All-Solid-State Lithium Batteries under Low-Temperature and Fast-Charging Conditions: Challenges, Mechanisms, and Design Strategies

Abstract

All-solid-state lithium batteries (ASSLBs) are promising next-generation energy-storage systems owing to their intrinsic safety, high energy density, and compatibility with lithium metal anodes. However, their operation under low-temperature and fast-charging conditions remains severely constrained by sluggish ion transport, intensified polarization, interfacial instability, and dendrite-induced failure. In this review, we examine these limitations within a unified transport capability-demand mismatch framework. Low temperature weakens Li⁺ transport capability by suppressing thermal activation, lattice dynamics, interfacial charge transfer, and electrode diffusion, whereas fast charging increases Li⁺ transport demand through elevated current density and electrode loading. Their coupling further amplifies this mismatch, leading to transport heterogeneity, localized lithium accumulation, non-uniform reactions, chemo-mechanical degradation, and short-circuit failure. Based on this framework, we discuss recent advances in solid electrolytes, solid–solid interfaces, and electrode architectures, emphasizing wide-temperature ion conduction, adaptive interfacial regulation, homogeneous Li⁺ flux distribution, and mechanically resilient electrode design. Finally, we outline future directions involving electrolyte-interface-electrode co-design, operando diagnostics, and quantitative kinetic descriptors. This review provides a mechanistic perspective for developing ASSLBs capable of stable operation under low-temperature, fast-charging, and coupled extreme conditions.

Graphical abstract

Keywords

All-solid-state lithium batteries / Low-temperature / Fast-charging / Transport capability-demand mismatch

Highlight

	● A transport capability-demand mismatch framework is proposed for ASSLBs.
	● Low temperature weakens Li+ transport across electrolyte, interface, and electrode.
	● Fast charging increases Li+ flux, reaction rate, and electrode-loading demand.
	● Recent progress in electrolytes, interfaces, and electrodes is reviewed.
	● Future ASSLB design requires coupled transport–reaction–mechanical regulation.

1 Introduction

All-solid-state lithium batteries (ASSLBs) have emerged as one of the most promising next-generation energy storage technologies owing to their intrinsic safety, high energy density, and compatibility with lithium metal anodes [1-3]. Compared with conventional lithium-ion batteries employing liquid electrolytes, ASSLBs eliminate flammable organic solvents and enable the use of high-voltage cathodes and lithium metal anodes, thereby offering substantial improvements in both safety and energy density [4,5]. Consequently, ASSLBs have attracted extensive attention for applications ranging from electric vehicles and grid-scale energy storage to aerospace systems. However, beyond achieving high energy density and safety, practical deployment increasingly requires reliable operation under harsh environments, particularly low temperatures and high charging rates [6-9]. These conditions are frequently encountered in real-world applications such as cold-climate transportation and rapid-charging infrastructures, posing severe challenges to the electrochemical processes governing ASSLBs performance.

Low-temperature operation remains one of the most critical obstacles to the practical implementation of ASSLBs [10]. Because Li⁺ migration in solid electrolytes is inherently thermally activated, decreasing temperature significantly suppresses ionic conductivity and increases cell polarization. Sulfide electrolytes, represented by Li₁₀GeP₂S₁₂ (LGPS) and Li₆PS₅Cl argyrodites, exhibit room-temperature ionic conductivities exceeding 10^–3–10^–2 S·cm^–1; nevertheless, their transport capability deteriorates substantially at sub-zero temperatures [11-14]. In contrast, oxide electrolytes such as garnet-type Li₇La₃Zr₂O₁₂ (LLZO) generally possess higher migration activation energies and more rigid lattice frameworks, resulting in even more pronounced transport limitations under low-temperature conditions [15,16]. In addition to bulk transport degradation, sluggish charge-transfer kinetics and deteriorated solid–solid contact further increase interfacial resistance, making low-temperature operation a major bottleneck for ASSLBs.

Fast charging introduces another set of challenges associated with high current densities and accelerated electrochemical reactions in ASSLBs. Under fast-charging conditions, the demand for Li⁺ transport increases substantially, often exceeding the transport capability of solid electrolytes. This imbalance leads to severe polarization, non-uniform Li⁺ distribution, and ultimately lithium dendrite formation. Previous studies have shown that the critical current density (CCD) of many solid electrolytes is limited by interfacial instability and current constriction effects [17]. For instance, sulfide electrolytes, despite their high ionic conductivity, are prone to interfacial decomposition and dendrite penetration under high current densities. Similarly, oxide electrolytes suffer from poor interfacial contact and high interfacial resistance, which further limit their fast-charging performance. To mitigate these issues, significant efforts have been devoted to enhancing ionic conductivity, stabilizing interfaces, and homogenizing Li⁺ flux. Strategies such as introducing lithiophilic interlayers, constructing gradient interfaces, and designing composite electrolytes have shown promise in improving fast-charging capability while suppressing dendrite growth [18-20].

Importantly, low-temperature operation and fast charging are not independent challenges but are intrinsically coupled through Li⁺ transport and interfacial kinetics. Low temperatures suppress ion migration, charge transfer, and solid-state diffusion, thereby reducing the transport capability of ASSLBs, whereas fast charging substantially increases the transport demand throughout the battery system. The resulting transport capability-demand mismatch leads to severe polarization, localized lithium accumulation, interfacial degradation, and dendrite growth, ultimately governing the performance limits and failure mechanisms of ASSLBs under extreme conditions. Unlike previous reviews that discuss low-temperature operation, fast charging, electrolyte transport, interfacial degradation, and dendrite growth as separate topics, this review establishes a unified kinetic framework that bridges cross-scale Li⁺ transport-migration in solid electrolytes, charge transfer at interfaces, and diffusion within electrodes-with the continuous evolution of electrochemical and mechanical failure. Although this review primarily focuses on strictly defined ASSLBs, selected quasi-solid-state and solidified-electrolyte systems are also discussed when their design principles provide valuable insights into Li⁺ transport regulation and interfacial stabilization. Based on this framework, the coupled challenges, failure mechanisms, and corresponding design strategies are systematically discussed, providing insights into the rational design of ASSLBs capable of stable operation under low-temperature and fast-charging conditions.

2 Ion Transport in Solids

The electrochemical behavior of ASSLBs is fundamentally governed by the coupling between ion transport and interfacial reaction kinetics across multiple spatial domains. During battery operation, Li⁺ transport can be generally divided into three sequential processes: (i) Li⁺ migration through the solid electrolyte, (ii) charge transfer across solid–solid interfaces, and (iii) Li⁺ diffusion within electrode materials. Because these processes are kinetically connected in series, the overall electrochemical response is ultimately governed by the slowest transport or reaction step under a given operating condition.

Within solid electrolytes, Li⁺ migration proceeds through thermally activated hopping mechanisms, including vacancy-mediated diffusion, interstitial transport, and cooperative ion migration, depending on the crystal framework and local coordination environment [21]. Garnet- and NASICON-type electrolytes typically rely on three-dimensional percolating diffusion networks, whereas amorphous and disordered electrolytes often provide broader distributions of local coordination environments and multiple accessible migration pathways. Consequently, ionic conductivity generally follows Arrhenius-type behavior, indicating that migration barriers and lattice dynamics play decisive roles in determining ion transport efficiency. At solid–solid interfaces, Li⁺ transport is governed by interfacial charge-transfer kinetics and structural compatibility between the electrolyte and electrode. Unlike liquid-electrolyte systems, solid interfaces lack spontaneous wetting behavior and therefore consist of discrete contact regions with spatially heterogeneous ion-transfer pathways. As a result, interfacial transport is highly sensitive to interphase formation, local chemical reactions, and contact continuity [22]. Meanwhile, Li⁺ transport within electrode materials is controlled by solid-state diffusion processes, which strongly depend on crystal structure, diffusion dimensionality, defect chemistry, and local mechanical constraints [23]. Importantly, these transport processes do not operate independently. Variations in temperature, current density, electrode loading, and local electrochemical potential continuously redistribute the relative contributions of electrolyte transport, interfacial charge transfer, and electrode diffusion. Consequently, the dominant kinetic bottleneck may shift among different transport domains during battery operation. Therefore, ASSLB performance under low-temperature and fast-charging conditions cannot be interpreted solely by intrinsic ionic conductivity or interfacial resistance. Instead, it should be understood as the response of a dynamically coupled transport-reaction network, in which the dominant kinetic bottleneck shifts with temperature, current density, electrode loading, and local electrochemical environment.

3 Transport Capability-Demand Mismatch under Extreme Conditions

As illustrated in Fig. 1, the electrochemical performance of ASSLBs is fundamentally determined by the dynamic balance between transport capability and transport demand. Transport capability denotes the effective ability of the cell to sustain Li⁺ migration through solid electrolytes, charge transfer across solid–solid interfaces, and diffusion within electrode materials. In contrast, transport demand refers to the Li⁺ transport and reaction requirements imposed by a given operating condition, which are externally driven by current density and charging rate and are manifested as increased Li⁺ flux, accelerated reaction rate, and greater transport burden associated with electrode loading.

