Electrolytes For Lithium Metal Batteries Research Articles

Full gradient compensation of LiNO3 in the suspension electrolyte for lithium metal batteries

Uncontrolled side reactions between lithium metal and organic electrolytes seriously deteriorates the stability of corresponding battery due to the non-uniform Li+ deposition. Using lithium nitrate (LiNO3) as an additive can adjust the components in solid-electrolyte-interphase (SEI) for optimizing of lithium metal interface. However, the low solubility and rapid consumption of LiNO3 in ester-based electrolytes limit its further application. Herein, a kind of suspension electrolyte containing micron-sized LiNO3 particles is reported to realize a full gradient compensation against the consumption of NO3−. Benefiting from the uniformly dispersion of LiNO3 particles, a SEI layer containing even-distributed Li3N and LiNxOy with high content is constructed that promotes the rapid and uniform plating of Li+. Consequently, the Li/Cu batteries present a polarization of only 15–20 mV, and exhibit a consistent performance for 230 cycles with the CE of 98.1%, which is 4 times than that of conventional carbonate electrolytes. In addition, the cycling life of the assembled Li/NCM811 batteries can be extended to 260 cycles with a high capacity retention of 82.4 %.

Synergistic effect of Ti3C2Tx MXene/PAN nanofiber and LLZTO particles on high-performance PEO-based solid electrolyte for lithium metal battery

Solid polymer electrolytes (SPEs) have been considered the most promising separators for all-solid-state lithium metal batteries (ASSLMBs) due to their ease of processing and low cost. However, the practical applications of SPEs in ASSLMBs are limited by their low ionic conductivities and mechanical strength. Herein, we developed a three-dimensional (3D) interconnected MXene (Ti3C2Tx) network and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) particles synergistically reinforced polyethylene oxide (PEO)-based SPE, where the association of Li+ with ether-oxygen in PEO could be significantly weakened through the Lewis acid-base interactions between the electron-absorbing group (Ti–F, −O–) of Ti3C2Tx and Li+. Besides, the TFSI− in lithium salts could be immobilized by hydrogen bonds from the Ti–OH of Ti3C2Tx. The 3D interconnected Ti3C2Tx network not only alleviated the agglomeration of inorganic fillers (LLZTO), but also improved the mechanical strength of composite solid electrolyte (CSE). Consequently, the assembled Li||CSE||Li symmetric battery showed excellent cycling stability at 35 ℃ (stable cycling over 3000 h at 0.1 mA cm−2, 0.1 mAh cm−2) and −2 ℃ (stable cycling over 2500 h at 0.05 mA cm−2, 0.05 mAh cm−2). Impressively, the LiFePO4||CSE||Li battery showed a high discharge capacity of 145.3 mAh/g at 0.3 C after 300 cycles at 35 ℃. This rational structural design provided a new strategy for the preparation of high-performance solid-state electrolytes for lithium metal batteries.

Anion‐Derived Solid Electrolyte Interphase Enabled by Diluent Modulated Dimethyl Carbonate‐Based Localized High Concentration Electrolytes for Lithium Metal Batteries

Carbonate‐based electrolytes generally suffer from low Coulombic efficiency and poor cycling stability in lithium metal batteries. In this work, localized high concentration electrolytes (LHCEs) based on dimethyl carbonate (DMC) with varying diluent additions are designed. LHCEs demonstrate higher Li+ transference numbers and a greater proportion of contact ion pairs (CIPs) and ion pair aggregates (AGGs) in the solvation structures, facilitating the formation of anion‐derived solid electrolyte interphase (SEI). Furthermore, LHCEs enhance the Coulombic efficiency of Li||Cu cells and improve the anodic stability against lithium. One of these LHCEs, prepared with appropriate diluent addition, exhibits excellent capacity retention in Li||NCM622 cells at 0.5 C after 150 cycles, thus presenting promising possibilities for the development of high energy density lithium metal batteries.

Rational Lithium Salt Molecule Tuning for Fast Charging/Discharging Lithium Metal Battery.

