Designing Anode-Electrolyte Interfaces for Low-Temperature Lithium- and Sodium-Ion Batteries: Challenges and Strategies
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Designing Anode-Electrolyte Interfaces for Low-Temperature Lithium- and Sodium-Ion Batteries: Challenges and Strategies
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  • Jeong-A Lee
    Jeong-A Lee
    Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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  • Chaeeun Song
    Chaeeun Song
    Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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  • Seung Hee Han
    Seung Hee Han
    Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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  • Boguen Kim
    Boguen Kim
    Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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  • Nam-Soon Choi*
    Nam-Soon Choi
    Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    *E-mail: [email protected]
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    Orcidhttps://orcid.org/0000-0003-1183-5735
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ACS Energy Letters

Cite this: ACS Energy Lett. 2025, 10, 11, 5474–5484
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https://doi.org/10.1021/acsenergylett.5c02918
Published October 25, 2025

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Abstract

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Lithium-ion and sodium-ion batteries are gaining prominence as energy storage platforms for extreme environments, particularly at low temperatures. However, the prevailing assumption of electrochemical similarity between Li+ and Na+ in the conventional design paradigm has prevented exploration of their distinct low-temperature degradation pathways, which are intensified by hindered interfacial ion transport at the anode. Herein, we present the differences in solvation structures, desolvation kinetics, and ion-transport mechanisms across the solid-electrolyte interphase (SEI) between Li+ and Na+ at low temperatures. While lithium-ion systems are constrained by sluggish desolvation kinetics, sodium-ion systems face severe interfacial resistance arising from inhomogeneous SEI compositions and weakened interactions between Na+ ions and SEI species. Recognizing these ion-specific interfacial bottlenecks, we propose electrolyte design strategies that enhance ion transport and interfacial stability at the anode. These insights provide rational frameworks for developing next-generation alkali-ion batteries capable of overcoming the distinct challenges posed by low-temperature operation.

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Published as part of ACS Energy Letters special issue “The Evolving Landscape of Energy Research: Insights from Leading Researchers”.

The rapid expansion of electric mobility, aerospace exploration, military operations, and renewable energy deployment in extreme environments has led to a steadily growing demand for batteries capable of operating efficiently at subzero temperatures. (1) Because climate resilience and energy accessibility are considered key global challenges, development of advanced energy storage systems with stable low-temperature performance has attracted considerable interest in both industry and academia. Considering the technological maturity, cost-effectiveness, and scalability of lithium-ion and sodium-ion battery (LIB and SIB) systems, these battery chemistries continue to attract widespread attention as promising energy storage solutions for cold environments. (2,3) Therefore, a significant research effort has been devoted to enhancing the cycle stability, electrolyte ionic conductivity, and interfacial stability of LIB and SIB systems under low-temperature conditions. (4) However, as the operating temperature declines, the interfacial impedance at the anode markedly increases, inducing electrolyte decomposition, disrupting interfacial integrity, and hindering alkali-ion intercalation during charging. Although cathode-related limitations also contribute to battery performance degradation at low temperatures, the development of tailored interfacial stabilization strategies at the anode is vital for enabling high-efficiency operation under subambient conditions.
While LIBs typically utilize graphite anodes with a well-ordered layered structure and an interlayer spacing of 3.35 Å, which enables efficient Li+ intercalation and a theoretical capacity of 372 mAh g–1, SIBs employ hard carbon anodes with a turbostratic structure, characterized by disordered graphene layers and a larger interlayer spacing of ∼3.7 Å. (5−8) This expanded spacing accommodates the larger Na+ ions, while disordered regions provide additional capacity through pore-filling mechanisms. Under the assumption of similarity between SIB and LIB chemistries, early research often directly applied electrolyte formulations and interfacial strategies developed for LIBs to SIBs. (9−19) This oversimplification has hindered any pursuit for a deep understanding of the electrochemical differences between Li+ and Na+ ions, including solvation structures, interfacial dynamics, and redox behavior, particularly under challenging conditions such as low-temperature operation (Table S1). Although LIBs and SIBs experience performance degradation at low temperatures, their primary limiting mechanisms differ significantly owing to the intrinsic properties of their charge carriers. In LIBs, the main bottleneck stems from the slow desolvation of Li+ ions at the graphite–electrolyte interface, a process influenced by the relatively strong interactions between Li+ ions and the solvents (Figure 1a). (20−22) The sluggish desolvation of Li+ ions significantly increases interfacial resistance by hindering charge-transfer kinetics at the graphite–electrolyte interface. As a result, parasitic reactions are more likely to occur, leading to the formation of an unstable solid electrolyte interphase (SEI) and promoting undesirable Li metal plating instead of uniform Li+ intercalation into the graphite lattice. By contrast, the larger ionic radius of Na+ compared to Li+ results in inherently weaker electrostatic interactions with solvents and anions in the electrolyte (Figure 1b). (23−25) This weaker coordination enables a more facile desolvation process, even under low-temperature conditions. Nonetheless, owing to their larger ionic radius of Na+ compared to Li+, SIBs using hard carbon anodes face a distinct bottleneck of the inherently sluggish Na+ transport through the SEI imposing significant interfacial resistance and limiting efficient sodiation kinetics. (26−29) The larger size also leads to a lower cationic charge density and weaker Lewis acidity of Na+ ions. (30) As a result, the Coulombic interactions between Na+ and SEI species are relatively weak, which slows down anode–electrolyte interfacial kinetics and impedes efficient Na+ migration across the SEI. Moreover, the lower ionic conductivity of crystalline NaF (4.6 × 10–21 S cm–1) relative to crystalline LiF (6.2 × 10–13 S cm–1) provides further evidence that Na+ ion transport through SEI is considerably hindered. (31)

