hydrogel electrolyte: high ionic conductivity and wide working temperature range. Adv. Funct. Mater. 35, 2417207 (2025).
Xia, H. et al. Single-ion-conducting hydrogel electrolytes based on slide-ring pseudo-polyrotaxane for ultralong-cycling flexible zinc-ion batteries. Adv. Mater. 35, 2301996 (2023).
Wang, X., Wang, B., Cheng, J. & Healable, M. MechanicAlly Durable Double Cross-linked Polyacrylamide Electrolyte Incorporating hydrophobic interactions for dendrite-free flexible zinc-ion batteries. Adv. Funct. Mater. 33, 2304470 (2023).
Zhang, J. et al. A hydrogel electrolyte with high adaptability over a wide temperature range and mechanical stress for long-life flexible zinc-ion batteries. Small 20, 2312116 (2024).
Shim, G., Tran, M. X., Liu, G., Byun, D. & Lee, J. K. Flexible, fiber-shaped, quasi-solid-state Zn-polyaniline batteries with methanesulfonic acid-doped aqueous gel electrolyte. Energy Storage Mater. 35, 739–749 (2021).
Xu, J. et al. Understanding the electrical mechanisms in aqueous zinc metal batteries: from electrostatic interactions to electric field regulation. Adv. Mater. 36, 2309726 (2024).
Yan, Y. et al. Tough hydrogel electrolytes for anti-freezing zinc-ion batteries. Adv. Mater. 35, 2211673 (2023).
Lu, H. et al. Multi-component crosslinked hydrogel electrolyte toward dendrite-free aqueous Zn ion batteries with high temperature adaptability. Adv. Funct. Mater. 32, 2112540 (2022).
Shao, Y. et al. Regulating interfacial ion migration via wool keratin mediated biogel electrolyte toward robust flexible Zn-ion batteries. Small 18, 2107163 (2022).
Chen, M. et al. Realizing an all-round hydrogel electrolyte toward environmentally adaptive dendrite-free aqueous Zn-MnO2 batteries. Adv. Mater. 33, 2007559 (2021).
Li, Q. et al. Dendrite issues for zinc anodes in a flexible cell configuration for zinc-based wearable energy-storage devices. Angew. Chem. Int. Ed. 61, e202202780 (2022).
Zhao, Z. et al. In-situ formed all-amorphous poly (ethylene oxide)-based electrolytes enabling solid-state Zn electrochemistry. Chem. Eng. J. 417, 128096 (2021).
Yang, P. et al. Thermal self-protection of zinc-ion batteries enabled by smart hygroscopic hydrogel electrolytes. Adv. Energy Mater. 10, 2002898 (2020).
Chen, Z. et al. An ultrahigh-modulus hydrogel electrolyte for dendrite-free zinc ion batteries. Adv. Mater. 36, 2413268 (2024).
Wu, Y. et al. Solvent-exchange-assisted wet annealing: a new strategy for superstrong, tough, stretchable, and anti-fatigue hydrogels. Adv. Mater. 35, 2210624 (2023).
Fu, R. et al. A tough and self-powered hydrogel for artificial skin. Chem. Mater. 31, 9850–9860 (2019).
Wan, H., Wu, B., Hou, L. & Wu, P. Amphibious polymer materials with high strength and superb toughness in various aquatic and atmospheric environments. Adv. Mater. 36, 2307290 (2024).
Cao, G. et al. “Salting out” in hofmeister effect enhancing mechanical and electrochemical performance of amide-based hydrogel electrolytes for flexible zinc-ion battery. Small 19, 2207610 (2023).
Liu, D. et al. Tough, transparent, and slippery PVA hydrogel led by syneresis. Small 19, 2206819 (2023).
Yang, X. et al. Reinforcing hydrogel by nonsolvent-quenching-facilitated in situ nanofibrosis. Adv. Mater. 35, 2303728 (2023).
Zhang, G. et al. Hofmeister effects in supramolecular chemistry for anion-modulation to stabilize Zn anode. Adv. Mater. 36, 2405949 (2024).
Tang, N. et al. Evolutionary reinforcement of polymer networks: a stepwise-enhanced strategy for ultrarobust eutectogels. Adv. Mater. 36, 2309576 (2024).
Yang, G. et al. An aqueous zinc-ion battery working at −50 °C enabled by low-concentration perchlorate-based chaotropic salt electrolyte. EcoMat 4, e12165 (2022).
Park, J. et al. Unraveling concentration-dependent solvation structures and molecular interactions in water-in-salt electrolytes for enhanced performance of electric double-layer capacitors. Energy Storage Mater. 65, 103137 (2024).
