Insights on electrolyte engineering toward aqueous zinc-ion batteries

Abstract

The pursuit of safety and efficiency in electrochemical energy storage and conversion systems has long been a central theme. Among these systems, aqueous zinc-ion batteries (AZIBs) are considered promising candidates for next-generation energy storage devices due to their high safety, low cost, and high capacity. However, several critical issues associated with Zn²⁺ ion transport, including dendrite formation and side reactions at zinc (Zn) metal anodes, severely restricted their practical applications. As the “blood” of AZIBs, electrolytes play a crucial role in stabilizing Zn metal anodes by introducing various components or optimizing the liquid environment. Therefore, a comprehensive understanding of electrolyte engineering for AZIBs is of great significance. In this review, the development of electrolytes is first discussed. Then, the roles of electrolytes in AZIBs are summarized based on recent advances, including regulation of the solvation process, optimization of the solid electrolyte interphase layer, and modulation of ionic transport. Finally, perspectives on the further development of electrolytes for AZIBs are provided. This review may offer valuable insights for the design of functional electrolytes for advanced electrochemical energy storage and conversion systems.

Keywords

Aqueous zinc-ion batteries / zinc dendrites / Zn²⁺ ion transport / electrolytes / solvation process

References

[1] Chu S.Opportunities and challenges for a sustainable energy future.Nature2012;488:294-303

[2] Yao Z,Johnston A.Machine learning for a sustainable energy future.Nat Rev Mater2023;8:202-15 PMCID:PMC9579620

[3] Fuso Nerini F,To LS.Mapping synergies and trade-offs between energy and the sustainable development goals.Nat Energy2017;3:10-5

[4] Karijadi I,Dewabharata A.Wind power forecasting based on hybrid CEEMDAN-EWT deep learning method.Renew Energy2023;218:119357

[5] Naik N,Behera H.Wave power extraction by a dual OWC chambers over an undulated bottom.Renew Energy2023;216:119026

[6] Zhang H,Degrève J.Concentrated solar power plants: review and design methodology.Renew Sustain Energy Rev2013;22:466-81

[7] Sun J,He Y.The energy security risk assessment of inefficient wind and solar resources under carbon neutrality in China.Appl Energy2024;360:122889

[8] Ayodele T.Mitigation of wind power intermittency: storage technology approach.Renew Sustain Energy Rev2015;44:447-56

[9] Rahman F,Abdul-Majeed MA.Overview of energy storage systems for storing electricity from renewable energy sources in Saudi Arabia.Renew Sustain Energy Rev2012;16:274-83

[10] Kim T,Son D,Qi Y.Lithium-ion batteries: outlook on present, future, and hybridized technologies.J Mater Chem A2019;7:2942-64

[11] Scrosati B,Sun Y.Lithium-ion batteries. A look into the future.Energy Environ Sci2011;4:3287

[12] Fu K,Sun K.Thick electrode design for lithium-ion batteries from an ion-electron coupled transport perspective: from independent regulation to cooperative design.Energy Z2026;2:200002

[13] Janek J.A solid future for battery development.Nat Energy2016;1:16141

[14] Hao Z,Tang J.Functional separators towards the suppression of lithium dendrites for rechargeable high-energy batteries.Mater Horiz2021;8:12-32

[15] Ma L,Yao S.Dendrite-free lithium metal and sodium metal batteries.Energy Storage Mater2020;27:522-54

[16] Zhao Q,Luo Z.High-capacity aqueous zinc batteries using sustainable quinone electrodes.Sci Adv2018;4:eaao1761 PMCID:PMC5837429

[17] Shang Y,Chen N.A universal strategy for high-voltage aqueous batteries via lone pair electrons as the hydrogen bond-breaker.Energy Environ Sci2022;15:2653-63

[18] Nian Q,Liu S,Ren X.Issues and opportunities on low-temperature aqueous batteries.Chem Eng J2021;423:130253

[19] Li TC,Zhang J.Recent progress in aqueous zinc-ion batteries: a deep insight into zinc metal anodes.J Mater Chem A2021;9:6013-28

[20] Hao Z,Xu X.Strategies for addressing the challenges of aqueous zinc batteries enabled by functional separators.J Mater Chem A2023;11:11031-47

[21] Luo C,Xiao Y.Recent development in addressing challenges and implementing strategies for manganese dioxide cathodes in aqueous zinc ion batteries.Energy Mater2024;4:400036

[22] Xue R,Wang Z.Enhancing temperature adaptability of aqueous zinc batteries via antifreezing electrolyte and site-selective ZnSe-Ag interface layer design.ACS Nano2023;17:17359-71