Figure 1

Figure 1. Schematic illustration of challenges encountered in (a) Li-ion and (b) Na-ion batteries under low-temperature conditions.

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The increased interfacial resistance not only impedes efficient pore-filling of Na+ within the hard carbon anodes but also induces localized Na metal plating, indicating ineffective Na+ insertion. (26) These limitations become increasingly pronounced at lower operating temperatures, where the sluggish Na+ transport across the SEI exacerbates interfacial polarization and promotes parasitic side reactions, ultimately deteriorating the electrochemical performance of batteries. Consequently, given the fundamentally different degradation mechanisms that significantly influence low-temperature operation in LIBs and SIBs, electrolyte design strategies must be tailored to the distinct interfacial chemistry and ion transport characteristics at the anode surface. Based on this perspective, we present a comparative framework for understanding how the solvation chemistry and SEI functionality in Li- and Na-ion battery systems differ under low-temperature conditions.
Given the fundamentally different degradation mechanisms that significantly influence low-temperature operation in LIBs and SIBs, electrolyte design strategies must be tailored to the distinct interfacial chemistry and ion transport characteristics at the anode surface.
By analyzing the charge-transfer bottlenecks and interfacial phenomena specific to each system, we propose electrolyte engineering that enables efficient ion transport and charge-transfer reactions at the anode–electrolyte interface, thereby facilitating a robust cryogenic performance. These insights are expected to guide the development of next-generation alkali-ion batteries capable of overcoming the distinct challenges posed by low-temperature operation.

Interfacial Challenges Underlying Anode Instability at Low Temperatures

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The desolvation energy barrier in LIBs is closely related to the minimum electrostatic potential (ESPmin) of the solvent. More negative ESPmin values reflect stronger Li+–solvent interactions; consequently, a higher desolvation energy is required (Figure 2a). (23,32) This relationship establishes ESPmin as a critical descriptor for rational electrolyte design. In LIBs, Li+ ions exhibit substantially higher desolvation energy barriers (∼50 kJ mol–1) relative to Na+ ions (∼20 kJ mol–1) (Figure 2b). This fundamental difference in electronic properties, attributed primarily to the inherently higher charge density and stronger Lewis acidity of Li+ ions, causes Li+ ions to form stronger electrostatic interactions with electron-donating solvent molecules. As a result, the desolvation process becomes the predominant rate-limiting step in the interfacial charge transfer kinetics. When electrolytes incorporate solvents containing carbonate, sulfolane, amide, or dinitrile functional groups capable of forming mono- or bidentate coordination with Li+ ions, the desolvation barrier further increases (Figure 2b,c). The detachment of the solvent sheath of Li+ ions becomes more important at subzero temperatures. Cho et al. experimentally demonstrated that the number of coordinating carbonates in the first solvation shell of Li+ ions increases with a decrease in the population of the contact ion pairs (CIP) as the temperature decreases. More specifically, two or more carbonate molecules replace a single PF6– anion, and this substitution becomes more pronounced as the solvation structure transitions toward solvent-separated ion pair (SSIP) configurations. (33) The dominance of the SSIP structure at subzero temperatures corresponds to an increased desolvation energy barrier, which hinders efficient charge transfer at the anode. At subzero temperatures, the increased fraction of SSIP configurations significantly alters the interfacial chemistry by promoting the reductive decomposition of solvent molecules during charging (Figure 2d).

