Advanced materials and computational methods in potassium-sulfur batteries

Abstract

Potassium-sulfur (K-S) batteries have emerged as an ideal candidate for large-scale energy storage because of the high theoretical energy density and low material cost. However, the practical deployment of K-S batteries is impeded by challenges such as polysulfide shuttling, sluggish conversion kinetics, and interfacial instability. Despite extensive experimental work in materials development, the underlying mechanisms at the atomic and molecular levels remain poorly understood. Computational methods have proven useful for elucidating K-S electrochemistry from a microscopic perspective. Nevertheless, a comprehensive review that systematically combines these experimental advances with computational insights is still lacking. To address this gap, this review provides a comprehensive overview of advances in K-S battery research, with emphasis on the materials engineering and computational research. We first summarize the fundamental mechanisms of K-S batteries and progress in key battery components including cathode, anode, electrolyte, as well as binder and separator. Complementing these experimental efforts, we introduce the theoretical foundations of density functional theory and molecular dynamics simulations, and review their recent applications in critical aspects such as adsorption energetics, reaction kinetics, electronic properties, and dynamic behaviors. Finally, we outline future directions for K-S battery research, including the integration of advanced characterization with multi-scale simulation, the development of high-throughput experimental and computational platforms, and the application of artificial intelligence to accelerate the development of materials and computational simulations. This review aims to provide guidance for the rational design of high-performance K-S battery systems by integrating experimental and theoretical insights.

Keywords

Potassium-sulfur batteries / advanced materials / density functional theory / molecular dynamics

References

[1] Braff WA,Trancik JE.Value of storage technologies for wind and solar energy.Nat Clim Chang2016;6:964-9

[2] Vogt ETC.The refinery of the future.Nature2024;629:295-306

[3] Zhu Z,Ali M.Rechargeable batteries for grid scale energy storage.Chem Rev2022;122:16610-751

[4] Ngoy KR,Yoro KO.Lithium-ion batteries and the future of sustainable energy: a comprehensive review.Renew Sustain Energy Rev2025;223:115971

[5] Jiang T,Zhang Z.Battery technologies for grid-scale energy storage.Nat Rev Clean Technol2025;1:474-92

[6] Li M,Chen Z.30 years of lithium-ion batteries.Adv Mater2018;30:1800561

[7] Khan A,Roy PK,Sathi SA.Challenges and the way to improve lithium-ion battery technology for next-generation energy storage.Energy Environ Mater2025;8:e70088

[8] Yao W,Lai T,Manthiram A.Rechargeable metal-sulfur batteries: key materials to mechanisms.Chem Rev2024;124:4935-5118

[9] Ma L,Wu J,Jin Z.Recent advances in emerging non-lithium metal-sulfur batteries: a review.Adv Energy Mater2021;11:2100770

[10] Li J,Zheng W.Addressing cation mixing in layered structured cathodes for lithium-ion batteries: a critical review.Nano Mater Sci2023;5:404-20

[11] Prajapati A, Bhatnagar A. A review on anode materials for lithium/sodium-ion batteries.J Energy Chem2023;83:509-40

[12] Seh ZW,Zhang Q.Designing high-energy lithium-sulfur batteries.Chem Soc Rev2016;45:5605-34

[13] Shao Y,Bird L,Shearing PR.Contemporary trends in lithium-sulfur battery design: a comparative review of liquid, quasi-solid, and all-solid-state architectures and mechanisms.Adv Energy Mater2025;16:e03239

[14] Chen Z,Wang W.Interface engineering strategies for shuttle mitigation in alkali metal-sulfur batteries: a comparative review from Li-S to Na-S and K-S systems.Nano Micro Lett2026;18:167 PMCID:PMC12765804

[15] Ding J,Fan W,Hu W.Review of emerging potassium-sulfur batteries.Adv Mater2020;32:1908007

[16] Streng RL,Senyshyn A.A low-cost and high-energy aqueous potassium-ion battery.J Energy Chem2025;106:523-31

[17] Zhao X,Qian Z,Guo Z.Potassium-sulfur batteries: status and perspectives.EcoMat2020;2:e12038

[18] Liu P.Emerging potassium metal anodes: perspectives on control of the electrochemical interfaces.Acc Chem Res2020;53:1161-75

[19] Hosaka T,Hameed AS.Research development on K-ion batteries.Chem Rev2020;120:6358-466

[20] Salado M,Pozo-Gonzalo C,Lanceros-Méndez S.Advanced and sustainable functional materials for potassium-ion batteries.Energy Mater2023;3:300037

[21] Lei YJ,Liang Y.Progress and prospects of emerging potassium-sulfur batteries.Adv Energy Mater2022;12:2202523

[22] Wang H,Kang F.Solid electrolyte interphase (SEI) in potassium ion batteries.Energy Environ Sci2020;13:4583-608

[23] Zhao Q,Zhang K.Potassium-sulfur batteries: a new member of room-temperature rechargeable metal-sulfur batteries.Inorg Chem2014;53:9000-5