[23] Cui F,Hu F.Deficiency and surface engineering boosting electronic and ionic kinetics in NH₄V₄O₁₀ for high-performance aqueous zinc-ion battery.Energy Storage Mater2022;44:197-205

[24] Hu Y,Li M,Liang S.Challenges and industrial considerations towards stable and high-energy-density aqueous zinc-ion batteries.Energy Environ Sci2024;17:8078-93

[25] Shin J,Park Y.Aqueous zinc ion batteries: focus on zinc metal anodes.Chem Sci2020;11:2028-44 PMCID:PMC7053421

[26] Wang K,Jin H.Multifunctional zinc silicate coating layer for high-performance aqueous zinc-ion batteries.Energy Mater2025;5:500012

[27] Hao Z,Cao S.Functional ion-sieving separators based on covalent organic frameworks toward stable aqueous energy storage and conversion.ACS Mater Lett2025;7:3634-41

[28] Shang Y.A path forward for the translational development of aqueous zinc-ion batteries.Joule2023;7:244-50

[29] Cao J,Li C.Achieving high current density, high areal capacity, and high DOD AZIBs by screening amino acids.J Mater Chem A2024;12:29869-85

[30] Wei J,Sun J.Advanced electrolytes for high-performance aqueous zinc-ion batteries.Chem Soc Rev2024;53:10335-69

[31] Higashi S,Lee JS,Cui Y.Avoiding short circuits from zinc metal dendrites in anode by backside-plating configuration.Nat Commun2016;7:11801 PMCID:PMC4897743

[32] Han D,Zhang S.A corrosion-resistant and dendrite-free zinc metal anode in aqueous systems.Small2020;16:e2001736

[33] Kao CC,Hao J,Zhang SJ.Achieving high energy density in aqueous zinc-ion batteries.Adv Energy Mater2025;15:2501201

[34] Rana A,Bhadouria A.Interfacial pH gradients suppress HER at high currents in zinc metal batteries.Joule2025;9:102167

[35] Roy K,Heil JN,Dick JE.For zinc metal batteries, How many electrons go to hydrogen evolution? An electrochemical mass spectrometry study..Angew Chem Int Ed2024;63:e202319010

[36] Tang B,Liang S.Issues and opportunities facing aqueous zinc-ion batteries.Energy Environ Sci2019;12:3288-304

[37] Yang H,Yang W,Zhu R.Correlating hydrogen evolution and zinc deposition/dissolution kinetics to the cyclability of metallic zinc electrodes.Energy Environ Sci2024;17:1975-83

[38] Rana A,Heil JN.Realizing the kinetic origin of hydrogen evolution for aqueous zinc metal batteries.Adv Energy Mater2024;14:2402521

[39] Dong N,Pan H.Towards the practical application of Zn metal anodes for mild aqueous rechargeable Zn batteries.Chem Sci2022;13:8243-52 PMCID:PMC9297528

[40] Chen J,Jiang J.Challenges and perspectives of hydrogen evolution-free aqueous Zn-ion batteries.Energy Storage Mater2023;59:102767

[41] Li X,Han C.Corrosion of metallic anodes in aqueous batteries.Energy Environ Sci2025;18:2050-94

[42] Yang J,Sun Y.Zinc anode for mild aqueous zinc-ion batteries: challenges, strategies, and perspectives.Nanomicro Lett2022;14:42 PMCID:PMC8724388

[43] Blanc LE,Nazar LF.Scientific challenges for the implementation of Zn-ion batteries.Joule2020;4:771-99

[44] Kao CC,Hao J,Li H.Suppressing hydrogen evolution via anticatalytic interfaces toward highly efficient aqueous Zn-ion batteries.ACS Nano2023;17:3948-57

[45] Wang Z,Wang D.A HER‐inhibiting layer based on M‐H bond regulation for achieving stable zinc anodes in aqueous zinc-ion batteries.Adv Funct Mater2025;35:2502186

[46] Xing Z,Xie X.Zincophilic electrode interphase with appended proton reservoir ability stabilizes Zn metal anodes.Angew Chem Int Ed2023;62:e202215324

[47] Yao R,Wang L.A corrosion-free zinc metal battery with an ultra-thin zinc anode and high depth of discharge.Energy Environ Sci2024;17:3112-22

[48] Huang H,Zhao J.Boosting reversibility and stability of Zn anodes via manipulation of electrolyte structure and interface with addition of trace organic molecules.Adv Energy Mater2022;12:2202419