Figure 2

Figure 2. (a) Correlation between the absolute |ESPmin| values of solvent species and the desolvation energy of Li+ ion. Reproduced with permission from ref (23). Copyright 2013 The Electrochemical Society. (b) Comparative desolvation energies of different cation species. (c) Correlation between the coordination number of cations and the solvation power depending on the functional groups. (d) Effect of operating temperature on the solvation environment and SEI structure. Reproduced with permission from ref (35). Copyright 2024 Wiley-VCH. (e) Temperature-dependent bond-breaking modes and corresponding changes in SEI composition at low temperatures. Reproduced with permission from ref (37). Copyright 2023 Springer Nature.

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The solvent-dominated solvation sheath promotes the creation of an amorphous organic-rich SEI on the anode surface, typically comprising long-chain and cyclic species such as lithium ethylene dicarbonate (Li2EDC) and 1,3-dioxol-2-one. (34) These components fail to block solvent molecule infiltration, resulting in undesired SEI thickening and a high energy barrier for Li+ ion transport. Thus, the solvation sheath affects not only the desolvation kinetics but also the SEI structure. In particular, reduced anion participation in the solvation sheath at low temperatures promotes the formation of a less compact organic-dominant SEI. This results in a higher probability of solvent molecule infiltration near the anode and an increase in the charge transfer resistance (Rct) due to solvent-decomposition-induced SEI thickening. (35) By contrast, at room temperature, enhanced entry of anions in the solvation shell facilitates the formation of inorganic SEI species such as LiF and Li3P. These crystalline inorganic species are more tolerant during repeated cycling, maintaining a thin and uniform SEI that ensures a low energy barrier for Li+ ion migration. (36) In addition to the changes in the solvation structure at low temperatures, the bond-breaking pathways of solvent molecules such as ethylene carbonate (EC), dimethyl carbonate (DMC), and fluoroethylene carbonate (FEC) are also altered. This leads to the formation of metastable intermediate species such as -RC═O···Li (R = (CH2)x) along with various organic substances (R-O···Li), contributing to a less compact and more fragile SEI structure that remains susceptible to further changes through continued decomposition reactions (Figure 2e). (37) To counteract these effects, the use of weakly solvating solvents is critical for the design of electrolytes for low-temperature batteries.
In LIBs, the solvation environment controls the desolvation energy of Li+ ions, thereby modulating interfacial charge transfer kinetics and the structural evolution of the SEI, particularly under low-temperature environment.
These solvents, which are characterized by less negative ESPmin values, facilitate easier Li+ desolvation while simultaneously promoting the construction of an inorganic-rich SEI. Such SEIs exhibit high chemical, electrochemical, and mechanical stabilities, effectively reducing the charge-transfer resistance and enhancing the low-temperature performance of LIBs. Compared to LIB electrolytes, which suffer from sluggish desolvation at low temperatures, SIB electrolytes exhibit a substantial energy barrier for Na+ ion transport across the SEI (Figure 1b). In particular, under low-temperature operation, this kinetic limitation is exacerbated because the suppressed Na+ ion mobility across the SEI markedly increases the interfacial resistance, leading to severe polarization and degradation of battery performance. In such environments, SEI resistance emerges as the primary kinetic bottleneck in SIB systems, in contrast to the desolvation-dominated kinetic limitations observed at the anode-electrolyte interface in LIBs. During this process, the sluggish insertion of Na+ into the nanopores and interlayers of hard carbon anodes at subambient temperatures further exacerbates the interfacial instability. Incomplete sodiation promotes undesired Na metal plating on the surface of hard carbon anodes, which intensifies parasitic reactions at the anode-electrolyte interface and the accumulation of electrolyte decomposition byproducts. These side reactions induce uncontrolled SEI formation with spatially heterogeneous chemical compositions and morphological inhomogeneities. In addition, the SEI lacks structural continuity, giving rise to discontinuous ion transport pathways that increase the tortuosity of Na+ ion transport (Figure 1b). This discontinuity not only raises the overpotential but also leads to irreversible capacity loss and interfacial instability during cycling. Intrinsic differences in Li- and Na-ion chemistry lead to markedly different degradation pathways at low temperatures, underscoring the need for electrolyte designs tailored to each alkali-ion battery system.
Degradation mitigation for SIBs under low-temperature operation requires the design of a compositionally and morphologically uniform SEI that sustains continuous Na+ ion transport pathways and reduces interfacial resistance.
For LIBs, engineering of solvation structures to reduce desolvation barriers is key, whereas for SIBs, formation of uniform, ionically conductive SEIs is essential for mitigation of the interfacial transport limitations arising from sluggish Na+ transport kinetics. System-specific design strategies are crucial for ensuring the reliable low-temperature operation of emerging Li- and Na-based energy storage technologies.

