Inorganic-Enriched Solid Electrolyte Interphases: A Key to Enhance Sodium-Ion Battery Cycle Stability?

The characteristics of solid electrolyte interphase (SEI) at both the cathode and anode interfaces are crucial for the performance of sodium-ion batteries (SIBs). The research demonstrates the merits of a balanced organic component, specifically the organic sodium alkyl sulfonate (ROSO2Na) featured in this work, in conjunction with the inorganic sodium fluoride (NaF), to enhance the interfacial stability. Using a customized electrolyte, it has optimized the interphase, curbing excess NaF production, and created a thin and uniform NaF/ROSO2Na-rich SEI layer. It offers exceptional protection against interface deterioration, transition metal dissolution, and concurrently ensures a consistent reduction in interfacial impedance. This creative approach results in a substantial improvement in the performance of both the Na0.9Ni0.4Fe0.2Mn0.4O2 cathode and the hard carbon anode. The cathode demonstrates remarkable average Coulombic efficiency exceeding 99.9% and a capacity retention of 81% after 500 cycles. Furthermore, the Ah-level pouch cell has shown outstanding performance with an 87% capacity retention after 400 cycles. Moving beyond the prevailing focus on inorganic-rich SEI, these results highlight the effectiveness of the customized organic-inorganic hybrid SEI formulation in improving SIB technology, offering an adaptable solution that ensures superior interfacial stability.

Low-cost BPO4 In Situ Synthetic Li3PO4 Coating and B/P-Doping to Boost 4.8 V Cyclability for Sulfide-Based All-Solid-State Lithium Batteries.

Structural damage of Ni-rich layered oxide cathodes such as LiNi0.8Co0.1Mn0.1O2 (NCM811) and serious interfacial side reactions and physical contact failures with sulfide electrolytes (SEs) are the main obstacles restricting ≥4.6 V high-voltage cyclability of all-solid-state lithium batteries (ASSLBs). To tackle this constraint, here, a modified NCM811 with Li3PO4 coating and B/P co-doping using inexpensive BPO4 as raw materials via the one-step in situ synthesis process is presented. Phosphates have good electrochemical stability and contain the same anion (O2-) and cation (P5+) as in cathode and SEs, respectively, thus Li3PO4 coating precludes interfacial anion exchange, lessening side reactivity. Based on the high bond energy of B─O and P─O, the lattice O and crystal texture of NCM811 can be stabilized by B3+/P5+ co-doping, thereby suppressing microcracks during high-voltage cycling. Therefore, when tested in combination with Li─In anode and Li6PS5Cl solid electrolytes (LPSCl), the modified NCM811 exhibits extraordinary performance, with 200.36 mAh g-1 initial discharge capacity (4.6 V), cycling 2300 cycles with decay rate as low as 0.01% per cycle (1C), and 208.26 mAh g-1 initial discharge capacity (4.8 V), cycling 1986 cycles with 0.02% per cycle decay rate. Simultaneously, it also has remarkable electrochemical abilities at both -20 °C and 60 °C.

Correlating Differences in the Surface Activity to Interface-Induced Particle Formation in Different Protein Modalities: IgG mAb Versus Fc-Fusion Protein.

The propensity of protein-based biologics to form protein particles during bioprocessing can be related to their interfacial properties. In this study, we compare the surface activity and interfacial film properties of two structurally different biologics, an IgG and Fc-fusion, in the absence and presence of interfacial dilatational stresses, and correlate these differences to their tendency to form interface-induced protein particles. Our results show that interface-induced particle formation is protein-dependent, with the Fc-fusion demonstrating greater interfacial stability. This observation can be correlated with faster adsorption kinetics of the Fc-fusion protein, and formation of a less incompressible film at the air-liquid interface. The addition of polysorbate 80 (PS80), commonly added to mitigate protein particle formation, led to a surfactant-dominant interface for quiescent conditions and coadsorption of protein and surfactant for the Fc-fusion when exposed to interfacial stress. On the other hand, for the IgG molecule, the surface always remained surfactant dominant. Image analysis demonstrated that PS80 was more effective in mitigating particle formation for the IgG than Fc-fusion. This suggests that a surfactant-dominant interface is necessary to prevent interface-induced protein particle formation. Further, while PS80 is effective in mitigating particle formation in the IgG formulation, it may not be the best choice for other protein modalities.