The electrolytes for lithium metal batteries (LMBs) are plagued by a low Li+ transference number (T+) of conventional lithium salts and inability to form a stable solid electrolyte interphase (SEI). Here, we synthesized a self-folded lithium salt, lithium 2-[2-(2-methoxy ethoxy)ethoxy]ethanesulfonyl(trifluoromethanesulfonyl) imide (LiETFSI), and comparatively studied with its structure analogue, lithium 1,1,1-trifluoro-N-[2-[2-(2-methoxyethoxy)ethoxy)]ethyl]methanesulfonamide (LiFEA). The special anion chemistry imparts the following new characteristics: i) In both LiFEA and LiETFSI, the ethylene oxide moiety efficiently captures Li+, resulting in a self-folded structure and high T+ around 0.8. ii) For LiFEA, a Li-N bond (2.069 Å) is revealed by single crystal X-ray diffraction, indicating that the FEA anion possesses a high donor number (DN) and thus an intensive interphase "self-cleaning" function for an ultra-thin and compact SEI. iii) Starting from LiFEA, an electron-withdrawing sulfone group is introduced near the N atom. The distance of Li-N is tuned from 2.069 Å in LiFEA to 4.367 Å in LiETFSI. This alteration enhances ionic separation, achieves a more balanced DN, and tunes the self-cleaning intensity for a reinforced SEI. Consequently, the fast charging/discharging capability of LMBs is progressively improved. This rationally tuned anion chemistry reshapes the interactions among Li+, anions, and solvents, presenting new prospects for advanced LMBs.

Rational Lithium Salt Molecule Tuning for Fast Charging/Discharging Lithium Metal Battery

AbstractThe electrolytes for lithium metal batteries (LMBs) are plagued by a low Li+ transference number (T+) of conventional lithium salts and inability to form a stable solid electrolyte interphase (SEI). Here, we synthesized a self‐folded lithium salt, lithium 2‐[2‐(2‐methoxy ethoxy)ethoxy]ethanesulfonyl(trifluoromethanesulfonyl) imide (LiETFSI), and comparatively studied with its structure analogue, lithium 1,1,1‐trifluoro‐N‐[2‐[2‐(2‐methoxyethoxy)ethoxy)]ethyl]methanesulfonamide (LiFEA). The special anion chemistry imparts the following new characteristics: i) In both LiFEA and LiETFSI, the ethylene oxide moiety efficiently captures Li+, resulting in a self‐folded structure and high T+ around 0.8. ii) For LiFEA, a Li−N bond (2.069 Å) is revealed by single crystal X‐ray diffraction, indicating that the FEA anion possesses a high donor number (DN) and thus an intensive interphase “self‐cleaning” function for an ultra‐thin and compact SEI. iii) Starting from LiFEA, an electron‐withdrawing sulfone group is introduced near the N atom. The distance of Li−N is tuned from 2.069 Å in LiFEA to 4.367 Å in LiETFSI. This alteration enhances ionic separation, achieves a more balanced DN, and tunes the self‐cleaning intensity for a reinforced SEI. Consequently, the fast charging/discharging capability of LMBs is progressively improved. This rationally tuned anion chemistry reshapes the interactions among Li+, anions, and solvents, presenting new prospects for advanced LMBs.

Ionic liquid-based self-healing gel electrolyte for high-performance lithium metal batteries

The gel electrolytes with self-healing function are being considered as promising replacement for traditional liquid electrolytes in lithium metal batteries due to their excellent battery safety, high energy density and minimum electrolyte damage. However, balancing self-healing, conductivity and mechanical properties remains a challenge for their practical application. Herein, a new ion liquid-based self-healing gel polymer electrolyte (IL-SHGPE) is introduced. The electrolyte was synthesized via UV-induced cross-linking of a polymer containing quadruple hydrogen bond units and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BMIM-TFSI) ion liquid. The resultant IL-SHGPE demonstrates exceptional self-healing ability (with 95% healing efficiency within 30 min), excellent thermal stability over a wide temperature range up to 410 °C. It also exhibits impressive mechanical strength with 41.3% elongation and 1.9 MPa tensile stress, room temperature ionic conductivity of 1.29 × 10−3 S/cm, and a wide electrochemical stability window of 5.18V (vs Li/Li+). Lithium metal batteries with this electrolyte showed an initial discharge capacity of 139 mAh g−1 at 1C rate, and a capacity retention of 88.3% after 200 cycles. Therefore, this work provides a significant exploration for balancing self-healing ability, mechanical attributes, and electrochemical performance of lithium batteries, and thus contributing valuable insights towards the development of high-performance self-healing gel electrolytes for lithium metal batteries.