Electrolyte Design Strategies to Overcome Low-Temperature Performance Limits

Recent advances have highlighted that molecular-level precision in controlling cation-solvent, solvent–solvent, and cation–anion interactions can provide new avenues for optimization of low-temperature battery performance (Figure 3a and Table S2). The solvation environment surrounding the Li+ ions plays a key role in governing the desolvation kinetics and interfacial charge transfer efficiency. The high electronegativity of the oxygen atoms in the NO3– anion enhances anion participation in the primary solvation shell with strong affinity toward Li+, shifting the 7Li NMR peak downfield and indicating weakened solvation states. Furthermore, steric modulation of the solvent molecules enables the formation of anion-incorporated weak solvation structures through diminishing Li+–solvent interactions. Bulky alkyl substituents positioned adjacent to the coordinating oxygen atoms, such as those in cyclopentyl methyl ether, enable anion-dominated weak coordination, thereby facilitating Li+ desolvation and the formation of an inorganic-rich SEI (Figure 3a). Consequently, the graphite/Li half-cell exhibited outstanding low-temperature performance with a high discharge capacity of 319 mAh g–1 and an initial Coulombic efficiency of 86.3% at −60 °C and 0.1 C. (38) In addition to steric regulation, molecular fluorination provides an effective approach to modulate Li+ ion coordination strength. Fluorinated esters, including ethyl difluoroacetate (EDFA) and methyl difluoroacetate (MDFA), reduce Li+ coordination strength by decreasing the electron density at the donor sites. Asymmetric fluorination of the difluoromethyl (CF2H) group induces a local dipole; F atoms also participate in the Li+ coordination structure, balancing solvation affinity and salt dissociation (Figure 3a, b). (39,40) In this configuration, asymmetric fluorination modifies the overcoordinated Li+-solvent complex, while the electron-withdrawing effect maintains ion-dipole interactions for effective salt dissociation. This balance positions the EDFA and MDFA within the blue-colored zone of the solvent design map shown in Figure 3b, which is characterized by a low donor number (DN) and moderate dielectric constants. The solvents in the blue-colored zone exhibit modest Li+-solvent binding energies and optimal salt dissociation, enabling both efficient desolvation kinetics and high ionic conductivity even under subzero conditions.

Figure 3

Figure 3. (a) Schematics of internal limitations and strategies for regulation of solvation structures for low-temperature LIBs. (b) Solvent diagram of DN versus dielectric constant. Solvents located in the blue-colored zone are denoted as soft solvents characterized by a lower DN and moderate dielectric constant, which reduce the Li+-solvent interactions without compromising ionic conductivity, where ε indicates the dielectric constant of solvents. (c) Electrolyte screening via the maximum and minimum values of the ESP surfaces. Reproduced with permission from ref (44). Copyright 2024 American Chemical Society. (d) Selection of deshielding anions based on the relative 7Li chemical shift and compatibility with graphite anodes. Reproduced with permission from ref (35). Copyright 2024 Wiley-VCH. (e) Transport barriers and ionic conductivities of SEI components at room temperature. (36,47−49) (f) Ionic conductivity of SEI as a function of grain size, where η and σ indicate viscosity and ionic conductivity, respectively. Reproduced with permission from ref (51). Copyright 2025 Wiley-VCH.