Under mild operating conditions, transport capability and transport demand can remain relatively balanced, allowing Li⁺ transport to sustain electrochemical reactions without severe polarization. However, this balance becomes increasingly difficult to maintain when the battery is operated at low temperature or under high charging rates. Low temperature primarily disrupts the balance from the capability side. At low temperatures, reduced thermal activation suppresses Li⁺ mobility in both solid electrolytes and electrode materials [24]. The weakened lattice dynamics make existing migration barriers more difficult to overcome and reduce local structural fluctuations that facilitate ion hopping, leading to progressively slower ion transport [25]. Simultaneously, interfacial charge-transfer reactions become sluggish because of reduced atomic mobility and limited interfacial adaptability. As a result, even when the external current is not substantially increased, the available transport capability may become insufficient to satisfy the required Li⁺ flux, giving rise to capability-side mismatch. Fast charging disrupts the balance from the demand side. Under high current densities, the required Li⁺ flux throughout the battery increases sharply, and steep electrochemical potential gradients develop across the electrolyte and electrode-electrolyte interfaces [26]. Meanwhile, the interfacial and electrode reactions must proceed at accelerated rates to match the imposed current, while high electrode loading further increases the total amount of Li⁺ that must be transported through longer and more tortuous pathways. In this sense, fast charging does not merely increase the external current; it imposes a coupled demand for rapid Li⁺ redistribution, accelerated interfacial/electrode reactions, and sustained transport through practical electrode architectures. When the imposed transport demand approaches or exceeds the available transport capability, concentration polarization becomes increasingly severe and local transport heterogeneity is progressively amplified. Therefore, fast charging can induce demand-side mismatch even at moderate temperatures, particularly in cells with limited interfacial contact, high electrode loading, or insufficient ionic transport pathways.

Under coupled low-temperature and fast-charging conditions, these two effects occur simultaneously: low temperature reduces transport capability, whereas fast charging increases transport demand. Their coupling widens the gap between available Li⁺ transport capability and imposed electrochemical demand, thereby producing a more severe and rapidly evolving transport capability-demand mismatch [27]. Crucially, this coupling operates through a positive feedback loop rather than simple additivity. The sluggish Li⁺ migration at low temperature cannot keep pace with the massive Li⁺ flux demanded by fast charging, leading to progressively aggravated local Li⁺ depletion and current constriction. This local depletion forces current to detour to adjacent regions, causing local current concentration and elevated overpotential, which accelerates interfacial side reactions and dendrite nucleation. Once initiated, dendrites and interfacial degradation further block ion transport pathways and weaken transport capability, entering the next round of amplified mismatch [28,29]. Consequently, Li⁺ transport within the electrolyte, across solid–solid interfaces, and inside electrode materials can no longer sustain the electrochemical reaction rate required by the external current. This amplified mismatch represents the fundamental kinetic origin of severe performance degradation in ASSLBs under extreme operating conditions. The resulting mismatch induces concentration polarization, large electrochemical-potential gradients, and spatially heterogeneous Li⁺ distributions throughout the cell. More importantly, transport heterogeneity continuously redistributes local current density, ion concentration, and interfacial overpotential during operation. Regions with limited transport capability become preferential sites for ion accumulation and current constriction, whereas regions with faster transport experience disproportionately high electrochemical activity. This spatially uneven reaction landscape further amplifies local instability, promoting a cascade from polarization to lithium accumulation, interfacial degradation, mechanical damage, and dendrite nucleation [30]. These degradation phenomena should not be regarded as isolated failure modes, but rather as different manifestations of the same underlying kinetic limitation: the inability of the transport network to accommodate the electrochemical demand imposed by the operating condition. Therefore, the transport capability-demand mismatch framework provides a unified basis for understanding ASSLBs degradation under low-temperature operation, fast charging, and coupled extreme conditions, while guiding the rational design of solid electrolytes, solid–solid interfaces, and electrode architectures.

4 Mitigation Strategies for Transport Capability-Demand Mismatch

4.1 Bulk transport limitation and electrolyte design strategies

Bulk ion transport within solid electrolytes represents the first and most fundamental kinetic bottleneck governing the performance of ASSLBs under low-temperature, fast-charging, and coupled extreme conditions. As discussed in Section 3, low temperatures suppress the intrinsic transport capability of solid electrolytes, whereas fast charging simultaneously increases the Li⁺ transport demand. The resulting transport capability–demand mismatch makes bulk ion conduction the earliest and most critical limitation under extreme operating conditions. As illustrated in Figs. 2A and 2B, efficient Li⁺ transport relies on well-defined migration networks embedded within the crystal framework of solid electrolytes [25]. Sulfide electrolytes such as LGPS possess interconnected one-dimensional and three-dimensional diffusion channels, enabling room-temperature ionic conductivities exceeding 10^–2 S·cm^–1. In contrast, garnet-type LLZO relies on a three-dimensional percolating Li sublattice, where continuous Li-site connectivity supports long-range ion migration (Fig. 2C) [31]. However, despite the structural diversity among different electrolyte families, ionic transport in all inorganic solid electrolytes remains fundamentally thermally activated. Consequently, decreasing temperature weakens lattice dynamics, reduces ion-hopping frequency, and increases migration resistance, resulting in a pronounced decline in ionic conductivity and transport kinetics. Beyond intrinsic conductivity limitations, transport heterogeneity within polycrystalline electrolytes becomes increasingly important under low-temperature fast-charging conditions. As shown in Figs. 2D–2, grain boundaries often exhibit transport properties distinct from those of the bulk lattice [32]. First-principles calculations on LLZO reveal that different grain-boundary structures can possess dramatically different Li⁺ diffusivities, ranging from bulk-like transport behavior to severely restricted diffusion pathways. Such structural heterogeneity generates local transport bottlenecks and current-constriction effects, which become progressively amplified as temperature decreases and current density increases. As a result, Li⁺ transport becomes spatially non-uniform, leading to localized ion accumulation and uneven current distribution throughout the electrolyte. More importantly, the consequences of transport heterogeneity extend far beyond conductivity loss. Under low-temperature, fast-charging, and coupled extreme conditions, localized Li accumulation continuously increases local overpotential and electric-field concentration.

As illustrated in Fig. 3A, localized lithium precipitation within inorganic solid-state electrolytes can trigger a progressive transition from transient soft short circuits to catastrophic hard short-circuit failure [33]. Defect-rich regions and grain boundaries serve as preferential sites for Li⁰ accumulation, where intermittent electronic pathways gradually evolve into continuous lithium connections, accompanied by chemo-mechanical degradation of the electrolyte. To mitigate this failure evolution, inorganic/polymer hybrid solid electrolytes introduce electronically insulating and mechanically adaptive polymer networks (Fig. 3B), which suppress lithium accumulation and electronic leakage while maintaining continuous Li⁺ transport pathways. Operando current–time measurements further reveal the dynamic transition from soft to hard short circuits (Fig. 3C). Intermittent current fluctuations indicate the initiation of soft short circuits, while subsequent current amplification corresponds to the formation of interconnected lithium pathways and irreversible hard short-circuit failure. These results demonstrate that short-circuit failure in solid-state electrolytes is a progressive electrochemical–mechanical degradation process rather than an instantaneous event.

Therefore, the degradation of solid electrolytes under low-temperature, fast-charging, and coupled extreme conditions originates not only from insufficient ionic conductivity, but also from the synergistic effects of transport heterogeneity, current constriction, chemo-mechanical degradation, and dendrite-induced failure. From this perspective, future electrolyte design should move beyond simply maximizing room-temperature conductivity and instead focus on simultaneously reducing migration barriers, homogenizing ion transport, stabilizing grain-boundary structures, and suppressing local transport bottlenecks. Such a strategy is essential for mitigating transport capability-demand mismatch and enabling stable ASSLBs operation under extreme conditions.