A Supramolecular Deep Eutectic Electrolyte Enhancing Interfacial Stability and Solution Phase Discharge in Li-O2 Batteries.

Li-O2 batteries (LOBs) have gained widespread recognition for their exceptional energy densities. However, a major challenge faced by LOBs is the lack of appropriate electrolytes that can effectively balance reactant transport, interfacial compatibility, and non-volatility. To address this issue, a novel supramolecular deep eutectic electrolyte (DEE) has been developed, based on synergistic interaction between Li-bonds and H-bonds through a combination of lithium salt (LiTFSI), acetamide (Ace) and boric acid (BA). The incorporation of BA serves as an interface modification additive, acting as both Li-bonds acceptor and H-bonds donor/acceptor, thereby enhancing the redox stability of the electrolyte, facilitating a solution phase discharge process and improving compatibility with the Li anode. Our proposed DEE demonstrates a high oxidation voltage of 4.5 V, an ultrahigh discharge capacity of 15225 mAh g-1 and stable cycling performance of 196 cycles in LOBs. Additionally, the intrinsic non-flammability and successful operation of a Li-O2 pouch cell indicate promising practical applications of this electrolyte. This research broadens the design possibilities for LOBs electrolytes and provides theoretical insights for future studies.

Quantification of Charge Transport and Mass Deprivation in Solid Electrolyte Interphase for Kinetically-Stable Low-Temperature Lithium-Ion Batteries.

Graphite (Gr)-based lithium-ion batteries with admirable electrochemical performance below -20 °C are desired but are hindered by sluggish interfacial charge transport and desolvation process. Li salt dissociation via Li+-solvent interaction enables mobile Li+ liberation and contributes to bulk ion transport, while is contradictory to fast interfacial desolvation. Designing kinetically-stable solid electrolyte interphase (SEI) without compromising strong Li+-solvent interaction is expected to compatibly improve interfacial charge transport and desolvation kinetics. However, the relationship between physicochemical features and temperature-dependent kinetics properties of SEI remains vague. Herein, we propose four key thermodynamics parameters of SEI potentially influencing low-temperature electrochemistry, including electron work function, Li+ transfer barrier, surface energy, and desolvation energy. Based on the above parameters, we further define a novel descriptor, separation factor of SEI (SSEI), to quantitatively depict charge (Li+/e-) transport and solvent deprivation processes at Gr/electrolyte interface. A Li3PO4-based, inorganics-enriched SEI derived by Li difluorophosphate (LiDFP) additive exhibits the highest SSEI (4.89×103) to enable efficient Li+ conduction, e- blocking and rapid desolvation, and as a result, much suppressed Li-metal precipitation, electrolyte decomposition and Gr sheets exfoliation, thus improving low-temperature battery performances. Overall, our work originally provides visualized guides to improve low-temperature reaction kinetics/thermodynamics by constructing desirable SEI chemistry.

Interfacial Stabilization by Prelithiated Trithiocyanuric Acid as an Organic Additive in Sulfide-Based All-Solid-State Lithium Metal Batteries.

Sulfide-based all-solid-state battery (ASSB) with a lithium metal anode (LMA) is a promising candidate to surpass conventional Li-ion batteries owing to their inherent safety against fire hazards and potential to achieve a higher energy density. However, the narrow electrochemical stability window and chemical reactivity of the sulfide solid electrolyte towards the LMA results in interfacial degradation and poor electrochemical performance. In this direction, we introduce an organic additive approach, that is the mixing of prelithiated trithiocyanuric acid, Li3TCA, with Li6PS5Cl, to establish a stable interface while preserving high ionic conductivity. Including 2.5 wt % Li3TCA alleviates the decomposition of the electrolyte on the lithium metal interface, decreasing the Li2S content in the solid-electrolyte interface (SEI) thus forming a more stable interface. In Li|Li symmetric cells, this strategy enables a rise in the critical current density from 1.0 to 1.9 mA cm-2 and stable cycling for over 750 hours at a high current density of 1.0 mA cm-2. This approach also enables Li|NbO-NCM811 full cell to operate more than 500 cycles at 0.3 C.

Stable Lithium-Sulfur Batteries Ensured by GeS2 and α-S8 Lattice Matching During the Charge Process.