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Beyond direct Li+-solvent modifications, solvent–solvent interactions provide additional control mechanisms beyond direct Li+-solvent modifications. Nonsolvating dipole-active molecules such as fluorobenzene (FB) act as “pull” cosolvents; in propylene carbonate (PC)-based electrolytes, FB interacts with PC through dipole–dipole interactions, weakening Li+-PC coordination and facilitating Li+ release to graphite anode under subzero conditions. (41,42) By contrast, cosolvents such as methyl pentafluoropropionate or 2,2-difluoroethyl trifluoromethanesulfonate (DTF) function as “push” molecules, forming hydrogen bonds with Li+-coordinated oxygen atoms to reduce the localized electron density. (43,44)
More specifically, the −CF2H group in DTF has a highly positive maximum electrostatic potential, pushing away the solvent molecules from Li+ ions during the desolvation process at low temperatures (Figure 3a,c). Another strategy for solvation sheath modulation involves controlling anions entering the first solvation sheath (Figure 3a). Variations in cation–anion interactions, determined by the specific anion, can suppress solvent participation in the solvation sheath, thereby lowering the Li+ desolvation energy. Anions such as NO3–, Cl–, and Br– exhibit strong coordination with Li+, reducing the shielding effect and enabling faster Li+ desolvation at the anode surface under low-temperature conditions (Figure 3d and Table S3). (35,45) Among these ions, NO3– is particularly notable, as it promotes the creation of anion-derived inorganic-rich SEI components such as Li3N, which facilitate Li+ transport and enhance electrochemical reversibility of the anode at low temperatures. Construction of an appropriate SEI is critical for overcoming the inherently sluggish Li+ migration through the SEI at low temperatures. (46) Organic-rich SEI species such as Li2EDC and Li alkyl carbonates that are generated from carbonate solvent decomposition possess high transport barriers, thereby impeding Li+ transport. Mechanistically, the low-dielectric alkyl carbonate components bind Li+ to the carbonyl sites, so that Li+ migration proceeds primarily via slow segmental motions, increasing activation energies and yielding tortuous conduction pathways. By contrast, inorganic-rich SEI species, such as LiF, Li2CO3, and Li3N, generally exhibit lower transport barriers for Li+ ions because their structures allow Li-ion permeability through vacant sites and grain boundary pathways (Figure 3e). However, even among the inorganic components, an additional criterion must be met for optimal low-temperature performance, namely, the inorganic component must show a high ionic conductivity. For example, Li3N, Li3P, and Li3PO4, formed via the decomposition of inorganic salts or additives such as LiNO3 and LiPO2F2, offer particularly high ionic conductivities compared to LiF, enabling rapid Li+ insertion into the anode and effectively suppressing Li dendrite growth, which is one of the primary degradation modes at low temperatures. (50) For LiF, the strong Li–F ionic bond leads to a high lattice defect formation energy, thereby limiting the creation of Li+ vacancies and resulting in inherently low ionic conductivity. By contrast, Li3N and Li3P have intrinsically high Li+ vacancy concentrations within their frameworks, enabling vacancy-mediated diffusion and more rapid migration of Li+ ions through their structures. In addition to the chemical composition, the geometric characteristics of the SEI are crucial. Small-grained SEI structures provide abundant pathways for Li+ transport across the anode-electrolyte interface (Figure 3f), while also offering accessible insertion sites, thereby minimizing the energy barrier for Li+ migration. (51) Collectively, the reduction of both desolvation energy and SEI transport resistance, achieved through electrolyte design that tailors solvation structures and engineers SEI composition and morphology is essential for mitigating low-temperature degradation. While both LIB and SIB systems face sluggish ion transport kinetics, hindered desolvation process, and limited ionic conductivity of SEI species, lower ionic mobility of Na+ across the SEI necessitates Na-specific interfacial engineering to address the distinct rate-limiting steps in SIBs. (24,31,52) The structural tolerance of hard carbon anodes in SIBs enables the use of solvents such as PC, DME, and G2 which are incompatible with graphite anodes due to solvent cointercalation, broadening the range of possible solvent electrolytes with low freezing points and high ionic conductivities. (53−56) Owing to its weaker Coulombic interactions with solvent molecules, Na+ promotes cation–anion aggregation, increasing anion participation in the primary solvation sheath and facilitating the formation of an inorganic-rich SEI phase with low electrolyte solubility, high mechanical strength, and chemical inertness. (11) Effective anion participation to form a uniform, inorganic SEI is the key criterion in low-temperature electrolyte design. Highly concentrated electrolytes (HCEs), localized high-concentration electrolytes (LHCEs), and weakly solvating electrolytes (WSEs) aim to create anion-dominated solvation environments. However, HCE and LHCE systems are less suitable for low-temperature operation due to sluggish ion transport in the bulk electrolyte. Under WSE conditions, anion-rich solvation environments are more prevalent in Na+-based electrolytes, facilitating the formation of highly conductive and mechanically robust inorganic-rich SEIs for low-temperature operation. However, strongly solvating electrolytes (SSEs) and WSEs exhibit significant temperature-dependent solvation shifts. A decrease in the operational temperature increases solvent coordination, displacing anions from the primary solvation shell and weakening the benefits of WSEs. (57−60) Hybrid solvating electrolytes (HSEs) blend solvents with strong and weak cation-solvent binding strengths and maintain anion-rich structures by stabilizing CIP and aggregates under subzero conditions (Figure 4a). Solvents with high salt-dissociation ability can serve as the strongly binding solvents in an HSE when combined with a cosolvent of relatively low binding strength (Figure S1). This facilitates the generation of inorganic-enriched SEI that promotes interfacial stability at subambient temperatures. Moreover, the resulting solvation heterogeneity increases the entropy, reduces the ion-cluster size, and enhances the ion mobility at low temperatures. (58,61,62) The solvent coordination number (CNs) and charge-transfer activation energy (Ea,ct) highlight the superior performance of HSEs (Figure 4b). (62−65) Compared to WSEs, HSEs exhibit slightly increased CNs while lowering Ea,ct, forming dense, inorganic-rich SEIs that improve ion transport and suppress electrolyte decomposition during low-temperature cycling. Uniform inorganic-rich SEIs, and particularly NaF-rich layers, offer high ion transport through their grain boundaries and enhance SEI stability owing to their chemical inertness. (28,29,31,66) Inorganic-rich SEI can be obtained by tuning solvation structures toward temperature-resilient anion dominance for preferential reduction. (Figure 4c,d).