Sulfide electrolytes represent the most extensively studied class of inorganic solid electrolytes for high-power ASSLBs owing to their soft lattice frameworks, highly polarizable sulfur anions, and exceptionally high ionic conductivities [39,40]. Over the past decade, a wide range of sulfide systems have been developed, including LGPS-type electrolytes (Li₁₀GeP₂S₁₂ and its derivatives) [11,41-43], argyrodite electrolytes (Li₆PS₅Cl [20,44,45], Li₆PS₅Br [46,47], and Li₆PS₅I [37,48]), thio-LISICON compounds, Li₂S–P₂S₅ glass–ceramic electrolytes [49,50], and more recently, high-entropy and structurally disordered sulfide electrolytes [51-53]. Many of these materials exhibit room-temperature ionic conductivities in the range of 10^–3–10^–2 S·cm^–1, approaching those of conventional liquid electrolytes. Such exceptional transport properties make sulfide electrolytes particularly attractive for low-temperature fast-charging ASSLBs, where maintaining sufficient Li⁺ transport capability is essential for accommodating the large ion flux required under high current densities [54]. Nevertheless, room-temperature ionic conductivity alone is an insufficient descriptor for evaluating sulfide electrolytes under low-temperature, fast-charging, and coupled extreme conditions. As temperature decreases, weakened lattice dynamics reduce Li⁺ hopping frequency and increase migration resistance, leading to conductivity decay and spatially heterogeneous ion transport. Under fast charging, the imposed Li⁺ flux demand increases sharply, and severe concentration polarization emerges once the required ion flux approaches the intrinsic transport limit of the electrolyte. Therefore, the key challenge for sulfide electrolytes is not merely to maximize conductivity, but to maintain sufficient transport capability while suppressing interfacial degradation, current constriction, and chemo-mechanical failure. Accordingly, current sulfide-electrolyte design has evolved toward three interconnected strategies: surface/interface stabilization to preserve charge-transfer kinetics, compositional engineering to reduce migration barriers and improve Li-site connectivity, and structural-disorder engineering to flatten migration-energy landscapes and broaden the accessible temperature window. Representative examples are summarized in Fig. 4.

Surface and interface stabilization are essential for preserving the intrinsic transport advantage of sulfide electrolytes under high-rate or low-temperature operation. As shown in Figs. 4A–4C, non-destructive surface polymerization can improve chemical stability without sacrificing bulk ion conduction. Surface S^2– species on Li₆PS₅Cl initiate the ring-opening polymerization of 1,3,2-dioxathiolane-2,2-dioxide, forming a thin polysulfate protective layer on electrolyte particles [34]. The resulting PS-LPSC retains an ionic conductivity of approximately 4.3 mS·cm^–1 and enables high-rate operation at 60 °C, delivering 228.9, 175.8, 125.8, and 91.1 mAh·g^–1 at 0.44, 10, 50, and 100 C, respectively. This example indicates that interfacial stabilization can preserve high Li⁺ flux tolerance without compromising the fast lattice transport characteristic of sulfide frameworks. Beyond surface protection, anion/cation disorder provides a direct route to improving bulk transport capability under high-rate demand. As shown in Fig. 4D, Yao et al. designed multi-cation/anion co-substituted high-entropy HE-LPSBrCl argyrodite electrolyte to overcome the low conductivity and severe electro-chemo-mechanical failure of conventional LPSBr under fast-charging conditions [35]. The core innovation is boosting configurational entropy and anion site disorder via Si/Ge/Sn/Cl co-doping, which creates abundant inter-cage Li⁺ transport paths and reduces migration barriers. HE-LPSBrCl delivers a high room-temperature conductivity of 7.96 mS·cm^–1 (one order higher than LPSBr) with a low activation energy of 0.18 eV. The NCM712@Nb||Li-In full cell retains 37% of 0.1 C capacity at an ultrahigh 10 C rate, far superior to the pristine LPS counterpart. This result highlights that disorder engineering can improve rate capability by expanding the accessible Li⁺ migration network rather than simply increasing the nominal conductivity.

Interfacial chemistry regulation is equally important for mitigating low-temperature kinetic deterioration. Fig. 4E illustrates a LiTFSI-induced interphase design that constructs an F-rich cathode electrolyte interphase and an F/N-containing composite solid electrolyte interphase [36]. These interphases suppress parasitic reactions, facilitate Li⁺ transfer across interfaces, and stabilize electrode–electrolyte contact. Consequently, NCM811/LiTFSI@LPSC/Li cells retain 94.6 mAh·g^–1 after 75 cycles at −20 °C (Fig. 4F). Such low-temperature performance suggests that maintaining interfacial charge-transfer kinetics can be as important as enhancing bulk ionic conductivity, particularly when the transport capability is thermally suppressed. Compositional and structural engineering further provide effective routes to sustaining Li⁺ transport at low temperatures. Sb substitution in halide-sulfide hybrid electrolytes enables regulation of lattice geometry and Li⁺ migration pathways [37]. As shown in Figs. 4G and 4H, tuning the Sb content modifies both ionic conductivity and migration barriers. The optimized x = 1/3 composition delivers a room-temperature ionic conductivity of 12.7 mS·cm^–1 and a reduced Li⁺ migration barrier. The corresponding all-solid-state cell operates stably for 40 cycles at −20 °C, delivering a specific capacity of 109 mAh·g⁻¹ at 0.1 C (Fig. 4I). Similarly, Kanno et al. introduced Ge, Br, and O into the LGPS framework to form LSiGePSBrO (Figs. 4J–4L) [38]. This electrolyte maintains structural stability at ultralow temperature and exhibits a low activation energy of 0.24 eV. It delivers ionic conductivities of 32 mS·cm^–1 at 25 °C and 9 mS·cm^–1 at −10 °C. When coupled with an 800 μm-thick electrode, the corresponding ASSLB achieves an areal capacity of 22.7 mAh/cm² at room temperature and retains 73% capacity at −10 °C. These results demonstrate that reducing the temperature sensitivity of Li⁺ migration is essential for translating high room-temperature conductivity into practical low-temperature transport capability.

Collectively, sulfide electrolytes offer the highest intrinsic ion-transport capability among major inorganic solid electrolyte families, but their practical performance under low-temperature or fast-charging conditions is governed by a balance among bulk conductivity, activation energy, interfacial stability, current tolerance, and chemo-mechanical robustness. Surface/interface stabilization mainly addresses interfacial reaction and charge-transfer bottlenecks, whereas compositional disorder and high-entropy regulation enhance bulk Li⁺ mobility by broadening migration pathways and flattening energy landscapes. However, sulfide electrolytes still face critical limitations, including moisture sensitivity, interfacial reactivity toward Li metal and high-voltage cathodes, pressure-dependent contact stability, and mechanically assisted dendrite penetration under high current densities. Therefore, future sulfide-electrolyte design should move beyond conductivity-centered optimization and instead establish a multi-parameter evaluation framework that combines low-temperature ionic conductivity, activation energy, critical current density, interfacial resistance evolution, stack-pressure tolerance, and long-term cycling stability. Such a framework is essential for mitigating transport capability-demand mismatch and enabling reliable ASSLBs operation under low-temperature, high-rate, and coupled extreme conditions.

Halide electrolytes have recently received increasing attention as a complementary class of inorganic solid electrolytes for ASSLBs, particularly under low-temperature and fast-charging conditions [58,59]. Compared with sulfide electrolytes, which offer ultrahigh ionic conductivity but suffer from interfacial reactivity and moisture sensitivity, halide electrolytes generally exhibit better oxidative stability, improved compatibility with high-voltage layered cathodes, and favorable mechanical deformability [60]. Representative systems such as Li₃YCl₆ [61], Li₃YBr₆ [62,63], Li₃InCl₆ [55,64,65], Li₃ScCl₆ [66,67], and Li₂ZrCl₆ [68,69] have demonstrated room-temperature ionic conductivities in the range of 10^–3–10^–2 S·cm^–1, making them promising candidates for high-energy ASSLBs. However, most conventional halides still face limitations including moderate ionic conductivity, close-packed anion frameworks, restricted Li⁺ migration pathways, and insufficient low-temperature transport capability [70,71]. Therefore, recent studies have shifted from simply screening new halide compositions toward rationally regulating the local coordination environment, anion framework, structural disorder, and lattice dynamics to sustain fast Li⁺ transport over a wide temperature range.

Deng et al. developed a Zr–O co-doping modification strategy for Li₃InCl₆ halide solid electrolytes to address the poor Li⁺ transport and severe interfacial degradation of conventional halide conductors (Figs. 5A and 5B). Their core innovation lies in the synergistic regulation of cation and anion lattice sites: high-valence Zr⁴⁺ partial substitution creates abundant Li⁺ vacancies and introduces local lattice distortion to flatten Li⁺ migration barriers, while O^2– anion doping strengthens the structural rigidity of the host framework and suppresses harmful side reactions at halide-sulfide electrolyte interfaces. Compared with pristine Li₃InCl₆ with limited rate tolerance, the optimized Zr–O co-doped electrolyte delivers greatly boosted ionic conductivity and superior high-rate adaptability. The assembled NCM955 all-solid-state cell with modified electrolyte retains a considerable reversible capacity at an ultrahigh 5 C fast-charging rate and exhibits far milder capacity decay across 0.1–5 C gradient cycling, verifying that dual cation-anion co-doping is a reliable strategy to advance fast-charging performance of halide electrolytes. Local coordination regulation represents another important strategy for improving halide electrolytes. As illustrated in Figs. 5C–5E, Ta/Nb doping reduces the effective charge of chloride ions and improves the flexibility of anion frameworks. The as-obtained (Li_1.25Zr_0.25Ta_0.75Cl₆) delivers a high room-temperature ionic conductivity of 10.3 mS·cm^–1. As the catholyte for all-solid-state batteries, it achieves a reversible capacity of 120.7 mAh·g^–1 at 4 C and maintains 82.5% capacity after 20,000 cycles, exhibiting much better fast-charging capability and cycling stability than pristine Li₂ZrCl₆. As shown in Figs. 5F and 5G, Sun et al. developed a partially amorphous LTLOC oxyhalide electrolyte by embedding La-based functional modules into an amorphous Li⁺ conductive matrix. The core innovation of this work lies in the disordered amorphous lattice design: different from crystalline halides with fixed single Li⁺ migration tunnels, the disordered matrix creates abundant diversified local coordination environments and multi-parallel Li⁺ diffusion pathways, which weakens the rigid lattice dependence of ionic conduction. Atomic-scale simulation in Fig. 5F visualizes the interconnected continuous Li⁺ diffusion network formed inside the disordered framework. Low-temperature electrochemical measurements further verify the practical advantage of this structural design. At −30 °C, the assembled NCM88 full cell with an active material loading of ~11.5 mg·cm⁻² can deliver reversible discharge capacity under current densities ranging from 20 to 100 mA·g⁻¹ (Fig. 5G).