[49] Lu H,Wei L,Guo X.Manipulating Zn²⁺ solvation environment in poly(propylene glycol)‐based aqueous Li⁺/Zn²⁺ electrolytes for high‐voltage hybrid ion batteries.Carbon Energy2023;5:e365

[50] Zhang Y,Ding Y,Zhao Y.Electrolyte solvation chemistry for stabilizing the Zn anode via functionalized organic agents.Small2024;20:e2311407

[51] Lin L,Liu S.High-entropy aqueous electrolyte induced formation of water-poor Zn²⁺ solvation structures and gradient solid-electrolyte interphase for long-life Zn-metal anodes.Angew Chem Int Ed2025;64:e202425008

[52] Wang Y,Qi L,Li G.Regulating additive electroactivity for self-assembled multifunctional SEI in aqueous zinc batteries.Energy Storage Mater2025;81:104544

[53] Zheng Q,Hu Z.Altering the Zn²⁺ Migration mechanism enables the composite hydrogel electrolytes with high Zn²⁺ conduction and superior anti-dehydration.Adv Funct Mater2025;35:2504782

[54] Zhang Q,Ji H.Issues and rational design of aqueous electrolyte for Zn‐ion batteries.SusMat2021;1:432-47

[55] Zhu Y,Huang Y.A new insight of anti-solvent electrolytes for aqueous zinc-ion batteries by molecular modeling.Small Struct2023;4:2200270

[56] Liu Z,Li X.Constructing eutectic solvation sheath by weak solvation effect for stabilizing Zn-ion batteries with low-temperature adaptability.Energy Storage Mater2025;83:104727

[57] Yang M,Bi S.The construction of anion-induced solvation structures in low-concentration electrolyte for stable zinc anodes.Angew Chem Int Ed2024;63:e202400337

[58] Dong Y,Wang Y.Long-life zinc/vanadium pentoxide battery enabled by a concentrated aqueous ZnSO₄ electrolyte with proton and zinc ion co-intercalation.ACS Appl Energy Mater2020;3:11183-92

[59] Dai Y,Zhang C.Fluorinated interphase enables reversible Zn²⁺ storage in aqueous ZnSO₄ electrolytes.ACS Energy Lett2023;8:4762-7

[60] He Y,Gao Q,Hao Z.Dynamic interface modulation of aqueous zinc-ion batteries by rational design of organic additives.Small2025;21:e06244

[61] Zhang Y,Huang F.“Water‐in‐salt” nonalkaline gel polymer electrolytes enable flexible zinc‐air batteries with ultra-long operating time.Adv Funct Mater2022;32:2203204

[62] Emanuele E,Cerullo G.Solving ZIB challenges: the dynamic role of water in deep eutectic solvents electrolyte.J Mater Chem A2025;13:9778-90

[63] Xie J,Lei H.Electrolyte and interphase engineering of aqueous batteries beyond "water-in-salt" strategy.Adv Mater2024;36:e2306508

[64] Mo F,Meng Q.A flexible rechargeable aqueous zinc manganese-dioxide battery working at -20 °C.Energy Environ Sci2019;12:706-15

[65] Yang P,Liu Y.Thermal self‐protection of zinc‐ion batteries enabled by smart hygroscopic hydrogel electrolytes.Adv Energy Mater2020;10:2002898

[66] Jiang C,Jia M.Anti-freezing hydrogel electrolytes: from molecular engineering to applications in aqueous zinc-ion batteries.Mater Today2025;90:706-23

[67] Dong J,Yang H.Suspension electrolytes with catalytically self-expediating desolvation kinetics for low-temperature zinc metal batteries.Adv Mater2025;37:e2501079 PMCID:PMC12051820

[68] Xie D,Wang DH.ZnF₂ -riched inorganic/organic hybrid SEI: in situ-chemical construction and performance-improving mechanism for aqueous zinc-ion batteries.Angew Chem Int Ed2023;62:e202216934

[69] Sand HJ.III. On the concentration at the electrodes in a solution, with special reference to the liberation of hydrogen by electrolysis of a mixture of copper sulphate and sulphuric acid.London Edinburgh Dublin Philo. Mag J Sci2010;1:45-79

[70] Su Y,Zhang Q.Printing‐Scalable Ti₃C₂T_x MXene‐decorated janus separator with expedited Zn²⁺ flux toward stabilized Zn anodes.Adv Funct Mater2022;32:2204306

[71] Bai P,Brushett FR.Transition of lithium growth mechanisms in liquid electrolytes.Energy Environ Sci2016;9:3221-9

[72] Jiao S,Wu M,Hu H.Ion sieve: tailoring Zn²⁺ desolvation kinetics and flux toward dendrite-free metallic zinc anodes.ACS Nano2022;16:1013-24