Malfait, B., Jani, A. & Morineau, D. Confining deep eutectic solvents in nanopores: insight into thermodynamics and chemical activity. J. Mol. Liq. 349, 118488 (2022).
Qiu, M. et al. Entropy-driven hydrated eutectic electrolytes with diverse solvation configurations for all-temperature Zn-ion batteries. Angew. Chem. Int. Ed. 63, e202407012 (2024).
Yao, L. et al. Ultra-stable Zn anode enabled by fiber-directed ion migration using mass-producible separator. Adv. Funct. Mater. 33, 2209301 (2022).
Li, Y. et al. A novel ultrathin multiple-kinetics-enhanced polymer electrolyte editing enabled wide-temperature fast-charging solid-state zinc metal batteries. Adv. Funct. Mater. 34, 2307736 (2023).
Zhao, X. et al. Designable polypyrrole pattern in hydrogel achieved by photo-controllable concentration of Fe3+ initiator. Smart Mol. 2, e20240015 (2024).
Xiao, X., Chen, Z., Varley, R. J. & Li, C. Smart bistable coordination complexes. Smart Mol. 2, e20230028 (2024).
Kumankuma-Sarpong, J. et al. Entanglement added to cross-linked chains enables tough gelatin-based hydrogel for Zn metal batteries. Adv. Mater. 36, 2403214 (2024).
Liu, Q., Li, J., Xing, D., Zhou, Y. & Yan, F. Ternary eutectic electrolyte for flexible wide-temperature zinc-ion batteries from −20 °C to 70 °C. Angew. Chem. Int. Ed. 64, e202414728 (2025).
Guo, S. et al. Anti-freezing hydrogel electrolyte with a regulated hydrogen bond network enables high-rate and long cycling zinc batteries. Energy Environ. Sci. 18, 418–429 (2025).
Huang, Y., Yang, Y., Peng, C., Li, Y. & Feng, W. High strength, strain, and resilience of gold nanoparticle reinforced eutectogels for multifunctional sensors. Adv. Sci. 12, 2416318 (2025).
Zheng, Y., Wu, D., Wang, T., Liu, Q. & Jia, D. Advanced eutectogel electrolyte for high-performance and wide-temperature flexible zinc-air batteries. Angew. Chem. Int. Ed. 64, e202418223 (2024).
Deng, Y. et al. Inhibition of side reactions and dendrite growth using a low-cost and non-flammable eutectic electrolyte for high-voltage and super-stable zinc hybrid batteries. J. Mater. Chem. A 11, 8368–8379 (2023).
Sun, Z. et al. Hyperstable eutectic core-spun fiber enabled wearable energy harvesting and personal thermal management fabric. Adv. Mater. 36, 2310102 (2023).
Zhai, J. et al. Ultrathin cellulosic gel electrolytes with a gradient hydropenic interface for stable, high-energy and flexible zinc batteries. Energy Environ. Sci. 18, 4241–4250 (2025).
Xia, H. et al. Ultra-thin amphiphilic hydrogel electrolyte for flexible zinc-ion paper batteries. Energy Environ. Sci. 17, 6507–6520 (2024).
Zhang, X. et al. Polyzwitterionic gel electrolyte: dual optimization of polyiodide shuttle suppression and anode stabilization in aqueous Zn-I2 batteries. Adv. Funct. Mater. 35, 2505132 (2025).
Tian, Y., Chen, S., Ding, S., Chen, Q. & Zhang, J. A highly conductive gel electrolyte with favorable ion transfer channels for long-lived zinc–iodine batteries. Chem. Sci. 14, 331–337 (2023).
Zhou, X. et al. Molecular bridging induced anti-salting-out effect enabling high ionic conductive ZnSO4-based hydrogel for quasi-solid-state zinc ion batteries. Angew. Chem. Int. Ed. 63, e202410434 (2024).
Aurbach, D., Gofer, Y. & Langzam, J. The correlation between surface chemistry, surface morphology, and cycling efficiency of lithium electrodes in a few polar aprotic systems. J. Electrochem. Soc. 136, 3198 (1989).
Chen, Y. et al. Coupling high hardness and Zn affinity in amorphous-crystalline diamond for stable Zn metal anodes. ACS Nano 18, 14403–14413 (2024).
Zhu, R. et al. High strength hydrogels enable dendrite-free Zn metal anodes and high-capacity Zn-MnO2 batteries via a modified mechanical suppression effect. J. Mater. Chem. A 10, 3122–3133 (2022).
Zheng, Z. et al. An extended substrate screening strategy enabling a low lattice mismatch for highly reversible zinc anodes. Nat. Commun. 15, 753 (2024).