As illustrated in Fig. 6, anion sublattice engineering provides an effective strategy for enhancing the wide-temperature transport capability of halide electrolytes. LTOC, featuring a mixed oxygen-chlorine anion sublattice, exhibits a high room-temperature ionic conductivity of 13.7 mS·cm⁻¹ and maintains favorable Li⁺ transport capability over a broad temperature range (Fig. 6A). The corresponding NCM83-based ASSLBs deliver stable long-term cycling performance under ultralow-temperature conditions, retaining a reversible capacity of approximately 75 mAh·g⁻¹ after 400 cycles at −30 °C under 0.2 C (Fig. 6B) and maintaining a discharge capacity of approximately 70 mAh·g⁻¹ over 2000 cycles at −50 °C under 0.1 C (Fig. 6C). These results highlight that rational anion sublattice design can effectively improve low-temperature Li⁺ transport and extend the operating temperature window of halide-based ASSLBs.

Overall, the development of halide electrolytes is moving beyond conventional composition optimization toward coordination-chemistry regulation, anion-framework softening, and controlled structural disorder. Compared with sulfides, halides generally provide better high-voltage cathode compatibility and chemical robustness, but their low-temperature and fast-charging performance remains constrained by limited Li⁺ pathway connectivity, framework rigidity, and composition-dependent interfacial compatibility. Therefore, future halide-electrolyte design should not only pursue high room-temperature ionic conductivity, but also consider low-temperature activation energy, Li⁺ vacancy distribution, anion-framework flexibility, cathode interfacial stability, and high-rate cycling durability. Such a multi-parameter evaluation strategy is essential for translating the intrinsic stability of halides into practical transport capability under low-temperature, high-rate, and coupled extreme conditions.

Oxide electrolytes are widely regarded as one of the most promising solid-electrolyte families because of their excellent electrochemical stability, wide electrochemical window, and superior mechanical robustness [73,74]. Representative systems, including garnet-type Li₇La₃Zr₂O₁₂ (LLZO) [15,75], NASICON-type LATP and LAGP [76,77], and perovskite-type oxides. These materials generally exhibit high oxidative stability toward high-voltage cathodes, whereas their compatibility with lithium metal strongly depends on composition and interfacial protection. In particular, Ti- or Ge-containing oxides such as LATP, LLTO, and LAGP may suffer from interfacial reduction when directly contacted with lithium metal. From the perspective of the transport capability-demand mismatch framework, oxide electrolytes face intrinsic challenges under low-temperature, fast-charging, and coupled extreme conditions. Their rigid oxygen frameworks usually lead to relatively high Li⁺ migration barriers, strong temperature-dependent ionic transport, and pronounced grain-boundary resistance [78]. As temperature decreases, reduced lattice dynamics significantly suppress Li⁺ mobility, while fast charging simultaneously increases the transport demand, resulting in severe polarization and transport heterogeneity.

Compared with sulfide and halide electrolytes, the central challenge for oxide electrolytes is not simply achieving high room-temperature ionic conductivity, but maintaining continuous Li⁺ transport across rigid bulk frameworks, resistive grain boundaries, and mechanically mismatched solid–solid interfaces. Composite and grain-boundary engineering have therefore become important strategies for improving the rate capability of oxide-based solid electrolytes. Zheng et al. constructed a ceramic-polymer composite oxide solid electrolyte PMV-LLTeO-LiTFSI to overcome the inherent trade-off between ionic conductivity and mechanical property of single-phase oxide or polymer electrolytes [79]. The core innovation lies in constructing dual continuous Li⁺ transport networks: rigid LLTeO double perovskite fillers provide low-barrier lattice diffusion channels, while flexible PMMA/PVDF blend matrix improves conformal contact with electrodes, and LiTFSI lithium salt dissociates abundant free charge carriers. DFT calculations confirm that the heterogeneous ceramic-polymer interfaces serve as fast ion transport highways with reduced migration barriers. Optimized composite delivers a room-temperature ionic conductivity of 0.826 mS·cm⁻¹, tensile strength of 27 MPa and wide electrochemical window up to 4.88 V. Li||Li symmetric cells maintain stable plating/stripping cycling over 600 h at 1 mA·cm⁻², effectively inhibiting lithium dendrite growth. When matched with LFP cathode, the full cell retains 98.1% capacity after 300 cycles under 3 C fast-charging condition, and exhibits favorable rate capability up to 5 C. This example demonstrates that coupling rigid oxide conduction networks with flexible polymer matrices can simultaneously alleviate transport limitation and interfacial contact loss under high-rate operation. Grain-boundary regulation provides another effective route for enhancing the current tolerance of oxide electrolytes. Rosero-Navarro et al. adopted glassy Li₂O-B₂O₃ (LBO) as grain boundary modifier to address the low critical current density (CCD) limitation of garnet-type LLZT electrolyte for fast-charging batteries [80]. The core innovation is introducing amorphous LBO distributed along grain boundaries during sintering, which homogenizes Li⁺ flux and blocks dendrite propagation along intergranular channels. DFT calculations confirm that LBO delivers wider electrochemical stability window and low Li⁺ migration barrier. Although LLZT-LBO exhibits slightly higher grain boundary resistance, the modified electrolyte achieves a remarkably improved CCD of 10 mA·cm⁻², far superior to the 0.2 mA·cm⁻² of bare LLZT. The Li//LLZT-Li symmetric cell maintains stable cycling over 60 cycles at 10 mA·cm⁻² with low polarization below 15 mV, and no dendrite penetration is observed on cycled electrolyte cross-sections. These results indicate that grain boundaries should not be viewed only as resistive transport barriers; when properly engineered, they can also function as flux-homogenizing and dendrite-blocking regions under high current density.

Overall, oxide electrolytes provide chemical stability and mechanical robustness that are difficult to achieve in sulfide or halide systems, but their low-temperature and fast-charging performance remains constrained by rigid oxygen frameworks, grain-boundary-dominated resistance, poor interfacial conformity, and composition-dependent Li-metal compatibility. Their main advantage therefore lies not in maximizing intrinsic low-temperature ion mobility, but in offering high oxidative stability, mechanical support, and dendrite-resistance capability. Future oxide-electrolyte design should move beyond room-temperature conductivity optimization and instead establish a multi-parameter strategy that integrates migration-barrier reduction, defect-chemistry regulation, grain-boundary engineering, adaptive interfacial contact, electrolyte-thickness reduction, and composite toughening. Such integrated regulation is essential for preserving transport continuity and mitigating transport capability-demand mismatch under low-temperature, high-rate, and coupled extreme conditions.

Polymer and composite electrolytes provide a fundamentally different strategy for addressing the transport capability-demand mismatch in ASSLBs [83,84]. Unlike inorganic solid electrolytes, where ion transport is mainly governed by crystal structure and defect chemistry, Li⁺ migration in polymer electrolytes is strongly coupled with segmental motion, polymer–salt interactions, and local solvation environments [85]. As a result, low temperatures can severely restrict chain mobility and reduce ionic conductivity, whereas fast charging imposes elevated Li⁺ flux demand, making polymer-based electrolytes particularly sensitive to kinetic limitations. It should be noted, however, that some polymer-based systems with excellent low-temperature or high-rate performance are demonstrated in quasi-solid-state or solidified-electrolyte configurations rather than strictly all-solid-state cells. Therefore, these examples are discussed mainly for their transferable design principles, including solvation-structure regulation, weak-interaction-assisted salt dissociation, continuous Li⁺ transport networks, and mechanically adaptive interfaces.