Figure 4

Figure 4. (a) Schematic of conditions required for low-temperature operation with strongly solvating electrolyte, weakly solvating electrolyte, and hybrid solvating electrolyte. (b) Solvent coordination number and charge-transfer activation energy with strongly solvating solvent, weakly solvating solvent, and hybrid solvating solvent. (c) Solvent-derived SEI formation and slow Na+ transport through inhomogeneous organic-rich SEI. (d) Anion-derived SEI formation and fast Na+ transport through uniform inorganic-rich SEI.

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Hybridizing the solvation state can simultaneously address desolvation and SEI migration energy barriers at ultralow temperatures.
Inorganic-rich SEIs typically offer higher ionic conductivity compared to organic-rich SEIs, due to their abundant grain boundaries, mechanical integrity, and uniform, thin SEI with short ion-transport pathways. (67,68) Therefore, increasing the proportion of inorganic species within the SEI is an effective strategy for facilitating ion transport at the anode-electrolyte interface. (69) In addition, optimal electrochemical performance under subzero conditions necessitates not only an ion-transmittable inorganic-rich SEI, but also a homogeneous spatial distribution of its constituents (Figure 4c,d). (70) Regarding spatial uniformity, the PF6– anion outperforms FSI– and TFSI– by forming smaller ion clusters and facilitating a compact, uniform inorganic SEI. (71)
Inhomogeneous distribution of organic/inorganic domains disrupts the continuity of ion conduction pathways, resulting in localized current density and severe polarization at the anode, which triggers undesired Na metal plating. (72) Such heterogeneity also undermines the integrity of the SEI, inducing localized regions where persistent parasitic reactions are likely to occur. (73)
To further improve the ion transport through the SEI, reducing the grain size increases the density of the grain boundaries, which serve as fast ion transport channels, thereby improving the overall ionic diffusivity. Adjustment of the applied current density and desolvation energy of the electrolyte influences the nucleation behavior and growth kinetics of inorganic grains within SEI. (51,74) Moreover, electrolytes with multiple salts can diversify anion-derived inorganic constituents, promoting the formation of grain-boundary-rich SEI with improved electrochemical resilience. (75)

Summary and Outlook

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To enable widespread integration of alkali-ion batteries into temperature-sensitive sectors, such as electric mobility and aerospace technologies, it is crucial to ensure stable electrochemical performance across an extended temperature window. As depicted in Figure 5, mitigating the deterioration of battery performance at low temperatures involves multiple challenges. (34,62,64,65,76) The degradation triggers the divergence between LIBs and SIBs because of fundamental differences between the two in terms of ion transport properties, solvation thermodynamics, and interfacial chemistry.

Figure 5

Figure 5. Challenges for achieving suitable low-temperature battery performance and electrolyte design strategies. HFGA: hexafluoroglutaric anhydride, TMSP: tris(trimethylsilyl) phosphate, TMSB: tris(trimethylsilyl) borate, DTD: 1,3,2-dioxathiolane 2,2-dioxide.