The charge process of lithium-sulfur batteries (LSBs) is a process in which molecular polarity decreases and the volume shrinks gradually, which is the process most likely to cause lithium polysulfides (LiPSs) loss and interfacial collapse. In this work, GeS2 is utilized, whose (111) lattice plane exactly matches with the (113) lattice of α-S8 , to solve these problems. GeS2 can regulate the interconversion-deposition behavior of S-species during the charge process. Soluble LiPSs can be spontaneously adsorbed on the GeS2 surface, then obtain electrons and eventually convert to α-S8 molecules. More importantly, the α-S8 molecules will crystallize uniformly along the (111) lattice plane of GeS2 to maintain a stable cathode-electrolyte interface. Therefore, outstanding charge/discharge LSBs are successfully accomplished.

In Situ Constructing Robust and Highly Conductive Solid Electrolyte with Tailored Interfacial Chemistry for Durable Li Metal Batteries.

Employing nanofiber framework for in situ polymerized solid-state lithium metal batteries (SSLMBs) is impeded by the insufficient Li+ transport properties and severe dendritic Li growth. Both critical issues originate from the shortage of Li+ conduction highways and nonuniform Li+ flux, as randomly-scattered nanofiber backbone is highly prone to slippage during battery assembly. Herein, a robust fabric of Li0.33 La0.56 Ce0.06 Ti0.94 O3-δ /polyacrylonitrile framework (p-LLCTO/PAN) with inbuilt Li+ transport channels and high interfacial Li+ flux is reported to manipulate the critical current density of SSLMBs. Upon the merits of defective LLCTO fillers, TFSI- confinement and linear alignment of Li+ conduction pathways are realized inside 1D p-LLCTO/PAN tunnels, enabling remarkable ionic conductivity of 1.21 mS cm-1 (26 °C) and tLi+ of 0.93 for in situ polymerized polyvinylene carbonate (PVC) electrolyte. Specifically, molecular reinforcement protocol on PAN framework further rearranges the Li+ highway distribution on Li metal and alters Li dendrite nucleation pattern, boosting a homogeneous Li deposition behavior with favorable SEI interface chemistry. Accordingly, excellent capacity retention of 76.7% over 1000 cycles at 2 C for Li||LiFePO4 battery and 76.2% over 500 cycles at 1 C for Li||LiNi0.5 Co0.2 Mn0.3 O2 battery are delivered by p-LLCTO/PAN/PVC electrolyte, presenting feasible route in overcoming the bottleneck of dendrite penetration in in situ polymerized SSLMBs.

Correlation between the Protein Pharmaceutical Surface Activity and Interfacial Stability.

The interaction of protein drugs with the air-liquid interface plays a crucial role in the overall stability in aqueous formulations, particularly when the adsorbed proteins are subjected to the surface flow. Nonionic surfactants are usually added into the formulation solutions to address this issue. A diversity of studies have been focused on the usage of surfactants, the stability mechanism of surfactants, or seeking new pharmaceutical surfactants. However, the real protagonist, the basic properties of protein drugs, was neglected, which may play a vital role in the stability of protein drugs. Herein, we aim to clarify the correlation between the surface behavior of proteins and the interfacial stability. A force tensiometer is used to track the surface tension reduction and the competition between surfactants and proteins at the surface. We find that the surface behaviors of proteins vary with storage temperature and protein types including monoclonal antibodies (mAb), bispecific monoclonal antibodies (BsAb), and antibody-drug conjugates (ADCs). Especially for the protein stored at 5 °C, the surface activity of proteins is better than that of surfactants. It indicates that the ability of proteins to adsorb at the interface should not be ignored compared to surfactants. The significant difference in the interfacial stability of protein pharmaceuticals formulated in the same buffer and excipients as well as the surfactants with the same concentration further confirms the interfacial adsorption capacity of proteins that should not be ignored. These findings provide a new angle and valuable insights into the correlation between the surface activity of the proteins and interfacial stability, which may pave the way for future preformulation studies on therapeutic proteins and broaden the thoughts of formulation development.

Structural properties of Phoenix oolong tea polysaccharide conjugates and the interfacial stability in nanoemulsions.