[73] Lin C,Liu M.Dynamic regulation for the well-distribution of electrons and Zn²⁺ ions achieving uniform Zn redox in Ah-scale pouch cells.Adv Mater2025;37:e11484

[74] Liu Z,Ma Q.A dual-functional organic electrolyte additive with regulating suitable overpotential for building highly reversible aqueous zinc ion batteries.Adv Funct Mater2023;34:2214538

[75] Geng L,Wang X.Eutectic electrolyte with unique solvation structure for high-performance zinc-ion batteries.Angew Chem Int Ed2022;61:e202206717

[76] Zhu Y,Zheng X.Concentrated dual-cation electrolyte strategy for aqueous zinc-ion batteries.Energy Environ Sci2021;14:4463-73

[77] Deng S,Yang Z.Zwitterion‐separated ion pair dominated additive‐electrolyte structure for ultra‐stable aqueous zinc ion batteries.Adv Funct Mater2024;34:2408546

[78] Shi X,Wang J,Yang Z.A weakly solvating electrolyte towards practical rechargeable aqueous zinc-ion batteries.Nat Commun2024;15:302 PMCID:PMC10770389

[79] Ding Y,Du T.A trifunctional electrolyte enables aqueous zinc ion batteries with long cycling performance.Adv Funct Mater2024;34:2314388.

[80] Li G,Zhang S.A biocompatible electrolyte enables highly reversible Zn anode for zinc ion battery.Nat Commun2023;14:6526 PMCID:PMC10579325

[81] Liu S,Pang WK.Tuning the electrolyte solvation structure to suppress cathode dissolution, water reactivity, and Zn dendrite growth in zinc‐ion batteries.Adv Funct Mater2021;31:2104281

[82] Huang S,Li T,Wu P.Antifreezing hydrogel electrolyte with ternary hydrogen bonding for high-performance zinc-ion batteries.Adv Mater2022;34:e2110140

[83] Wang N,Wan H.Zincophobic electrolyte achieves highly reversible zinc-ion batteries.Adv Funct Mater2023;33:2300795

[84] Dong H,Liu R.Bio‐inspired polyanionic electrolytes for highly stable zinc‐ion batteries.Angew Chem Int Ed2023;135:e202311268 PMCID:PMC10962557

[85] Qiu H,Zhao J.Zinc anode-compatible in-situ solid electrolyte interphase via cation solvation modulation.Nat Commun2019;10:5374 PMCID:PMC6879498

[86] Gao J,Liang S,Zhou J.Inorganic colloidal electrolyte for highly robust zinc-ion batteries.Nanomicro Lett2021;13:69 PMCID:PMC8187543

[87] Xu L,Zheng X.Nanocellulose‐carboxymethylcellulose electrolyte for stable, high‐rate zinc‐ion batteries.Adv Funct Mater2023;33:2302098

[88] Chen ZJ,Xiao X.An ultrahigh-modulus hydrogel electrolyte for dendrite-free zinc ion batteries.Adv Mater2024;36:e2413268

[89] Lu H,Wei X.A recyclable biomass electrolyte towards green zinc-ion batteries.Nat Commun2023;14:4435 PMCID:PMC10363112

[90] Shi Y,Bi S,Liu L.An anti‐freezing hydrogel electrolyte for flexible zinc‐ion batteries operating at -70 °C.Adv Funct Mater2023;33:2214546

[91] Tian Z,Liu G.Electrolyte solvation structure design for sodium ion batteries.Adv Sci2022;9:e2201207 PMCID:PMC9353483

[92] Ma W,Wu X.Tailoring desolvation strategies for aqueous zinc-ion batteries.Energy Environ Sci2024;17:4819-46

[93] Liang Y,Sun P.Comprehensive review of electrolyte modification strategies for stabilizing Zn metal anodes.Adv Funct Mater2023;33:2304878

[94] Dai C,Jin X,Qu L.The emerging of aqueous zinc-based dual electrolytic batteries.Small2021;17:e2008043

[95] Deng W,Wang X.Zinc‐ion battery chemistries enabled by regulating electrolyte solvation structure.Adv Funct Mater2024;34:2405012

[96] Xu C,Du H.Energetic zinc ion chemistry: the rechargeable zinc ion battery.Angew Chem Int Ed2012;51:933-5

[97] Zhang L,Xin W,Yan Z.Engineering zincophilic sites on Zn surface via plant extract additives for dendrite-free Zn anode.Energy Storage Mater2022;44:408-15

[98] Nian Q,Feng Y.Designing electrolyte structure to suppress hydrogen evolution reaction in aqueous batteries.ACS Energy Lett2021;6:2174-80