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(1) Both LIBs and SIBs are prone to alkali-metal plating on the anode surface under subambient conditions because their limited electrochemical kinetics promote parasitic electrolyte decomposition and interfacial instability of the anodes. In addition, such adverse interfacial phenomena culminate in elevated impedance and deteriorated capacity retention during low-temperature operation. Furthermore, the nonuniform deposition of Li or Na exacerbates local current density hotspots, accelerating dendritic growth and increasing the risk of internal short-circuiting, which further undermines the cycling stability. Stringent overpotential control is required to suppress the Li or Na plating on the anode surface under kinetically constrained conditions at low temperatures. The desolvation energy barrier can be mitigated by precisely tuning cation-solvent coordination, optimizing solvent–solvent interactions, and modulating cation–anion associations (Figure 3a). Such adjustments collectively promote weaker Li+/Na+-solvent binding and enhance anion participation within the primary solvation sheath, thereby facilitating a faster charge transfer at the electrode–electrolyte interface. The predominantly inorganic, thin, and homogeneous SEI was mainly formed by the preferential decomposition of anions in the solvation shell. Inorganic-rich SEIs typically possess a high carrier concentration, which confers superior ionic conductivity and enhanced chemical stability. Furthermore, the uniform spatial distribution of the SEI components ensures consistent ion flux and minimizes tortuosity, thereby facilitating efficient charge transport. The strategic integration of finely tuned solvation structures with the use of functional additives enables the formation of optimized SEIs, which are particularly suited for stable subzero operation.
Engineering a crystalline, inorganic-rich SEI with coherent grain boundaries enhances interfacial stability and facilitates ion transport during subzero operation. (77) An additive-centric approach effectively complements the anion-derived SEI design. Fluorine-releasing additives, such as FEC and hexafluoroglutaric anhydride, promote LiF/NaF-rich robust and electrically insulating passivation layers, (78,79) while phosphorus- (tris(trimethylsilyl)phosphate, ethoxy (pentafluoro) cyclotriphosphazene), sulfur- (1,3,2-dioxathiolane 2,2-dioxide, trimethylsilyl methanesulfonate), and boron-containing additives (tris(trimethylsilyl)borate, sodium tetrakis [3,5-bis(trifluoromethyl)phenyl] borate) yield dense inorganic phases with favorable ionic transport properties. (80−84) Through preferential reduction at the anode-electrolyte interface, these additives suppress anion consumption from the primary solvation sheath and help preserve the intended anion-rich solvation structure over long-term cycling. The resulting grain-boundary-rich domains provide ion pathways that lower the activation barrier for Li+/Na+ migration, thereby improving the electrochemical stability and rate capability at low temperatures.
(2) Early investigations into electrolytes that can operate at low temperatures primarily emphasized physical properties such as the ionic conductivity and freezing point of the solvent. However, these parameters alone are not directly predictive of the electrochemical performance under subambient conditions. Recent advances in electrolyte design have revealed that tuning the solvation structure is a powerful strategy for regulating the SEI quality to enable high-performance LIBs and SIBs under extremely low-temperature conditions. In particular, enhancing anion participation in the primary solvation shell through electron donation by the coordinating atoms and the steric effects of bulky substituents can shift the coordination equilibrium toward anion-dominated SEI structures (Figure 2d). This approach weakens Li+–solvent interactions, facilitates Li+ desolvation, and promotes the formation of thin, stable, inorganic-rich SEIs with superior ionic conductivity.
(3) In LIBs, a decrease in the operating temperature intensifies the Li+-ion–solvent coordination, rendering desolvation at the anode-electrolyte interface the rate-determining step in interfacial transport. By contrast, SIBs benefit from intrinsically weaker Na+-ion–solvent interactions and a lower desolvation barrier but suffer from sluggish Na+ ion transport across a structurally and compositionally heterogeneous SEI (Figure 1a,b). This results in pronounced ion transport limitations and an elevated overpotential during low-temperature cycling. To address these challenges, electrolyte engineering should focus on modulating cation-solvent, solvent–solvent, and ion–ion interactions to optimize the solvation thermodynamics and interfacial ion transport. Specifically, promoting the formation of anion-derived SEI with electrochemical resilience is vital for mitigating Na-ion transport bottlenecks and ensuring reliable battery operation in low-temperature environments. HSEs, comprising a mixture of strongly and weakly solvating solvents, effectively preserved the anion-dominant solvation structures, even under sub–ambient conditions (Figure 4a). This configuration facilitates a low desolvation energy and promotes the formation of an inorganic-rich SEI at reduced temperatures. The entropically enhanced solvation environments in HSEs contribute to the dissociation of large ion aggregates into smaller clusters, thereby accelerating ion transport, while simultaneously mitigating salt crystallization and solvent freezing. Notably, the inorganic-rich SEI derived from HSEs exhibits superior uniformity, low interfacial resistance, and mechanical robustness and is particularly beneficial for Na-based battery systems operating under harsh thermal environments. Consequently, the rational design of temperature-resilient electrolyte systems offers a promising strategy for mitigating the intrinsic thermal limitations of LIBs and SIBs. By mitigating temperature-induced challenges, alkali-ion batteries can achieve wider applicability in sectors such as electric vehicles, aerospace, and grid storage, where environmental temperature fluctuations are critical design constraints.