BACKGROUND: Tea polysaccharide conjugate (TPC) is a naturally occurring active substance that is extracted from tea. Owing to its benefits in enhancing human immunity and antioxidant effects, TPC is widely used in culinary products. The binding mode of polysaccharides and proteins in TPC, however, has not been well studied; it may be closely related to their functional properties, especially emulsification. RESULTS: The molecular weights and monosaccharide compositions of TPC were determined by ion chromatography and high-performance gel permeation chromatography. Although the functional groups of polysaccharides and proteins were confirmed by infrared spectroscopy, the presence of proteins could not be detected by sodium dodecyl sulfate polyacrylamide gel electrophoresis and ultraviolet spectroscopy. It was hypothesized that the hydrophobic groups of the proteins in TPC were wrapped by polysaccharide chains, thus making the proteins undetectable. The rheology and interfacial protein adsorption results show that TPC forms a viscoelastic film at the oil-water interface to prevent the aggregation of oil droplets, thereby enhancing the stability of the emulsion. Based on these structural and emulsifying properties of TPC, the binding mode of polysaccharides and proteins along with their phase behavior at the oil-water interface of the emulsion was speculated. CONCLUSION: In TPC, the hydrophilic groups of the proteins are linked to polysaccharides by covalent interactions, where the hydrophobic groups are wrapped with the polysaccharide chains with the help of hydrophobic forces to form a hydrophobic core. The unique binding of polysaccharides and proteins in TPC enhances its amphiphilic properties, which can be effectively distributed at the oil-water interface and form stable emulsions. © 2023 Society of Chemical Industry.

Interface Design Enabling Stable Polymer/Thiophosphate Electrolyte Separators for Dendrite-Free Lithium Metal Batteries.

Organic/inorganic interfaces greatly affect Li+ transport in composite solid electrolytes (SEs), while SE/electrode interfacial stability plays a critical role in the cycling performance of solid-state batteries (SSBs). However, incomplete understanding of interfacial (in)stability hinders the practical application of composite SEs in SSBs. Herein, chemical degradation between Li6 PS5 Cl (LPSCl) and poly(ethylene glycol) (PEG) is revealed. The high polarity of PEG changes the electronic state and structural bonding of the PS4 3- tetrahedra, thus triggering a series of side reactions. A substituted terminal group of PEG not only stabilizes the inner interfaces but also extends the electrochemical window of the composite SE. Moreover, a LiF-rich layer can effectively prevent side reactions at the Li/SE interface. The results provide insights into the chemical stability of polymer/sulfide composites and demonstrate an interface design to achieve dendrite-free lithium metal batteries.

Impact of the Chlorination of Lithium Argyrodites on the Electrolyte/Cathode Interface in Solid-State Batteries.

Lithium argyrodite-type electrolytes are regarded as promising electrolytes due to their high ionic conductivity and good processability. Chemical modifications to increase ionic conductivity have already been demonstrated, but the influence of these modifications on interfacial stability remains so far unknown. In this work, we study Li6 PS5 Cl and Li5.5 PS4.5 Cl1.5 to investigate the influence of halogenation on the electrochemical decomposition of the solid electrolyte and the chemical degradation mechanism at the cathode interface in depth. Electrochemical measurements, gas analysis and time-of-flight secondary ion mass spectrometry indicate that the Li5.5 PS4.5 Cl1.5 shows pronounced electrochemical decomposition at lower potentials. The chemical reaction at higher voltages leads to more gaseous degradation products, but a lower fraction of solid oxygenated phosphorous and sulfur species. This in turn leads to a decreased interfacial resistance and thus a higher cell performance.

Influencing Factors on Li-ion Conductivity and Interfacial Stability of Solid Polymer Electrolytes, Exampled by Polycarbonates, Polyoxalates and Polymalonates.

The application of solid polymer electrolytes (SPEs) in all-solid-state(ASS) batteries is hindered by lower Li+ -conductivity and narrower electrochemical window. Here, three families of ester-based F-modified SPEs of poly-carbonate (PCE), poly-oxalate (POE) and poly-malonate (PME) were investigated. The Li+ -conductivity of these SPEs prepared from pentanediol are all higher than the counterparts made of butanediol, owing to the enhanced asymmetry and flexibility. Because of stronger chelating coordination with Li+ , the Li+ -conductivity of PME and POE is around 10 and 5 times of PCE. The trifluoroacetyl-units are observed more effective than -O-CH2 -CF2 -CF2 -CH2 -O- during the in situ passivation of Li-metal. Using trifluoroacetyl terminated POE and PCE as SPE, the interfaces with Li-metal and high-voltage-cathode are stabilized simultaneously, endowing stable cycling of ASS Li/LiNi0.6 Co0.2 Mn0.2 O2 (NCM622) cells. Owing to an enol isomerization of malonate, the cycling stability of Li/PME/NCM622 is deteriorated, which is recovered with the introduce of dimethyl-group in malonate and the suppression of enol isomerization. The coordinating capability with Li+ , molecular asymmetry and existing modes of elemental F, are all critical for the molecular design of SPEs.