Transesterification Induced Multifunctional Additives Enable High‐Performance Lithium Metal Batteries

AbstractThe electrolyte chemistry is crucially important for promoting the practical application of lithium metal batteries (LMBs). Here, we demonstrate for the first time that 1,3‐dimethylimidazolium dimethyl phosphate (DIDP) and trimethylsilyl trifluoroacetate (TMSF) can undergo in situ transesterification in carbonate electrolyte to generate dimethyl trimethylsilyl phosphate (DTMSP) and 1,3‐dimethylimidazolium trifluoroacetate (DITFA) as multifunctional additives for LMBs. H2O and HF can be removed by the Si−O group in DTMSP to improve the moisture resistance of electrolyte and the stability of cathode. Furthermore, the dissolution of lithium nitrate (LiNO3) in carbonate electrolyte can be promoted by the trifluoroacetate anion (TFA−) in DITFA, thereby optimizing the solvation structure and transport kinetics of Li+. More importantly, both DTMSP and DITFA tend to preferential redox decomposition due to the low lowest unoccupied molecular orbital (LUMO) and high highest occupied molecular orbital (HOMO). Consequently, a thin and robust layer rich in P/N/Si on the cathode and an inorganic‐rich layer (e.g. Li3N/Li3P) on the anode can be constructed and superior electrochemical performances are achieved. This artificial transesterification strategy to introduce favorable additives paves an efficient and ingenious route to high‐performance electrolyte for LMBs.

Reevaluate low-concentration ether-based electrolytes for lithium metal batteries

Ether is regarded as an exceptional solvent in liquid electrolytes for lithium (Li) metal batteries due to its outstanding compatibility with Li metal anode. Low salt concentration in ether-based electrolytes (LCEEs) is highly favorable to reducing the cost of future Li metal batteries. Nevertheless, LCEEs have been reported to exhibit poor anodic stability (as low as 4.0 V vs. Li/Li+), therefore considered unsuitable for practical batteries using LiNixMnyCozO2 as cathodes and charge up to 4.4 V. Here, using 1.0 M lithium bis(fluorosulfonyl)imide (LiFSI) in 1,2-dimethoxyethane (DME) as the baseline, we demonstrate the intrinsic anodic stability window of LCEE to be above 4.5 V. We revealed the true failure mechanism of LCEE to be various electrochemical reactions with different working electrodes (WEs). We further provide electrolyte and electrode design rules to prevent LCEE decomposition, as well as electrode and packaging materials corrosion at high voltage. This study highlights the importance of previously overlooked battery component compatibility in electrolyte development and offers valuable insights into battery engineering considerations toward high-energy and cost-effective Li metal batteries.

Highly Conductive Imidazolate Covalent Organic Frameworks with Ether Chains as Solid Electrolytes for Lithium Metal Batteries.

Poly(ethylene oxide) (PEO)-based electrolytes are often used for Li+ conduction as they can dissociate the Li salts efficiently. However, high entanglement of the chains and lack of pathways for rapid ion diffusion limit their applications in advanced batteries. Recent developments in ionic covalent organic frameworks (iCOFs) showed that their highly ordered structures provide efficient pathways for Li+ transport, solving the limitations of traditional PEO-based electrolytes. Here, we present imidazolate COFs, PI-TMEFB-COFs, having methoxyethoxy chains, synthesized by Debus-Radziszewski multicomponent reactions and their ionized form, Li+ @PI-TMEFB-COFs, showing a high Li+ conductivity of 8.81 mS cm-1 and a transference number of 0.974. The mechanism for such excellent electrochemical properties is that methoxyethoxy chains dissociate LiClO4 , making free Li+ , then those Li+ are transported through the imidazolate COFs' pores. The synthesized Li+ @PI-TMEFB-COFs formed a stable interface with Li metal. Thus, employing Li+ @PI-TMEFB-COFs as the solid electrolyte to assemble LiFePO4 batteries showed an initial discharge capacity of 119.2 mAh g-1 at 0.5 C, and 82.0 % capacity and 99.9 % Coulombic efficiency were maintained after 400 cycles. These results show that iCOFs with ether chains synthesized via multicomponent reactions can create a new chapter for making solid electrolytes for advanced rechargeable batteries.