Hu et al. proposed a PVDF-HFP solidified localized high-concentration quasi-solid electrolyte (S-LHCE) to address severe lithium metal corrosion and rapid capacity decay under high-temperature ultrafast charging [81]. As visualized in Fig. 7A, conventional liquid LCE and HCE generate abundant solvent-separated ion pairs and contact aggregates, which trigger sustained parasitic corrosion of lithium anodes, while the non-solvating PVDF-HFP framework of S-LHCE confines free DMSO solvent and rearranges solvation clusters to decouple ion pairing and Li⁺ conduction. Fig. 7B presents multi-rate discharge profiles collected at 100 °C; the S-LHCE cell delivers considerable reversible capacity even at an extreme ultrahigh rate of 50 C. The long-cycle test at 100 °C and 20 C fast-charging condition (Fig. 7C) further verifies its excellent thermal and rate durability. Benefiting from this solvation-structure regulation, the S-LHCE achieves a high Li⁺ transference number of 0.72 and stable electrochemical output within −10 to 100 °C, which enables the full cell to retain 83.3% of its theoretical capacity at 30 C and 60.1% at 50 C under 100 °C, validating the great potential of solvation engineering for wide-temperature fast-charging applications. Beyond solventized quasi-solid systems, weak-interaction modulation with MOF and ionic liquid additives is adopted to boost lithium salt dissociation and accelerate room-temperature fast-charging kinetics. As illustrated in Fig. 7D, researchers introduced carboxyl-functionalized ionic liquid (CIL) and MOF fillers into PVDF matrix to construct a weakly bonded continuous Li⁺ transport network [82]. The weak intermolecular forces among CIL, MOF and lithium salts weaken the strong Coulombic interaction between Li⁺ and anions, elevate the concentration of free mobile Li⁺, and form interconnected ion migration tunnels. Fig. 7E compares the cycling stability of pure PVDF, simple MOF/PVDF and optimized CIL-MOF/PVDF composite electrolytes under stepwise elevated rates, and Fig. 7F displays its discharge voltage platforms from 0.2 C to 7 C. The optimized CIL-MOF/PVDF electrolyte attains an ionic conductivity of 1.14 × 10⁻³ S·cm⁻¹ at 30 °C, and the assembled full cell maintains steady cycling over 500 cycles at a fast-charging rate of 6 C.

Interface mechanical adaptability and ultralow-temperature ion transport represent another critical bottleneck for polymer electrolytes. Mi’s group fabricated Ag-modified LLZTO composite PVDF electrolyte (PALA) blended with AgNO₃ additives to construct ductile Li⁺ conductive interphase [86]. Fig. 8A quantifies the room-temperature ionic conductivity of four electrolyte systems: pure PVDF only reaches 3.16 × 10⁻⁴ S·cm⁻¹, while PALA delivers an enhanced conductivity of 9.65 × 10⁻⁴ S·cm⁻¹. Fig. 8B records galvanostatic Li plating/stripping curves of PL, PAL and PALA symmetric cells under harsh −30 °C, 5 mA·cm⁻² and 5 mAh·cm⁻² conditions. The in-situ generated Ag₂S/AgF-rich interphase on PALA simultaneously reduces Li⁺ diffusion barriers and accommodates volume deformation during cycling, allowing the PALA symmetric cell to operate stably for more than 7000 h without voltage polarization surge under extreme subzero high-current conditions. To resolve disordered polymer chain motion and low-temperature conductivity drop of conventional solid polymer electrolytes, Cu-coordinated polyrotaxane (PRSE-Cu) electrolyte with ordered one-dimensional ion channels was designed [87]. Fig. 8C depicts its synthesis procedure and internal ordered Li⁺ migration pathways locked by Cu–O coordination crosslinks, which suppress random sliding of cyclodextrin rings and flatten Li⁺ migration energy barriers. Fig. 8D exhibits wide-temperature cycling performance from −20 to 60 °C under 0.1–0.5 C. This ordered channel architecture simultaneously elevates ionic conductivity and Li⁺ transference number, and the corresponding full cell retains 90.1% capacity after 1000 cycles at 0 °C, demonstrating outstanding low-temperature cycling reliability. Overall, polymer and composite electrolytes differ from inorganic electrolytes in that their transport capability is governed not only by lattice or defect structures, but also by solvation chemistry, chain dynamics, ion-pair dissociation, and interfacial mechanics. Their main advantage lies in interfacial conformity, tunable solvation environments, and mechanical adaptability, whereas their limitations include temperature-sensitive chain mobility, generally lower intrinsic ionic conductivity, possible liquid-like components in quasi-solid systems, and uncertainty in long-term stability under practical stack pressure and high cathode loading. Therefore, future polymer-based electrolyte design should move beyond conductivity enhancement alone and establish an integrated design framework combining high Li⁺ transference number, weak ion-pair association, continuous transport-network construction, solvent/activity confinement, mechanical compliance, and stable Li/electrolyte interphases. Such regulation is essential for mitigating transport capability-demand mismatch under low-temperature, high-rate, and coupled extreme conditions.

In summary, the four electrolyte families discussed above exhibit distinct advantages and limitations under low-temperature and fast-charging conditions, and no single system is universally optimal. Sulfide electrolytes offer high intrinsic ionic conductivity and favorable mechanical deformability, which benefit low-temperature ion transport and high-rate operation, but their practical application is constrained by moisture sensitivity, interfacial reactivity, pressure-dependent contact stability, and mechanically assisted dendrite penetration. Halide and oxyhalide electrolytes provide superior oxidative stability and high-voltage cathode compatibility, yet their low-temperature and fast-charging performance remains limited by insufficient ion-pathway connectivity, framework rigidity, and composition-dependent interfacial stability. Oxide electrolytes exhibit excellent chemical stability and mechanical robustness, but their rigid oxygen frameworks, high grain-boundary resistance, and poor interfacial conformity restrict ion transport and high-power operation. Polymer and composite electrolytes offer tunable ion-coordination environments, conformal interfaces, and mechanical adaptability, whereas their performance is limited by temperature-sensitive chain dynamics, relatively low intrinsic ionic conductivity, possible liquid-like components in quasi-solid systems, and uncertain long-term stability under practical stack pressure and high cathode loading. These differences indicate that electrolyte selection should be guided by the dominant transport limitation and specific operating conditions, rather than by room-temperature ionic conductivity alone. To further compare the practical relevance of different low-temperature ASSLB systems, Table 1 summarizes representative cell configurations tested at or below 0 °C, together with key metrics including operating temperature, low-temperature ionic conductivity, electrode loading, areal capacity, current density, capacity retention, and cycling stability.

4.2 Interfacial transport limitation and interface engineering strategies

Beyond bulk ion transport, solid–solid interfaces represent another critical kinetic bottleneck governing the low-temperature fast-charging performance of ASSLBs [103,104]. Unlike liquid electrolytes that can spontaneously wet electrode surfaces, ion transport in ASSLBs relies on direct solid–solid contact between electrodes and solid electrolytes. Consequently, interfacial contact quality directly determines Li⁺ transfer efficiency and strongly influences the overall transport capability of the battery system. As illustrated in Fig. 9A, the electrode–electrolyte interface is typically composed of discrete contact regions rather than a continuous contact layer [89]. Under low-temperature conditions, thermal contraction and repeated volume changes during cycling promote the formation of interfacial voids and partial delamination, reducing the effective contact area available for Li⁺ transport. Meanwhile, fast charging dramatically increases the required Li⁺ flux across the interface. As transport demand approaches or exceeds the local transport capability, current constriction and concentration polarization become increasingly pronounced, resulting in highly heterogeneous ion transport behavior. Recent multiphysics simulations have further quantified the relationship between interfacial contact and electrochemical performance. As shown in Fig. 9B, decreasing the contact coefficient leads to a substantial increase in both interfacial resistance and charge-transfer resistance, accompanied by accelerated electrolyte-matrix damage [15]. These results suggest that interfacial contact degradation not only impedes Li⁺ transport but also promotes local stress accumulation and structural deterioration, thereby creating a positive feedback loop between contact loss, impedance growth, and mechanical damage. However, emerging studies indicate that interfacial failure cannot be solely attributed to impedance increase.

Cryogenic electron microscopy observations reveal that continuous interfacial reactions play an equally important role in long-term degradation. As shown in Fig. 10A, extensive interfacial reaction layers and isolated reaction regions are formed at the Si/LGPS interface after cycling [105]. Such reactions continuously consume active lithium and electrolyte components, leading to progressive capacity loss even when impedance evolution becomes less significant. This finding suggests that sustainable interfacial reactions, rather than impedance growth alone, can dominate performance degradation under extreme operating conditions. To mitigate these challenges, increasing efforts have focused on multifunctional interfacial engineering. A representative example is shown in Figs. 10B and 10C, where simultaneous stabilization of both cathode and anode interfaces is achieved through an F-rich cathode interphase and a Mg₁₆Bi₈₄-modified lithium anode interface [19]. Such designs not only suppress parasitic reactions but also facilitate Li⁺ transport and improve interfacial structural stability. These results highlight the importance of integrating electrochemical, chemical, and mechanical considerations in interfacial design. Overall, interfacial degradation under coupled low-temperature and fast-charging conditions originates from the synergistic interaction of contact loss, transport heterogeneity, continuous interfacial reactions, and chemo-mechanical damage. Together, these processes progressively intensify the transport capability–demand mismatch and ultimately govern the performance decay and failure of ASSLBs.