Progress in Solid Polymer Electrolytes for Lithium-Ion Batteries and Beyond.

Solid-state polymer electrolytes (SPEs) for high electrochemical performance lithium-ion batteries have received considerable attention due to their unique characteristics; they are not prone to leakage, and they exhibit low flammability, excellent processability, good flexibility, high safety levels, and superior thermal stability. However, current SPEs are far from commercialization, mainly due to the low ionic conductivity, low Li+ transference number (tLi+ ), poor electrode/electrolyte interface contact, narrow electrochemical oxidation window, and poor long-term stability of Li metal. Recent work on improving electrochemical performance and these aspects of SPEs are summarized systematically here with a particular focus on the underlying mechanisms, and the improvement strategies are also proposed. This review could lead to a deeper consideration of the issues and solutions affecting the application of SPEs and pave a new pathway to safe, high-performance lithium-ion batteries.

Surface Potential Regulation Realizing Stable Sodium/Na3 Zr2 Si2 PO12 Interface for Room-Temperature Sodium Metal Batteries.

Inorganic Na3 Zr2 Si2 PO12 is prospective with a high ionic conductivity but suffers large interfacial resistance and stability issues against sodium metal, hindering its practical application in all-solid-state sodium batteries. A surface potential regulation strategy is adopted to address these issues. Na3 Zr2 Si2 PO12 (NZSP) ceramic with homogeneously-sintered surface is synthesized by a simple two-step sintering method to promote its uniform surface potential, which is favorable for mitigating the potential fluctuations at the interface against Na metal and enhancing interfacial compatibility. The Na/NZSP interface can be stabilized for over 4 months with a low interfacial resistance of 129 Ω cm2 at 25 °C. The symmetrical Na/NZSP/Na cell exhibits ultra-stable sodium platting/stripping cycling for over 1000 cycles under 0.1 mA cm-2 . Superior interfacial performance is well retained even under 0.2 mA cm-2 at room temperature. The robust interface is further signified by its excellence under higher current densities of up to 0.85 mA cm-2 at 60 °C. A 4 V all-solid-state Na3 V1.5 Cr0.5 (PO4 )3 /NZSP/Na metal battery is demonstrated at ambient conditions, which exhibits superior rate capability and delivers a high reversible capacity of 103 mA h g-1 under 100 mA g-1 for over 400 cycles with a Coulombic efficiency of over 99%.

Single-Crystal-Layered Ni-Rich Oxide Modified by Phosphate Coating Boosting Interfacial Stability of Li10 SnP2 S12 -Based All-Solid-State Li Batteries.

All-solid-state lithium batteries (ASSLBs) adopting sulfide electrolytes and high-voltage layered oxide cathodes have moved into the mainstream owing to their superior safety and immense potential in high energy density. However, the poor electrochemical compatibility between oxide cathodes and sulfide electrolytes remains a challenge for high-performance ASSLBs. In this study, a nanoscale Li1.4 Al0.4 Ti1.6 (PO4 )3 (LATP) phosphate coating is reasonably constructed on the surface of single-crystal LiNi0.6 Co0.2 Mn0.2 O2 particles to achieve cathode/electrolyte interfacial stability. The conformal LATP layer with inherent high-voltage stability can effectively suppress the oxidation decomposition of the electrolyte and demonstrate chemical inertness to both the oxide cathode and Li10 SnP2 S12 electrolyte. ASSLBs with an LATP-modified cathode exhibited a high initial discharge capacity (152.1 mAh g-1 ), acceptable rate capability, and superior cycling performance with a capacity retention of 87.6% after 100 cycles at 0.1 C. Interfacial modification is an effective approach for achieving high-performance sulfide-based ASSLBs with superior interfacial stability.

Simultaneous Enhancement of Interfacial Stability and Kinetics of Single-Crystal LiNi0.6Mn0.2Co0.2O2 through Optimized Surface Coating and Doping.