Highly Conductive Imidazolate Covalent Organic Frameworks with Ether Chains as Solid Electrolytes for Lithium Metal Batteries

AbstractPoly(ethylene oxide) (PEO)‐based electrolytes are often used for Li+ conduction as they can dissociate the Li salts efficiently. However, high entanglement of the chains and lack of pathways for rapid ion diffusion limit their applications in advanced batteries. Recent developments in ionic covalent organic frameworks (iCOFs) showed that their highly ordered structures provide efficient pathways for Li+ transport, solving the limitations of traditional PEO‐based electrolytes. Here, we present imidazolate COFs, PI‐TMEFB‐COFs, having methoxyethoxy chains, synthesized by Debus–Radziszewski multicomponent reactions and their ionized form, Li+@PI‐TMEFB‐COFs, showing a high Li+ conductivity of 8.81 mS cm−1 and a transference number of 0.974. The mechanism for such excellent electrochemical properties is that methoxyethoxy chains dissociate LiClO4, making free Li+, then those Li+ are transported through the imidazolate COFs’ pores. The synthesized Li+@PI‐TMEFB‐COFs formed a stable interface with Li metal. Thus, employing Li+@PI‐TMEFB‐COFs as the solid electrolyte to assemble LiFePO4 batteries showed an initial discharge capacity of 119.2 mAh g−1 at 0.5 C, and 82.0 % capacity and 99.9 % Coulombic efficiency were maintained after 400 cycles. These results show that iCOFs with ether chains synthesized via multicomponent reactions can create a new chapter for making solid electrolytes for advanced rechargeable batteries.

Low-cost and high-safety montmorillonite-based solid electrolyte for lithium metal batteries

Composite solid-state electrolyte have good interfacial compatibility and mechanical properties, but their safety (such as easy to catch fire) and economic cost are still problems. In present work, an composite solid-state electrolyte was prepared by inserting poly(vinylidene fluoride)-based polymer electrolyte matrix into the interlayer of a low cost clay mineral-montmorillonite. The composite electrolyte exhibited remarkable characteristics, including excellent flame retardancy, high room temperature ionic conductivity of 2.28 × 10−4 S cm−1, wide electrochemical stability window of 4.8 V, high lithium-ion transference number of 0.57 and good mechanical strength of 12.58 MPa. Furthermore, LiFePO4-based solid-state battery, utilizing this composite solid-state electrolyte, exhibited stable cycling with discharge specific capacity of 130 mAh g−1 for over 100 cycles at a rate of 0.5C at room temperature. This successful performance demonstrated the potential of utilizing low-cost and environmentally friendly raw clay mineral materials in high energy density solid-state battery applications.

Highly liquid retentive, ordered ion transport quasi-solid polymer electrolytes for lithium metal batteries

Solid-state lithium metal batteries (SSLMB) offer a compelling solution to address the low energy density issue present in current liquid lithium-ion batteries (LIB). Nevertheless, SSLMB electrolytes continue to face specific challenges that impede their commercial viability. These challenges encompass low ionic conductivity, high production cost, instability of interfacial contact, and other hurdles. In this context, a cost-effective quasi-solid polymer electrolyte (QPE) based on Polyvinylidene fluoride (PVDF) was developed to reshape the transport of lithium-ion (Li+) within the electrolyte, resulting in accelerated Li+ transport, with an achieved ionic conductivity of 0.71 mS cm−1 at 25 °C. The assembled LiFePO4|PVDF-OH|Li cell demonstrates exceptional battery performance, boasting an initial capacity of 145.9 mAh/g at 30 °C and maintaining an impressive capacity retention of 85.4 % even after 1000 cycles. The experimental findings underscore the critical role played by the immobilized solvent within the innovative PVDF-based QPE in facilitating the migration of Li+, consequently enhancing electrochemical performance. This study showcases a pioneering approach aimed at enhancing ionic conductivity, representing a significant stride towards the development of low-cost, high-performance, and easily processable solid polymer electrolytes, with potential implications for broader research in the field of energy storage systems.