After clarifying the origins of interfacial degradation, recent studies have increasingly focused on interface-engineering strategies that can maintain stable charge-transfer kinetics under low-temperature, high-rate, and coupled extreme conditions. Rather than simply reducing the initial interfacial resistance, modern interface design aims to construct chemically stable, mechanically compliant, and transport-continuous interfaces that can accommodate evolving electrochemical and mechanical environments during cycling. Representative strategies include soft interfacial buffering, mechanical anchoring, dynamically adaptive interphase reconstruction, and self-limiting interfacial chemistry, as summarized in Fig. 11.

As shown in Figs. 11A and 11B, soft interfacial buffer layers provide an effective approach for improving solid–solid contact in garnet-based ASSLBs [106]. By filling interfacial voids and enhancing conformal contact between LLZTO and electrodes, polymer-based interlayers can suppress space-charge accumulation and construct continuous Li⁺ transport pathways. For example, Li/MPE@LLZTO@MPE/LFP cells deliver a capacity retention of 87% after 200 cycles at 1 C, while NCM523-based cells retain 98% capacity after 100 cycles at 1 C. These results indicate that interfacial buffer layers improve performance not only by lowering interfacial resistance, but also by increasing the fraction of electrochemically active contact area. Beyond improving initial contact quality, maintaining interfacial continuity during repeated cycling is equally important. Figs. 11C and 11D present a nanoanchor-based strategy in which lithiated iron chloride species are formed in situ on NCM cathode surfaces [107]. These nanoanchors mechanically bind electrolyte particles to cathode surfaces, suppress interfacial crack propagation, and preserve cathode-electrolyte adhesion during repeated cycling. This mechanically reinforced interface is particularly valuable for high-loading solid-state cathodes, where repeated volume changes can otherwise induce contact loss, isolated reaction regions, and increasingly heterogeneous Li⁺ transport. Recent advances further indicate that static interphases may be insufficient for long-term operation under extreme conditions. As illustrated in Figs. 11E and 11F, dynamically adaptive interphases can continuously reconstruct the electrode–electrolyte interface through controlled anion migration and interfacial reorganization [104]. In this design, mobile anions migrate under the local electric field and form ion-conducting interphases that compensate for interfacial voids and contact loss. Such adaptive regulation enables Li metal full cells to retain 90.7% capacity after 2400 cycles at 1.25 mA·cm⁻². More importantly, pouch cells operated under zero external pressure still retain 74.4% capacity after 300 cycles, highlighting the practical relevance of dynamically adaptive interfaces for pressure-limited ASSLB configurations.

Figs. 12A and 12B demonstrate that fluorinated molecular precursors can induce the formation of thin and stable LiF-rich interphases that spontaneously terminate further interfacial reactions [108]. Such self-limiting interphases simultaneously provide chemical stability, rapid Li⁺ transport, and long-term cycling durability without continuous consumption of active lithium or electrolyte components. Compared with uncontrolled decomposition layers, thin self-limiting interphases are more favorable for maintaining low interfacial impedance and stable Li⁺ flux under high-rate operation. Collectively, these studies indicate that interface engineering in ASSLBs is evolving from static passivation toward dynamic and multifunctional regulation. Soft buffer layers mainly improve initial contact and reduce local current constriction; nanoanchors reinforce cathode-electrolyte adhesion; adaptive interphases compensate for evolving voids and contact loss; and self-limiting chemistry suppresses continuous parasitic reactions. However, most current interface designs are still evaluated under limited combinations of temperature, current density, cathode loading, and stack pressure. Future interfaces should therefore be assessed using more practical metrics, including interfacial resistance evolution, Li⁺ flux homogeneity, pressure tolerance, mechanical durability, and long-term cycling under low-temperature or high-rate conditions. Such criteria are essential for mitigating transport capability-demand mismatch at solid–solid interfaces. Because fast-charging performance is strongly affected by both transport demand and practical cell parameters, Table 2 compares representative fast-charging ASSLBs (at charge rates of 2 C or higher) in terms of areal loading, areal capacity, current density, capacity retention, and cycling life. These metrics help distinguish true high-rate capability under practical conditions from performance obtained at low loading or limited current density.

4.3 Electrode kinetic heterogeneity and structural degradation

Beyond electrolyte transport and interfacial charge transfer, electrode kinetic heterogeneity and structural instability constitute another critical limitation governing ASSLB performance under low-temperature, fast-charging, and coupled extreme conditions. Under such conditions, low temperature reduces solid-state Li⁺ diffusivity and slows electrode reaction kinetics, whereas fast charging imposes a substantially higher Li⁺ flux demand. This imbalance amplifies the transport capability-demand mismatch within electrode architectures, leading to non-uniform reaction distribution, local state-of-charge heterogeneity, stress accumulation, particle cracking, and lithium deposition instability.

For layered oxide cathodes, fast charging can induce strong reaction heterogeneity across both the electrode thickness and individual particles. As shown in Figs. 13A and 13B, electrochemo-mechanical simulations reveal that the Li concentration distribution remains relatively uniform under mild charging conditions, whereas severe Li concentration gradients emerge at high charging rates [122]. In practical thick electrodes, particles close to the separator experience higher local reaction rates because they are exposed to stronger ionic flux, while particles deeper in the electrode remain less utilized. This electrode-scale heterogeneity is further coupled with particle-scale diffusion limitations. Large polycrystalline cathode particles, owing to their long diffusion length and grain-boundary-rich structure, are more susceptible to steep intraparticle Li concentration gradients and localized stress accumulation. By contrast, small single-crystalline particles provide shorter diffusion pathways and higher mechanical robustness, thereby enabling more homogeneous delithiation and suppressing crack formation in current-concentrated regions. Electrode kinetic limitations are not restricted to bulk solid-state diffusion. Surface reaction kinetics and interphase-mediated Li⁺ transfer also play important roles, particularly at low temperatures where interfacial reaction barriers become more pronounced. As illustrated in Fig. 13C, constructing a low-barrier cathode interphase can facilitate Li⁺ transfer at the cathode surface and stabilize the electrode–electrolyte interface [123]. For ultrahigh-nickel layered oxides, solvation-structure regulation and in situ formation of inorganic-rich interphases have been shown to reduce interfacial Li⁺ transfer resistance, suppress parasitic reactions, and improve low-temperature cycling stability. Although such strategies are often demonstrated in liquid- or gel-electrolyte systems, they highlight an important principle relevant to solid-state cathode design: the electrode surface must provide not only chemical stability but also sufficiently rapid Li⁺ exchange kinetics under low-temperature operation.

Recent operando characterization further indicates that Li transport inside electrode particles cannot be fully described by classical concentration-gradient-driven diffusion. As shown in Fig. 13D, operando STXM combined with BCDI reveals nanoscale Li-rich and Li-poor regions that continuously emerge, migrate, and relax within single-crystalline NMC particles during cycling [124]. These fluctuations suggest that Li migration is governed by chemical-potential gradients rather than concentration gradients alone. Local strain fields generated by heterogeneous lithiation and delithiation can modify the chemical-potential landscape and redirect Li transport pathways, even in nominally single-crystalline particles without internal grain boundaries. This strain-associated transport behavior provides an important mechanistic link between kinetic heterogeneity, stress evolution, and structural degradation under high-rate operation. As reaction heterogeneity and stress accumulation intensify, mechanical degradation becomes increasingly difficult to avoid. Non-uniform lithiation/delithiation generates local volume mismatch within cathode particles, promoting microcrack initiation and propagation. Once formed, cracks interrupt ionic and electronic percolation pathways, expose fresh surfaces to side reactions, and isolate portions of active material from the surrounding solid electrolyte. Therefore, particle cracking is not merely a consequence of mechanical fatigue but also a source of further kinetic heterogeneity and transport collapse. On the anode side, the consequences of kinetic heterogeneity are manifested as non-uniform Li deposition and dendrite-induced failure. Under low-temperature fast-charging conditions, sluggish Li⁺ transport and increased overpotential promote localized Li accumulation at current hotspots. As shown in Figs. 13E–13G, Li dendrites can penetrate garnet-type LLZTO solid electrolytes and propagate along mechanically weakened paths [125]. Recent cryogenic electron microscopy studies reveal that plated Li can fill nanoscale crack tips and generate substantial hydrostatic stress, which induces tensile fracture of the ceramic electrolyte and drives both intergranular and transgranular crack propagation. This finding indicates that dendrite penetration in solid electrolytes should be regarded as a mechanically driven electro-chemo-mechanical fracture process rather than a purely electrochemical growth phenomenon. Based on the above failure analysis, Table 3 summarizes electrode-level design strategies that have been developed to improve high-rate ASSLBs performance. By correlating electrode side, cell configuration, charging condition, design strategy, and key performance metrics, this table emphasizes that high-rate electrode design requires simultaneous optimization of Li⁺ transport, electronic conduction, interfacial contact, and mechanical stability.