Balancing interfacial stability and Li+ transfer kinetics through surface engineering is a key challenge in developing high-performance battery materials. Although conformal coating enabled by atomic layer deposition (ALD) has shown great promise in controlling impedance increase upon cycling by minimizing side reactions at the electrode-electrolyte interface, the coating layer itself usually exhibits poor Li+ conductivity and impedes surface charge transfer. In this work, we have shown that by carefully controlling postannealing temperature of an ultrathin ZrO2 film prepared by ALD, Zr4+ surface doping could be achieved for Ni-rich layered oxides to accelerate the charge transfer yet provide sufficient protection. Using single-crystal LiNi0.6Mn0.2Co0.2O2 as a model material, we have shown that surface Zr4+ doping combined with ZrO2 coating can enhance both the cycle performance and rate capability during high-voltage operation. Surface doping via controllable postannealing of ALD surface coating layer reveals an attractive path toward developing stable and Li+-conductive interfaces for single-crystal battery materials.

Enabling a Durable Electrochemical Interface via an Artificial Amorphous Cathode Electrolyte Interphase for Hybrid Solid/Liquid Lithium-Metal Batteries.

A hybrid solid/liquid electrolyte with superior security facilitates the implementation of high-energy-density storage devices, but it suffers from inferior chemical compatibility with cathodes. Herein, an optimal lithium difluoro(oxalato)borate salt was introduced to build in situ an amorphous cathode electrolyte interphase (CEI) between Ni-rich cathodes and hybrid electrolyte. The CEI preserves the surface structure with high compatibility, leading to enhanced interfacial stability. Meanwhile, the space-charge layer can be prominently mitigated at the solid/solid interface via harmonized chemical potentials, acquiring promoted interfacial dynamics as revealed by COMSOL simulation. Consequently, the amorphous CEI integrates the bifunctionality to provide an excellent cycling stability, high Coulombic efficiency, and favorable rate capability in high-voltage Li-metal batteries, innovating the design philosophy of functional CEI strategy for future high-energy-density batteries.

Graphitic Hollow Nanocarbon as a Promising Conducting Agent for Solid-State Lithium Batteries.

All-solid-state batteries (ASSBs) have lately received enormous attention for electric vehicle applications because of their exceptional stability by engaging all-solidified cell components. However, there are many formidable hurdles such as low ionic conductivity, interface instability, and difficulty in the manufacturing process, for its practical use. Recently, carbon, one of the representative conducting agents, turns out to largely participate in side reactions with the solid electrolyte, which finally leads to the formation of insulating side products at the interface. Although the battery community mentioned that parasitic reactions are presumably attributed to carbon itself or the generation of electronic conducting paths lowering the kinetic barrier for reactions, the underlying origin for such reactions as well as appropriate solutions have not been provided yet. In this study, for the first time, it is verified that the functional group on carbon is an origin for causing negative effects on interfacial stability and a graphitized hollow nanocarbon as a promising solution for improving-electrochemical performance is introduced. This work offers an invaluable lesson that a relatively minor part, such as a conducting agent, in ASSBs sometimes gives more positive impact on improving electrochemical performance than huge efforts for resolving other parts.

An Ultrahigh Modulus Gel Electrolytes Reforming the Growing Pattern of Li Dendrites for Interfacially Stable Lithium-Metal Batteries.

Gel polymer electrolytes (GPEs) have aroused intensive attention for their moderate comprehensive performances in lithium-metal batteries (LMBs). However, GPEs with low elastic moduli of MPa magnitude cannot mechanically regulate the Li deposition, leading to recalcitrant lithium dendrites. Herein, a porous Li7 La3 Zr2 O12 (LLZO) framework (PLF) is employed as an integrated solid filler to address the intrinsic drawback of GPEs. With the incorporation of PLF, the composite GPE exhibits an ultrahigh elastic modulus of GPa magnitude, confronting Li dendrites at a mechanical level and realizing steady polarization at high current densities in Li||Li cells. Benefiting from the compatible interface with anodes, the LFP|PLF@GPE|Li cells deliver excellent rate capability and cycling performance at room temperature. Theoretical models extracted from the topology of solid fillers reveal that the PLF with unique 3D structures can effectively reinforce the gel phase of GPEs at the nanoscale via providing sufficient mechanical support from the load-sensitive direction. Numerical models are further developed to reproduce the multiphysical procedure of dendrite propagation and give insights into predicting the failure modes of LMBs. This work quantitatively clarifies the relationship between the topology of solid fillers and the interface stability of GPEs, providing guidelines for designing mechanically reliable GPEs for LMBs.