Biomimetic Channels Design in Metal-Organic Framework Enabling Highly Lithium-Ion Conduction for Lithium-Metal Batteries.

Solid-state electrolytes (SSEs) based on metal-organic frameworks (MOFs) are an ideal material for constructing high-performance lithium metal batteries (LMBs). However, the low ion conductivity and poor interface contact (especially at low temperatures) still seriously hinder its further application. Herein, inspired by the Na+/K+ conduction in biology systems, a series (NH2, OH, NH-(CH2)3-SO3H)-modified MIL-53-X as SSEs is reported. These functional groups are similar to anions suspended in biological ion channels, partially repelling anions while allowing cations to be effectively transported through pore channels. Subsequently, MIL-53-X with hierarchical pore structure (H-MIL-53-X) is obtained by introducing lauric acid as a regulator, and then the effects of structural design and morphology control on its performance are explored. The conductivity of H-MIL-53-NH-SO3Li with multi-level pore structure and modified by sulfonic acid groups reached 2.2 × 10-3 S cm-1 at 25 °C, lithium-ion transference number of 0.78. Besides, the H-MIL-53-NH-SO3Li still has an excellent conductivity of 10-4 S cm-1 at -40 °C. Additionally, LiFePO4/Li batteries equipped with H-MIL-53-NH-SO3Li SSEs could operate stably for over 200 cycles at 0.1 C. The strategy of combining structural and morphological design of MOFs with biomimetic ion channels opens new avenues for the design of high-performance SSEs.

Dual-Interphase-Stabilizing Sulfolane-Based Electrolytes for High-Voltage and High-Safety Lithium Metal Batteries.

High-voltage Li metal battery (HV-LMB) is one of the most promising energy storage technologies to achieve ultrahigh energy density. Nevertheless, electrolytes reported to date are difficult to simultaneously stabilize the Li metal anode and high-voltage cathode, especially without the assistance of expensive and corrosive high-concentration Li salts. Herein, a dual-interphase-stabilizing (DIS) and safe electrolyte that bypasses the high-concentration Li salt is reported. The electrolyte consists of high-flash-point sulfolane as solvent, molecular-orbital-engineered additives that enable stable B-F rich cathodic interphase, and unique C-F rich organic anodic interphase. The stable cycling of both Li metal anode and 4.75 V-LiCoO2 cathode in the DIS electrolyte (> 500 cycles) is demonstrated. HV-LMB pouch cells of a high energy density (435 Wh kg-1) can sustainably operate for more than 100 cycles. Moreover, the low cost and high thermal stability of the DIS electrolyte offer superior cost-effectiveness and safety for large-scale applications of HV-LMBs in the future.

Water and Electrolyte Content in Hypertension in the Skin (WHYSKI) in Primary Aldosteronism.

BACKGROUND: Primary aldosteronism (PA), the most common curable salt-dependent form of arterial hypertension, features renal K+ loss and enhanced Na+ reabsorption. We investigated whether the electrolyte, water, and TonEBP (tonicity-responsive enhancer binding protein)/NFAT5 (nuclear factor of activated T cells 5) content is altered in the skin of patients with PA and corrected by surgical cure. METHODS: We obtained skin biopsies from 80 subjects: 49 consecutive patients with PA, optimally treated with a mineralocorticoid receptor antagonist; 6 essential hypertensives; and 25 normotensive controls. We measured Na+, K+, water content with atomic absorption spectroscopy after ashing, and NFAT5 mRNA with digital droplet polymerase chain reaction. The patients with PA were retested after adrenalectomy. RESULTS: We discovered a higher dry weight of the skin biopsy specimen at surgery than at follow-up (P<0.001) and a direct correlation with electrolyte and water content (all P<0.01), indicating the need for dry weight adjustment of electrolyte and water data. Surgical cure of PA markedly increased skin dry weight-adjusted K+ (from 1.14±0.1 to 2.81±0.27 µg/mg; P<0.001) and water content (from 2.92±1.4 to 3.85±0.23 mg/mg; P<0.001), but left dry weight-adjusted skin Na+ content unaffected. In patients with PA, NFAT5 mRNA was higher (P=0.031) than in normotensive controls and decreased after surgery (P=0.035). CONCLUSIONS: Despite mineralocorticoid receptor antagonist treatment ensuring normokalemia, the patients with PA had a skin cell K+ depletion that was corrected by adrenalectomy. The activated NFAT5/TonEBP pathway during mineralocorticoid receptor antagonist administration suggests enhanced skin Na+ lymphatic drainage and can explain the lack of overt skin Na+ accumulation in patients with PA. Its deactivation after surgical cure can account for the lack of skin Na+ decrease postadrenalectomy. REGISTRATION: URL: https://www.clinicaltrials.gov; Unique identifier: NCT06090617.