Overall, electrode degradation under low-temperature fast-charging conditions originates from the progressive amplification of kinetic heterogeneity into chemical heterogeneity, strain heterogeneity, structural fracture, and lithium deposition instability. Therefore, electrode design should not only aim to accelerate Li⁺ diffusion, but also regulate spatial reaction distribution, stabilize surface reaction kinetics, accommodate strain evolution, and suppress mechanically driven dendrite penetration. Such integrated electrode-level regulation is essential for mitigating transport capability-demand mismatch and enabling stable ASSLB operation under extreme conditions.

To address electrode-level kinetic and structural degradation, recent strategies have moved beyond simply shortening Li⁺ diffusion lengths toward constructing transport-continuous, reaction-homogeneous, and mechanically adaptive electrode architectures. Within the transport capability-demand mismatch framework introduced in Section 3, electrodes must not only sustain the elevated Li⁺ flux required during fast charging, but also maintain homogeneous reaction distributions, stable solid–solid contact, and structural integrity. Low temperature suppresses solid-state diffusion, whereas fast charging increases the imposed transport demand. When the local Li⁺ flux exceeds the available transport capability of electrode domains, diffusion heterogeneity, chemical nonuniformity, and stress localization are progressively amplified, ultimately leading to particle fracture, active-material isolation, and unstable lithium deposition.

On the cathode side, diffusion-induced electro-chemo-mechanical degradation represents a major failure pathway in ASSLBs, particularly under low-temperature or high-rate operation. As illustrated in Fig. 14A, insufficient Li⁺ diffusion within NMC secondary particles promotes heterogeneous Li distribution and the formation of Li-rich and Li-poor domains [137]. The resulting volume-change mismatch accumulates internal strain, triggers crack propagation, and isolates partial cathode regions from the surrounding solid electrolyte. These fractured domains further aggravate diffusion heterogeneity and surface chemical segregation, forming a self-amplifying degradation cycle. Surface coating provides an effective route to mitigate such coupled degradation. Fig. 14B compares the long-term cycling performance of bare NMC811 and LiNbO₃ (LNO)-modified NMC811 cathodes in sulfide-based ASSLBs. The LNO coating suppresses interfacial side reactions, homogenizes the surface chemical environment, and alleviates stress accumulation. The coated cathode delivers an initial capacity of 133 mAh·g⁻¹ and retains 116 mAh·g⁻¹ after 200 cycles, whereas the uncoated counterpart suffers rapid capacity decay. This result confirms that cathode coatings can simultaneously stabilize interfacial chemistry, mitigate particle fracture, and preserve continuous Li⁺ transport pathways. Beyond conventional coated composite cathodes, integrated mixed ionic–electronic conducting (MIEC) electrode architectures provide a promising route to reducing transport tortuosity and interfacial complexity. Conventional composite cathodes require separate active materials, solid electrolytes, and conductive carbon additives, resulting in spatially separated Li⁺/electron pathways and numerous heterogeneous interfaces. As shown in Fig. 14C, the carbon-free all-in-one Li_1.3Fe_1.2Cl₄ cathode integrates redox-active sites, Li⁺ transport pathways, and electronic conduction channels within a single crystalline phase [132]. Its multi-rate cycling performance at 60 °C is shown in Fig. 14D; the material maintains high Coulombic efficiency across 0.5–20 C and retains 90% capacity after 3000 cycles at 5 C. Fig. 14E further compares the full-cell voltage profiles of NCM83 coupled with LYC or Li_1.3Fe_1.2Cl₄, demonstrating that the MIEC component facilitates charge transfer and increases the discharge voltage plateau. Even at an areal loading of 4 mAh/cm², Li_1.3Fe_1.2Cl₄-containing electrodes retain more than 90% of their capacity from −10 to 60 °C. These results highlight the importance of integrated ionic–electronic transport networks in relieving electrode-scale transport imbalance under low-temperature or high-rate conditions.

On the anode side, severe volume fluctuations, stress concentration, and irregular lithium deposition limit high-rate cycling durability. Fig. 14F schematically illustrates the architected continuum In_0.38Sn_0.33Bi_0.29 alloy anode, which constructs bicontinuous MIEC percolation networks for simultaneous Li⁺ and electron conduction [129]. Its multiphase intermetallic structure releases lithiation/delithiation-induced stress and suppresses crack propagation. Fig. 14G presents the multi-rate discharge profiles of the corresponding full cell, while Fig. 14H further verifies its stable discharge plateaus over a wide temperature range from −20 to 60 °C. The InSnBi alloy delivers a high specific capacity of 724 mAh·g⁻¹ and an ultrahigh critical current density of 150 mA·cm⁻² at an areal capacity of 5.0 mAh/cm². When paired with LiCoO₂ at an industry-level areal loading of 6.49 mAh/cm², the full cell retains 87.5% capacity after 1300 cycles at 4 C and achieves gravimetric/volumetric jellyroll energy densities of 203.1 Wh·kg⁻¹ and 670.6 Wh·L⁻¹ at 5 C. These results demonstrate that continuous and mechanically robust MIEC networks are indispensable for stable high-rate operation of thick alloy anodes [109]. At elevated charging rates, uncontrolled lithium dendrite growth becomes a major safety concern. Traditional theories attribute dendrite formation mainly to uneven current distribution and interfacial polarization, whereas recent crystallographic simulations provide an additional mechanistic perspective. Fig. 14I compares phase-field simulations of unconstrained lithium growth and uniformly confined nucleation. Without confinement, lithium nuclei preferentially grow along high-index crystal facets and evolve into dendritic protrusions; by contrast, sustained uniform nucleation restricts anisotropic crystal growth and suppresses dendrite formation. Based on this principle, high-adhesion PAMD-based solid polymer electrolytes (PAMD-SPEs) have been developed to regulate lithium deposition morphology [136]. As shown in Fig. 14J, compared with conventional SPEs, the viscous PAMD-SPE reduces interfacial corrosion and confines deposited lithium into nanoscale granular particles through strong Li/electrolyte affinity. The PAMD-SPE symmetric cell reaches a critical current density of 9 mA·cm⁻² and sustains stable Li plating/stripping for 4500 h at 0.2 mA·cm⁻². Fig. 14K shows the discharge capacity of Li||PAMD-SPE||S full cells with a sulfur cathode loading of 10 mg·cm⁻². The cell delivers capacities of 1541.8, 1409.5, 1003.4, and 701.8 mAh·g⁻¹ at 0.2, 0.5, 1, and 2 C, respectively, with 95.5% capacity retention after 200 cycles at 1 C. These results demonstrate that regulating Li deposition through strong interfacial adhesion can effectively suppress dendrite growth under high-flux conditions.

Overall, electrode degradation under low-temperature or fast-charging conditions can be understood as a progressive evolution from diffusion heterogeneity to chemical nonuniformity, stress accumulation, contact loss, and unstable lithium deposition. From the transport capability-demand mismatch perspective, increasing electrode loading, areal capacity, and thickness raises the required Li⁺ flux and extends the effective transport distance, thereby increasing transport demand. Meanwhile, high tortuosity, non-uniform distributions of active materials, solid electrolytes, and conductive additives, and discontinuous ionic/electronic percolation networks reduce the effective transport capability of the electrode. These architectural limitations are further amplified by sluggish diffusion at low temperatures and elevated Li⁺ flux during fast charging, leading to localized polarization and heterogeneous reactions. Cathode coatings mitigate interfacial reactions and stress concentration; MIEC cathodes reduce ionic/electronic pathway discontinuity; architected alloy anodes accommodate volume fluctuation while preserving percolation networks; and high-adhesion polymer electrolytes regulate Li nucleation and suppress dendrite growth. However, many reported electrode designs are still evaluated under isolated favorable conditions, and their practical relevance must be judged together with cathode loading, areal capacity, stack pressure, electrolyte thickness, temperature, current density, and long-term cycling stability. Future electrode design should therefore move beyond simply enhancing Li⁺ transport kinetics and instead establish an integrated electrode-level framework that couples transport-network continuity, reaction homogeneity, stress accommodation, solid–solid contact preservation, and Li deposition regulation. Such integrated regulation is essential for achieving electrochemical, chemical, and mechanical stability under low-temperature, high-rate, and coupled extreme operating conditions. In addition to high-rate operation, electrode design under low-temperature conditions requires particular attention to sluggish solid-state diffusion, increased interfacial resistance, and stress accumulation. Table 4 therefore summarizes representative electrode-level strategies for low-temperature ASSLBs, highlighting how cathode modification, anode regulation, and interfacial design contribute to maintaining transport continuity and structural stability under thermally limited conditions.

4.4 Coupled multi-mechanism failure under extreme conditions

Under low-temperature, fast-charging, and coupled extreme conditions, the degradation of ASSLBs cannot be attributed to any single failure mechanism. Instead, battery failure emerges from the dynamic coupling of ion transport limitations, interfacial instability, electrode kinetic heterogeneity, mechanical degradation, and lithium dendrite growth across multiple length scales. The simultaneous reduction in transport capability and increase in transport demand fundamentally disrupt the kinetic balance of the battery system, triggering a cascade of interconnected degradation processes that progressively evolve from localized transport fluctuations to catastrophic structural failure.