Jiao, M. et al. A polarized gel electrolyte for wide-temperature flexible zinc-air batteries. Angew. Chem. Int. Ed. 62, e202301114 (2023).
Liu, Z. et al. Unraveling paradoxical effects of large current density on Zn deposition. Adv. Mater. 36, 2404140 (2024).
Hao, J. et al. Low-cost and non-flammable eutectic electrolytes for advanced Zn-I2 batteries. Angew. Chem. Int. Ed. 62, e202310284 (2023).
Sun, M., Ji, G., Li, M. & Zheng, J. 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, 2402004 (2024).
Zhu, K. et al. Molecular engineering enables hydrogel electrolyte with ionic hopping migration and self-healability toward dendrite-free zinc-metal anodes. Adv. Mater. 36, 2311082 (2024).
Li, Q. et al. Crystal orientation engineering of perfectly matched heterogeneous textured ZnSe for an enhanced interfacial kinetic Zn anode. ACS Nano 17, 23805–23813 (2023).
Liang, G. et al. Gradient fluorinated alloy to enable highly reversible Zn-metal anode chemistry. Energy Environ. Sci. 15, 1086–1096 (2022).
Ren, B. et al. Inhibiting dendrite formation and electrode corrosion via a scalable self-assembled mercaptan layer for stable aqueous zinc batteries. Adv. Energy Mater. 14, 2302970 (2024).
Wang, Y. et al. Manipulating electric double layer adsorption for stable solid-electrolyte interphase in 2.3 Ah Zn-pouch cells. Angew. Chem. Int. Ed. 62, e202302583 (2023).
Hu, N. et al. A double-charged organic molecule additive to customize electric double layer for super-stable and deep-rechargeable Zn metal pouch batteries. Adv. Funct. Mater. 34, 2311773 (2024).
Wang, Y. et al. Sulfolane-containing aqueous electrolyte solutions for producing efficient ampere-hour-level zinc metal battery pouch cells. Nat. Commun. 14, 1828 (2023).
Liang, G. et al. Regulating inorganic and organic components to build amorphous-ZnFx enriched solid-electrolyte interphase for highly reversible Zn metal chemistry. Adv. Mater. 35, 2210051 (2023).
Zhu, K. et al. An integrated Janus hydrogel with different hydrophilicities and gradient pore structures for high-performance zinc-ion batteries. Energy Environ. Sci. 17, 4126–4136 (2024).
Acknowledgements
The authors are grateful to the funding supported from the National Natural Science Foundation of China (U25A20628, 22561160129, 22479074, 22475096 from Z.J. and 22425106, 22271139 from C.H.L.), the Equipment Pre-Research and Ministry of Education Joint Fund (8091B02052407, Z.J.), the Fundamental Research Program Key Project of Jiangsu Province (BK20253008, Z.J.), the Natural Science Foundation of Jiangsu Province (BK20240400, BK20241236, Z.J.), the Science and Technology Major Project of Jiangsu Province (BG2024013, Z.J.), the Scientific and Technological Achievements Transformation Special Fund of Jiangsu Province (BA2023037, Z.J.), the Academic Degree and Postgraduate Education Reforming Project of Jiangsu Province (JGKT24_C001, Z.J.), the Key Core Technology Open Competition Project of Suzhou City (SYG2024122, Z.J.), the Open Research Fund of Suzhou Laboratory (SZLAB-1308-2024-TS005, Z.J.), the Chenzhou National Sustainable Development Agenda Innovation Demonstration Zone Provincial Special Project (2023sfq11, Z.J.), and the Fundamental Research Funds for the Central Universities (020514380294, C.H.L.).
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Z.J. conceived the idea of this study. T.Y.S. and Z.J.C. designed the experiments. T.Y.S., Z.J.C., J.Y.W., K.X.H., W.M., J.C.L., and H.G.L. performed sample preparations. T.Y.S., Z.J.C., Y.M.Y., and Z.X.T. performed electrochemical measurements, battery tests, and data analyses. T.Y.S. and Y.X.Y. performed the theoretical calculations. Z.J., C.H.L., T.Y.S., Z.J.C., and Q.C.Y. wrote the manuscript. Z.J. and C.H.L. supervised the project. All authors participated in the scientific discussion of this project.
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Shen, T., Chen, ZJ., Yang, Y. et al. Thinner-than-paper and broad-temperature-adaptive zinc-iodine batteries enabled by nanophase separated deep-eutectic hydrogel electrolytes. Nat Commun (2026). https://doi.org/10.1038/s41467-026-71312-3
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DOI: https://doi.org/10.1038/s41467-026-71312-3