[24] Lu X,Sprenkle VL.A low cost, high energy density, and long cycle life potassium-sulfur battery for grid-scale energy storage.Adv Mater2015;27:5915-22

[25] Hwang J,Yoon CS.Toward high-safety potassium-sulfur batteries using a potassium polysulfide catholyte and metal-free anode.ACS Energy Lett2018;3:540-1

[26] Xiong P,Zhao X.Room-temperature potassium-sulfur batteries enabled by microporous carbon stabilized small-molecule sulfur cathodes.ACS Nano2019;13:2536-43

[27] Ge X,Wang P.Metal-organic framework-derived nitrogen-doped cobalt nanocluster inlaid porous carbon as high-efficiency catalyst for advanced potassium-sulfur batteries.ACS Nano2020;14:16022-35

[28] Ye C,Chao D.Catalytic oxidation of K₂S via atomic co and pyridinic N synergy in potassium-sulfur batteries.J Am Chem Soc2021;143:16902-7

[29] Lee S,Rizell J.High-energy and long-lifespan potassium-sulfur batteries enabled by concentrated electrolyte.Adv Funct Mater2022;32:2209145

[30] Ye C,Li H,Gu Q.Reducing overpotential of solid-state sulfide conversion in potassium-sulfur batteries.Angew Chem Int Ed2023;62:e202301681

[31] Song W,Zhang T.Optimizing potassium polysulfides for high performance potassium-sulfur batteries.Nat Commun2024;15:1005 PMCID:PMC10837207

[32] Chen X,Cen Z.Organosulfur-rich porous carbon cathode enables soluble-polysulfide-free and high-rate potassium-sulfur batteries.Angew Chem Int Ed2025;65:e05751

[33] Yu X.A reversible nonaqueous room-temperature potassium-sulfur chemistry for electrochemical energy storage.Energy Storage Mater2018;15:368-73

[34] Liu Y,Wang J.Sulfur nanocomposite as a positive electrode material for rechargeable potassium-sulfur batteries.Chem Commun2018;54:2288-91

[35] Hwang J,Sun Y.High performance potassium-sulfur batteries based on a sulfurized polyacrylonitrile cathode and polyacrylic acid binder.J Mater Chem A2018;6:14587-93

[36] Ma R,Wang J.Confined and covalent sulfur for stable room temperature potassium-sulfur battery.Electrochim Acta2019;293:191-8

[37] Ma S,Zhang H.Iodine-doped sulfurized polyacrylonitrile with enhanced electrochemical performance for room-temperature sodium/potassium sulfur batteries.Chem Commun2019;55:5267-70

[38] Zhang Y,Shuai Y.A novel rechargeable potassium-sulfur battery based on liquid alloy anode.Mater Lett2019;242:5-8

[39] Wang L,Liu Q.Concentrated electrolytes unlock the full energy potential of potassium-sulfur battery chemistry.Energy Storage Mater2019;18:470-5

[40] Yao Y,Chen M.Encapsulation of SeS₂ into nitrogen-doped free-standing carbon nanofiber film enabling long cycle life and high energy density K-SeS₂ battery.ACS Nano2019;13:4695-704

[41] Zhang S,Li M.Orbital electron coupling of Ga-Cd dual-atom sites catalyzes sulfur redox in potassium-sulfur battery.Nat Commun2025;16:8652 PMCID:PMC12484955

[42] Li Q,Kumar P.Ultralow concentration nonflammable electrolytes mediated by intermolecular interactions for safer potassium-ion sulfur batteries.Adv Funct Mater2024;35:2416714

[43] Li C,Yu J.Three birds with one stone: multifunctional separators based on SnSe nanosheets enable high-performance Li-, Na- and K-sulfur batteries.Adv Energy Mater2024;14:2303551

[44] Chen R,He J.Advanced computational methods in lithium-sulfur batteries.Adv Funct Mater2024;34:2407986

[45] Huang M,Hou Q.et al. Theoretical calculation and computational simulation on electrolyte for lithium metal battery.Prog Chem2023;35:1847-63

[46] Feng S,Chen X.A review on theoretical models for lithium-sulfur battery cathodes.InfoMat2022;4:e12304

[47] Yao N,Fu Z.Applying classical, ab initio, and machine-learning molecular dynamics simulations to the liquid electrolyte for rechargeable batteries.Chem Rev2022;122:10970-1021

[48] Wang X,Zhang J.Dual-conductivity optimization toward high-rate and ultralong life all-solid-state lithium-sulfur batteries.Adv Mater2026;38:e22976

[49] Yuan F,Zhang D.Fundamental understanding and research progress on the interfacial behaviors for potassium-ion battery anode.Adv Sci2022;9:2200683 PMCID:PMC9284147

[50] Hosaka T,Kubota K,Komaba S.Potassium metal as reliable reference electrodes of nonaqueous potassium cells.J Phys Chem Lett2019;10:3296-300