As discussed in the preceding sections, low temperatures suppress Li⁺ transport within solid electrolytes, across solid–solid interfaces, and inside electrode materials, thereby reducing the overall transport capability of the battery. In contrast, fast charging dramatically increases the Li⁺ flux required to sustain electrochemical reactions. When the required transport demand approaches or exceeds the available transport capability, concentration polarization and electrochemical potential gradients rapidly develop throughout the cell. Consequently, Li⁺ transport becomes increasingly heterogeneous, leading to spatial variations in lithium concentration, current density, and reaction rate. Such transport heterogeneity constitutes the earliest manifestation of the transport capability–demand mismatch under extreme operating conditions. The resulting transport non-uniformity subsequently propagates into interfacial and electrode processes. Localized Li accumulation and uneven current distribution intensify interfacial side reactions, accelerate impedance growth, and increase charge-transfer overpotentials. Simultaneously, heterogeneous lithiation and delithiation within electrode particles generate chemical heterogeneity and non-uniform state-of-charge distributions. Recent operando studies further reveal that local strain fields can strongly interact with lithium transport pathways, producing coupled electrochemo-mechanical fluctuations that cannot be described solely by concentration-gradient-driven diffusion. Therefore, transport heterogeneity progressively evolves into reaction heterogeneity and stress heterogeneity across the battery system. As degradation accumulates, mechanical failure becomes increasingly dominant. Low-temperature thermal contraction, repeated volume changes during cycling, and stress concentration around defects collectively promote particle cracking, interfacial delamination, and electrolyte fracture. Importantly, these structural defects are not merely consequences of degradation but also active contributors to further performance deterioration. Cracks and contact loss interrupt ion-transport pathways, generate local current constriction, and amplify transport heterogeneity. This feedback mechanism continuously accelerates the transition from kinetic degradation to structural failure. Ultimately, the coupled evolution of transport heterogeneity, reaction heterogeneity, and mechanical degradation creates favorable conditions for non-uniform lithium deposition and subsequent dendrite formation. Local Li⁺ accumulation and elevated overpotentials first promote preferential lithium deposition at microcracks, grain boundaries, and mechanically weakened regions. Continued deposition at these electrochemical and mechanical hotspots then initiates dendrite growth. Once formed, dendrites further distort local current distribution, induce additional stress concentration, and accelerate crack propagation, eventually leading to internal short circuits and catastrophic battery failure.

Therefore, the degradation of ASSLBs under extreme conditions should be understood as a hierarchical electrochemical-transport-mechanical failure process rather than a simple superposition of individual degradation mechanisms. From this perspective, transport capability–demand mismatch serves as the fundamental driving force linking electrolyte transport limitations, interfacial degradation, electrode instability, and dendrite growth. Consequently, overcoming the extreme-condition performance bottleneck of ASSLBs requires simultaneous regulation of transport kinetics, interfacial chemistry, mechanical integrity, and lithium-flux distribution across the entire battery system. Future advances will depend not on optimizing individual components in isolation, but on engineering coupled transport-reaction-mechanical processes capable of maintaining dynamic stability under extreme operating conditions.

5 Conclusions and Outlook

5.1 Conclusions

In this review, we systematically examined the performance limitations of ASSLBs under low-temperature, fast-charging, and coupled extreme conditions from a unified kinetic perspective. Unlike conventional studies that treat low temperature and fast charging as independent challenges, we highlight that these two operating conditions are intrinsically coupled through their simultaneous influence on ion transport and interfacial reaction kinetics. To establish a mechanistic understanding, a unified transport–reaction framework was proposed based on three fundamental processes: Li⁺ transport within solid electrolytes, charge transfer across solid–solid interfaces, and diffusion within electrode materials. Building upon this framework, the concept of transport capability–demand mismatch was introduced to describe the fundamental kinetic origin of performance degradation under extreme operating conditions. Specifically, low temperatures reduce the transport capability of ASSLBs by suppressing ion migration and charge-transfer kinetics, whereas fast charging dramatically increases transport demand by imposing high Li⁺ flux requirements. The resulting mismatch leads to severe polarization, transport heterogeneity, local lithium accumulation, interfacial degradation, and dendrite growth, ultimately governing battery failure. From this perspective, the challenges and mitigation strategies of ASSLBs can be understood as efforts to either enhance transport capability or reduce transport heterogeneity throughout the electrolyte, interface, and electrode domains. Electrolyte design aims to accelerate ion transport and improve transport uniformity, interface engineering focuses on stabilizing charge-transfer processes and suppressing interfacial degradation, while electrode optimization seeks to improve diffusion kinetics and alleviate chemo-mechanical stress. Together, these approaches provide a coherent pathway toward mitigating kinetic mismatch and enabling stable operation under low-temperature, fast-charging, and coupled extreme conditions.

5.2 Outlook

Despite substantial progress, developing ASSLBs capable of reliable operation under low-temperature, fast-charging, and coupled extreme conditions remains a formidable challenge. Future research should move beyond the isolated optimization of individual materials or components and instead focus on quantitatively engineering the coupled transport–reaction–mechanical processes that govern dynamic rate-limiting behavior across electrolyte, interface, and electrode domains.

(i) Future solid electrolytes should be designed to maintain high transport capability over a wide temperature range. Rather than simply pursuing high room-temperature ionic conductivity, greater emphasis should be placed on minimizing temperature-dependent degradation of Li⁺ mobility, by regulating migration barriers, lattice dynamics, and local coordination environments. Strategies such as lattice softening, structural-disorder engineering, multi-anion framework design, and high-entropy chemistry offer promising routes to flatten migration-energy landscapes and construct robust ion-transport networks. A key objective is to decouple conductivity magnitude from its temperature sensitivity, enabling stable Li⁺ flux under sub-zero and high-current conditions.

(ii) Interface design should evolve from passive stabilization toward dynamic and adaptive regulation. Future interphases should simultaneously provide fast charge-transfer kinetics, chemical compatibility, mechanical resilience, and long-term structural integrity. Adaptive and self-healing interfaces capable of accommodating stress accumulation, maintaining intimate solid–solid contact, and repairing local defects may offer transformative solutions. Importantly, interface engineering should be evaluated not only by initial resistance reduction, but also by interfacial resistance evolution under sustained current and pressure fluctuations.

(iii) Regulating Li⁺ flux distribution throughout the battery is essential for suppressing transport heterogeneity and dendrite formation. Advanced electrode architectures, including three-dimensional frameworks, porous transport networks, and compositionally graded structures, should be developed to homogenize current distribution and minimize local transport bottlenecks. Coupling these architectures with lithiophilic interfaces, alloy-based hosts, and controlled lithium-nucleation strategies may further improve deposition uniformity. A critical direction is to establish spatially resolved Li⁺ flux regulation rather than global conductivity enhancement.

(iv) A deeper mechanistic understanding requires the integration of advanced operando characterization and multiscale modeling. Techniques such as synchrotron X-ray imaging, neutron scattering, cryogenic electron microscopy, and operando spectroscopy, combined with machine-learning-assisted simulations and digital battery models, can provide critical insights into the dynamic evolution of ion-transport pathways, interfacial reactions, stress accumulation, and dendrite growth. Future studies should further correlate these observations with quantitative descriptors such as activation energy distribution, interfacial kinetic asymmetry, and critical current thresholds.

(v) Establishing comparable evaluation standards is essential for translating individual material innovations into meaningful cell-level performance comparisons. Future studies should report both intrinsic transport properties and practical cell parameters under clearly defined testing conditions. Key metrics include temperature-dependent ionic conductivity with corresponding activation energy, critical current density with specified temperature, stack pressure, electrolyte thickness, and testing protocol, electrode loading and areal capacity, interfacial resistance evolution upon cycling, and cycling stability under specified rates and operating conditions. Standardized reporting of these metrics will enable meaningful cross-system comparisons, allow the field to distinguish intrinsic material improvements from engineering optimizations, and clarify whether enhanced transport properties can be effectively translated into practical cell-level performance.

(vi) The next generation of ASSLBs will require an integrated electrolyte-interface-electrode co-design paradigm. Rather than independently optimizing ionic conductivity, interfacial stability, electrode diffusion, or mechanical strength, future battery systems should be designed as highly coupled transport–reaction–mechanical networks. In this framework, transport capability, transport demand, interfacial compatibility, reaction uniformity, and mechanical adaptability must be simultaneously matched. The central design principle should shift toward balancing local kinetic demand with spatially resolved transport capability across all battery domains.

Overall, future advances in ASSLBs will depend not only on breakthroughs in materials chemistry, but also on the establishment of integrated kinetic design principles that bridge ion transport, interfacial reactions, and mechanical stability. Such a framework will be essential for transforming ASSLBs design from empirical optimization to predictive, mechanism-guided engineering.

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