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  • Authors
    • Jeong-A Lee - Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    • Chaeeun Song - Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    • Seung Hee Han - Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    • Boguen Kim - Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
  • Author Contributions

    J.-A.L., C.S., S.H.H., and B.K. contributed equally to this work. N.-S.C. designed the project, administration, concept, supervision, original draft writing, and editing.

  • Notes
    The authors declare no competing financial interest.

Biographies

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Jeong-A Lee is a Ph.D. candidate in the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science and Technology (KAIST), South Korea, under the supervision of Prof. Nam-Soon Choi. Her research focuses on the development of functional electrolyte additives for lithium–metal batteries and anode-free lithium–metal batteries.

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Chaeeun Song is a Ph.D. candidate at the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science and Technology (KAIST), South Korea, under the supervision of Prof. Nam-Soon Choi. Her research focuses on the development of functional electrolytes for lithium-ion and lithium–metal batteries.

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Seung Hee Han is a Ph.D. candidate at the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science and Technology (KAIST), South Korea, under the supervision of Prof. Nam-Soon Choi. Her research focuses on the development of functional electrolytes for lithium-ion batteries and Zn–Br batteries.

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Boguen Kim is a Ph.D. candidate in the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science and Technology (KAIST), South Korea, under the supervision of Prof. Nam-Soon Choi. His research focuses on the development of electrolytes for lithium–metal batteries.

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Nam-Soon Choi is a Professor in the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science and Technology (KAIST) in South Korea. Her research focuses on the mechanistic studies of electrode–electrolyte interfaces and the design of tailored electrolyte systems for next-generation rechargeable batteries (https://surfchem.kaist.ac.kr/).

Acknowledgments

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This research was supported by the Global TOP Strategic Research Center Project through the Ministry of Science and ICT (MSIT), the National Research Council of Science and Technology (NST) (GTL24012-000), and a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. RS-2024-00427700).

References

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  • Abstract

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    Figure 1

    Figure 1. Schematic illustration of challenges encountered in (a) Li-ion and (b) Na-ion batteries under low-temperature conditions.

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    Figure 2

    Figure 2. (a) Correlation between the absolute |ESPmin| values of solvent species and the desolvation energy of Li+ ion. Reproduced with permission from ref (23). Copyright 2013 The Electrochemical Society. (b) Comparative desolvation energies of different cation species. (c) Correlation between the coordination number of cations and the solvation power depending on the functional groups. (d) Effect of operating temperature on the solvation environment and SEI structure. Reproduced with permission from ref (35). Copyright 2024 Wiley-VCH. (e) Temperature-dependent bond-breaking modes and corresponding changes in SEI composition at low temperatures. Reproduced with permission from ref (37). Copyright 2023 Springer Nature.

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    Figure 3

    Figure 3. (a) Schematics of internal limitations and strategies for regulation of solvation structures for low-temperature LIBs. (b) Solvent diagram of DN versus dielectric constant. Solvents located in the blue-colored zone are denoted as soft solvents characterized by a lower DN and moderate dielectric constant, which reduce the Li+-solvent interactions without compromising ionic conductivity, where ε indicates the dielectric constant of solvents. (c) Electrolyte screening via the maximum and minimum values of the ESP surfaces. Reproduced with permission from ref (44). Copyright 2024 American Chemical Society. (d) Selection of deshielding anions based on the relative 7Li chemical shift and compatibility with graphite anodes. Reproduced with permission from ref (35). Copyright 2024 Wiley-VCH. (e) Transport barriers and ionic conductivities of SEI components at room temperature. (36,47−49) (f) Ionic conductivity of SEI as a function of grain size, where η and σ indicate viscosity and ionic conductivity, respectively. Reproduced with permission from ref (51). Copyright 2025 Wiley-VCH.

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    Figure 4

    Figure 4. (a) Schematic of conditions required for low-temperature operation with strongly solvating electrolyte, weakly solvating electrolyte, and hybrid solvating electrolyte. (b) Solvent coordination number and charge-transfer activation energy with strongly solvating solvent, weakly solvating solvent, and hybrid solvating solvent. (c) Solvent-derived SEI formation and slow Na+ transport through inhomogeneous organic-rich SEI. (d) Anion-derived SEI formation and fast Na+ transport through uniform inorganic-rich SEI.

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    Figure 5

    Figure 5. Challenges for achieving suitable low-temperature battery performance and electrolyte design strategies. HFGA: hexafluoroglutaric anhydride, TMSP: tris(trimethylsilyl) phosphate, TMSB: tris(trimethylsilyl) borate, DTD: 1,3,2-dioxathiolane 2,2-dioxide.

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