Perfluorosulfonic Acid Membranes as Gel-Polymer Electrolytes for Lithium Metal Batteries

Perfluorosulfonic Acid Membranes as Gel-Polymer Electrolytes for Lithium Metal Batteries

Construction of high-performance solid-state electrolytes for lithium metal batteries by UV-curing technology

With high energy density and high safety, all-solid-state lithium metal batteries (ASSLMBs) are considered the most competitive next-generation energy storage batteries. In this work, different formulations of PEGDA-based solid-state electrolytes were prepared by solution flow casting and UV-irradiated in situ polymerization. Polyethylene oxide (PEO) was introduced to solve the problem of improving the flexibility of the substrate, and a 1:5 mass ratio between them was determined. Inorganic ceramic filler Li1.25Al0.25Zr1.75(PO4)3 (LAZP) and plasticizer butanedinitrile (SCN) were introduced to improve the ionic conductivity (σ) of the electrolyte. The best performing PP15-30-SCN sample showed a 40-fold improvement in room temperature ionic conductivity over PEGDA and lithium ion mobility number of 0.43. The ASSLMBs were assembled with composite electrolytes and tested at 60 °C. The polarization of PP15-30-SCN was significantly reduced, and the battery cycled stably at current densities from 0.1 to 2 C, with an average discharge specific capacity of 111.78 mAh g−1 at 1C. The average specific capacity at 1C was 111.78 mAh g−1. Meanwhile, the capacity retention rate was more than 99% after more than 70 long cycles at 0.5C.

Directing Fluorinated Solid Electrolyte Interphase by Solubilizing Crystal Lithium Fluoride in Aprotic Electrolyte for Lithium Metal Batteries

AbstractLithium fluoride (LiF) facilitates robust and fast‐ion‐transport solid electrolyte interphase (SEI) in lithium metal batteries. Fluorinated solvents/salts are ubiquitously employed to introduce LiF into SEI through electrochemical decomposition, but this approach is usually at the expense of their continuous consumption. A direct approach to fluorinate SEI that employs crystal LiF is limited by its poor solubility in the current battery electrolyte formulation. Dissolving crystal LiF in high‐dielectric‐constant solvents, like ethylene carbonate (EC) is nearly neglected. Herein, the feasibility of directly fluorinating SEI by the addition of crystal LiF in aprotic electrolyte with the assistance of EC is verified, and its mechanisms in fluorination of SEI and anti‐acidification of electrolyte are explored. The dissolved LiF is encapsulated by solvent‐/salt‐derived organic skins to promote the fluorinated SEI. Meanwhile, the presence of LiF in electrolyte alters hazardous thermodynamic equilibrium, suppressing the production of acid species to mitigate electrolyte acidification and SEI degradation. Such collective benefits yield a capacity retention ratio of ≈88% after 150 cycles at a high areal capacity (4.5 mAh cm−2) in Li||NCM622 cells. This facile and effective fluorination of SEI contributes to an in‐depth understanding of SEI formation and rational design of well‐performing lithium metal batteries.

Host–Guest Interactions and Transport Mechanism in Poly(vinylidene fluoride)-Based Quasi-Solid Electrolytes for Lithium Metal Batteries

Host–Guest Interactions and Transport Mechanism in Poly(vinylidene fluoride)-Based Quasi-Solid Electrolytes for Lithium Metal Batteries

All-Polymer Nanocomposite as Salt-Free Solid Electrolyte for Lithium Metal Batteries.

Solid polymer electrolytes that combine both a high lithium-ion transference number and mechanical properties at high temperatures are searched for improving the performance of batteries. Here, we show a salt-free all-polymer nanocomposite solid electrolyte for lithium metal batteries that improves the mechanical properties and shows a high lithium-ion transference number. For this purpose, lithium sulfonamide-functionalized poly(methyl methacrylate) nanoparticles (LiNPs) of very small size (20-30 nm) were mixed with poly(ethylene oxide) (PEO). The morphology of all-polymer nanocomposites was first investigated by transmission electron microscopy (TEM), showing a good distribution of nanoparticles (NPs) even at high contents (50 LiNP wt %). The crystallinity of PEO was investigated in detail and decreased with the increasing concentration of LiNPs. The highest ionic conductivity value for the PEO 50 wt % LiNP nanocomposite at 80 °C is 1.1 × 10-5 S cm-1, showing a lithium-ion transference number of 0.68. Using dynamic mechanic thermal analysis (DMTA), it was shown that LiNPs strengthen PEO, and a modulus of ≈108 Pa was obtained at 80 °C for the polymer nanocomposite. The nanocomposite solid electrolyte was stable with respect to lithium in a Li||Li symmetrical cell for 1000 h. In addition, in a full solid-state battery using LiFePO4 as the cathode and lithium metal as the anode, a specific capacity of 150 mAhg-1 with a current density of 0.05 mA cm-2 was achieved.