[99] Chodankar NR,Lee S.High energy superstable hybrid capacitor with a self‐regulated Zn/electrolyte interface and 3D graphene‐like carbon cathode.InfoMat2022;4:e12344

[100] Yan H,Li S.Adjusting zinc ion de-solvation kinetics via rich electron-donating artificial SEI towards high columbic efficiency and stable Zn metal anode.Chem Eng J2022;442:136081

[101] Xie X,Gao J.Manipulating the ion-transfer kinetics and interface stability for high-performance zinc metal anodes.Energy Environ Sci2020;13:503-10

[102] Adenusi H,Passerini S,Chen G.Lithium batteries and the solid electrolyte interphase (SEI) - progress and outlook.Adv Energy Mater2023;13:2203307

[103] Lin C,Xiong P.High-rate, large capacity, and long life dendrite-free Zn metal anode enabled by trifunctional electrolyte additive with a wide temperature range.Adv Sci2022;9:e2201433 PMCID:PMC9313946

[104] Wang J,Wu H.Visualizing and regulating dynamic evolution of interfacial electrolyte configuration during de‐solvation process on lithium-metal anode.Angew Chem Int Ed2024;136:e202400254

[105] Chen Z,Yao P,Hao Z.Insight into aqueous electrolyte additives: unraveling functional principles, electrochemical performance, and beyond.Green Chem2024;26:9939-56

[106] Liu X,Yao J.Endogenous organic-inorganic hybrid interface for reversible Zn electrochemistry.Adv Energy Mater2024;14:2400090.

[107] Wang N,Duan J.A review of zinc-based battery from alkaline to acid.Mater Today Adv2021;11:100149

[108] Jiang X,Hu T,Chen Y.Aqueous eutectic electrolyte-derived organic/inorganic hybrid interphase towards reversible zinc electrochemistry for long-life zinc ion batteries.Sci China Mater2025;68:1946-58

[109] Wang D,Peng H.Functional electrolyte additives for aqueous zinc-ion batteries: progress and perspectives.ChemSusChem2025;18:e202501387

[110] Dai Q,Tu T,Song L.An appropriate Zn²⁺/Mn²⁺concentration of the electrolyte enables superior performance of AZIBs.J Mater Chem A2022;10:23722-30

[111] Zhang Y,Sun B.Mitigating concentration polarization via ion-sieving interlayer towards long-life 510 Wh Kg^-1 lithium metal pouch cells.Angew Chem Int Ed2026;65:e24476

[112] Bai S,Yi J,Qiao Y.High-power Li-metal anode enabled by metal-organic framework modified electrolyte.Joule2018;2:2117-32

[113] Ouyang B.The rise of high-entropy battery materials.Nat Commun2024;15:973 PMCID:PMC10834409

[114] Lun Z,Kwon DH.Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries.Nat Mater2021;20:214-21

[115] Zhao X,Lun Z.Design principles for zero-strain Li-ion cathodes.Joule2022;6:1654-71

[116] Stallard JC,Booth SG.Mechanical properties of cathode materials for lithium-ion batteries.Joule2022;6:984-1007

[117] Yu C,Eck ERHV.Accessing the bottleneck in all-solid state batteries, lithium-ion transport over the solid-electrolyte-electrode interface.Nat Commun2017;8:1086 PMCID:PMC5651852

[118] He B,Xin Y.Halogen chemistry of solid electrolytes in all-solid-state batteries.Nat Rev Chem2023;7:826-42

[119] Huang D,Wu Y.TRPM4-inspired polymeric nanochannels with preferential cation transport for high-efficiency salinity-gradient energy conversion.J Am Chem Soc2024;146:16469-77

[120] Zou K,Wang Q.Turing-type nanochannel membranes with extrinsic ion transport pathways for high-efficiency osmotic energy harvesting.Nat Commun2024;15:10231 PMCID:PMC11599864

[121] Huang Y,Cao Y.Scalable integration of photoresponsive highly aligned nanochannels for self-powered ionic devices.Sci Adv2024;10:eads5591 PMCID:PMC11661449

[122] Ranjith KS,Raju GSR,Han Y.V₂CT_x-MXene/winery waste derived carbon-VO₂/V2C-MXene aerogel based high-performance cathode for quasi-solid-state Zn-ion batteries.Carbon2026;248:121152

[123] Tran H,Kim C.Design of functional and sustainable polymers assisted by artificial intelligence.Nat Rev Mater2024;9:866-86

[124] Meng Q,Li L,Chen R.Smart batteries for powering the future.Joule2024;8:344-73