[51] Xiao N,Wu Y.Reversible dendrite-free potassium plating and stripping electrochemistry for potassium secondary batteries.J Am Chem Soc2017;139:9475-8

[52] Shao J,Qin L,Ren Y.K₃SbS₄ as a potassium superionic conductor with low activation energy for K-S batteries.Angew Chem Int Ed2022;61:e202200606 PMCID:PMC9314013

[53] Schrödinger E.Quantisierung als eigenwertproblem.Ann Phys2006;384:361-76

[54] Schrödinger E.An undulatory theory of the mechanics of atoms and molecules.Phys Rev1926;28:1049-70

[55] Born M.Zur quantentheorie der molekeln.Ann Phys1927;389:457-84

[56] Hohenberg P.Inhomogeneous electron gas.Phys Rev1964;136:B864-71

[57] Kohn W.Self-consistent equations including exchange and correlation effects.Phys Rev1965;140:A1133-8

[58] Wang L.Local-density-derived semiempirical pseudopotentials.Phys Rev B1995;51:17398-416

[59] Perdew JP.Pair-distribution function and its coupling-constant average for the spin-polarized electron gas.Phys Rev B1992;46:12947-54

[60] Perdew JP,Ernzerhof M.Generalized gradient approximation made simple.Phys Rev Lett1996;77:3865-8

[61] Perdew JP.Accurate and simple analytic representation of the electron-gas correlation energy.Phys Rev B1992;45:13244-9

[62] Perdew JP,Burke K.Rationale for mixing exact exchange with density functional approximations.J Chem Phys1996;105:9982-5

[63] Heyd J,Ernzerhof M.Hybrid functionals based on a screened Coulomb potential.J Chem Phys2003;118:8207-15

[64] Stephens PJ,Chabalowski CF.Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields.J Phys Chem2002;98:11623-7

[65] Liang J,Wang H,Hu W.Porosity engineering towards nitrogen-rich carbon host enables ultrahigh capacity sulfur cathode for room temperature potassium-sulfur batteries.Nanomaterials2022;12:3968 PMCID:PMC9696911

[66] Wang B,Zhang Y.An energetic K⁺-S aqueous battery with 96% sulfur redox utilization.Joule2024;8:2033-48

[67] Zhang ZW,Zhao M.Heterogeneous/Homogeneous mediators for high-energy-density lithium-sulfur batteries: progress and prospects.Adv Funct Mater2018;28:1707536

[68] Zhang S,Gu Y.Strong d-π orbital coupling of Co-C₄ atomic sites on graphdiyne boosts potassium-sulfur battery electrocatalysis.J Am Chem Soc2024;146:4433-43

[69] Li Y,Xing Y.Multiscale simulation for electrolyte design: From microstructure-property decoding to macroscopic performance prediction.Energy Storage Mater2026;86:104927

[70] Wang J,Caldwell JW,Case DA.Development and testing of a general amber force field.J Comput Chem2004;25:1157-74

[71] Mackerell AD,Foloppe N.Development and current status of the CHARMM force field for nucleic acids.Biopolymers2000;56:257-65

[72] Jorgensen WL,Tirado-Rives J.Development and testing of the OPLS all-atom force field on conformational energetics and properties of organic liquids.J Am Chem Soc1996;118:11225-36

[73] Hermans J,Van Gunsteren WF.A consistent empirical potential for water-protein interactions.Biopolymers2004;23:1513-8

[74] Chenoweth K,Goddard WA.ReaxFF reactive force field for molecular dynamics simulations of hydrocarbon oxidation.J Phys Chem A2008;112:1040-53

[75] Song N,Zhang Y.B4C nanoskeleton enabled, flexible lithium-sulfur batteries.Nano Energy2019;58:30-9

[76] García-Melgarejo V,Núñez-Rojas E.Parametrization with explicit water of solvents used in lithium-ion batteries: cyclic carbonates and linear ethers.J Phys Chem B2020;124:4741-50

[77] Islam MM,Borodin O.ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials.Phys Chem Chem Phys2015;17:3383-93

[78] Hartree DR.The wave mechanics of an atom with a non-coulomb central field. Part I. theory and methods.Math Proc Camb Phil Soc2008;24:89-110

[79] Xu Y,Sun D,Zhou X.Recent advances in electrolytes for potassium-ion batteries.Adv Funct Mater2022;33:2211290

[80] Chen J,Wang S.Rechargeable potassium-ion full cells operating at -40 °C.Angew Chem Int Ed2023;62:e202307122

[81] Hu Y,Geng Y.Chloro-functionalized ether-based electrolyte for high-voltage and stable potassium-ion batteries.Angew Chem Int Ed2024;63:e202403269

[82] Ye S,Chen X.Boosting the “solid-liquid-solid” conversion reaction via bifunctional carbonate-based electrolyte for ultra-long-life potassium-sulfur batteries.Angew Chem Int Ed2023;62:e202307728