SnCl4 initiated formation of polymerized solid polymer electrolytes for lithium metal batteries with fast ion transport interfaces

Solid-polymer-electrolytes (SPEs) are under active consideration for their high-energy and safe electrochemical energy storage. However, conventional polymer electrolytes are facing poor electrolyte/electrode interfacial contact and undesired lithium dendrite problems. Here, we report a polymerized-dioxolane (P-DOL) electrolytes created by in situ polymerization of DOL in the presence of tin tetrachloride (SnCl4), which enables ultra-conformal interfacial contact with all cell components. More importantly, SnCl4 plays a dual function by initiating ring-opening polymerization of DOL and simultaneously forming a LiCl/LixSn-based alloy composite protective layer on Li metal anodes. The robust Li-rich ion conductive alloys coupled with an electronically insulating surface component form fast ion transport channels. Using the SnCl4-initiated P-DOL SPEs exhibits a high ionic conductivity (>2 mS cm−1) and a wide electrochemical window (4.7 V) at room temperature. Applications of P-DOL SPEs in Li/Li symmetric and Li/LiFePO4 batteries further demonstrate low polarization and high capacity retention. This work provides a facile and practical approach to designing P-DOL SPEs for high-performance lithium metal batteries.

Unveiling decaying mechanism of non-flammable all-fluorinated carbonate electrolytes in lithium metal batteries with 4.6-V LiCoO2 cathodes at elevated temperatures

Highly fluorinated electrolytes have attracted much attention in lithium metal batteries (LMBs) because of their unique properties, such as increased anodic stability and altered coordination state of Li+ ions. However, the complex decaying mechanism of fluorinated electrolytes at elevated temperatures is not well understood, which is essential to assess their suitability for practical applications in harsh environments. Herein the influence of elevated temperatures on the stability of fluorinated electrolytes and the formation of interphases between the 4.6-V LiCoO2 cathode and electrolyte are systematically investigated. The results reveal that elevated temperatures significantly affect the stability of the electrolyte and the formation of interphases. In particular, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether undergoes decomposition catalyzed by reactive oxygen from the delithiated cathode at high temperatures and 4.6 V. Meanwhile, the degradation of fluorinated electrolytes is primarily caused by the temperature-induced decomposition of fluoroethylene carbonate. Although methyl (2,2,2-trifluoroethyl) carbonate has the highest stability among the solvents in this fluorinated system, it still experiences degradation in harsh environments. These findings highlight the importance of considering highly fluorinated ethers and the synergistic effects between fluorinated carbonate solvents, lithium salts, and solvation structures when designing fluorinated electrolytes, especially for applications at elevated temperatures. This work sheds light on the design and optimization of highly fluorinated electrolytes, enabling the development of 4.6-V LiCoO2-based LMBs capable of withstanding challenging environments and operating conditions.

Interconnected Three-Dimensional Porous Alginate-Based Gel Electrolytes for Lithium Metal Batteries.

Lithium batteries have been widely used in our daily lives for their high energy density and long-term stability. However, their safety problems are of paramount concern for consumers, which restricts their scale applications. Gel polymer electrolytes (GPEs) compensate for the defects of liquid leakage and lower ionic conductivity of solid electrolytes, which have attracted a lot of attention. Herein, a 3D interconnected highly porous structural gel electrolyte was prepared with alginate dressing as a host material, poly(ethylene oxide) (PEO), and a commercial liquid electrolyte. With rich polar functional groups and (CH2-CH2-O) segments on the polymer matrix, the transportation of Li+ is faster and uniform; thus, the formations of lithium dendrite were significantly inhibited. The cycle stability of symmetrical Li||Li batteries with modified composite electrolytes (SAA) is greatly improved, and the overpotential remains stable after more than 1000 h. Meanwhile, under the same conditions, the cycle performance of batteries with unmodified electrolytes is inferior and overpotentials are nearly 1 V after 100 h. Additionally, the capacity retention of Li||LiFePO4 with SAA is more than 95% after 200 cycles, while those of the others declined sharply. The alginate dressing-based GPEs can greatly enhance the mechanical and thermal stability of PEO-based GPEs, which provides an environmentally friendly avenue for gel electrolytes' applications in lithium batteries.