Adaptation mechanism of Phan Rang sheep to salinity in drinking water under tropical conditions.

The aims of this study were to determine adaptation mechanism of sheep to salinity in drinking water. A group of 10 male sheep were used in a 6-week of experiment, with 1 week for pre-treatment period (Week 1), 4 weeks for during treatment period (Week 2 to Week 5), and 1 week for posttreatment period (Week 6). During the pre- and posttreatment periods, sheep consumed with fresh water. However, during treatment period, they were given with diluted seawater (DSW) at concentrations of 0.5%, 1.0%, 1.5%, and 2% for Weeks 2, 3, 4, and 5, respectively. Animal was offered 300 g concentrate and corn stover silage for ab libitum. Dry matter intake decreased as DSW increased, whereas sheep drinking DSW showed an increase in water intake and urine volume (p < 0.05). Body weight change decreased in 2% DSW. Sheep consuming 2% DSW exhibited higher plasma electrolyte levels compared to other groups. But plasma levels of AST, ALT, and creatinine were unaffected by DSW (p > 0.05). The elevated levels and excretions of urinary electrolytes were found in DSW groups (p < 0.05). Water balance was unaffected by DSW, except during the recovery period. It concluded that adapted sheep can consume DSW up to 1.5% without harmful effects.

Super SEI-Forming Anion for Enhanced Interfacial Stability in Solid-State Lithium Metal Batteries.

The extremely high chemical reactivity of lithium metal (Li°) electrodes and its enormous volume change during repetitive cycles cause continuous interfacial degradations in prevailing organic electrolytes, thus deteriorating the cycling performances of rechargeable lithium metal batteries (LMBs). Herein, departing from traditional wisdom on the design of electrolyte components, a super SEI-forming anion (SSA), as an efficient percussor for building stable interphases on Li° electrode, is proposed. Comprehensive investigations related to the unique anion chemistry of SSA reveal that the sulfonate and polyfluoroalkyl functionalities synergistically contribute to uniform spatial distributions of designer interfacial species, greatly improving the surface coverage property and conformal ability of the resulting interphases. Consequently, the incorporation of SSA leads to significant improvements in the cyclability of Li° electrode (exceeding 575 mAh cm-2 before failure) and the corresponding rechargeable Li°||LiFePO4 cells [a five-time increase in lifespan as compared to the benchmark cell with the popular SEI-forming anion bis(fluorosulfonyl)imide (FSI)]. The present work offers a paradigm shift to tame the notorious interfacial issues via upgraded anion chemistry, which can promote the practical development of rechargeable LMBs and other kinds of metal batteries.

Hydrogen-Bonded Ionic Co-Crystals for Fast Solid-State Zinc Ion Storage.

The development of new ionic conductors meeting the requirements of current solid-state devices is imminent but still challenging. Hydrogen-bonded ionic co-crystals (HICs) are multi-component crystals based on hydrogen bonding and Coulombic interactions. Due to the hydrogen bond network and unique features of ionic crystals, HICs have flexible skeletons. More importantly, anion vacancies on their surface can potentially help dissociate and adsorb excess anions, forming cation transport channels at grain boundaries. Here, it is demonstrated that a HIC optimized by adjusting the ratio of zinc salt and imidazole can construct grain boundary-based fast Zn2+ transport channels. The as-obtained HIC solid electrolyte possesses an unprecedentedly high ionic conductivity at room and low temperatures (≈11.2 mS cm-1 at 25 °C and ≈2.78 mS cm-1 at -40 °C) with ultra-low activation energy (≈0.12 eV), while restraining dendrite growth and exhibiting low overpotential even at a high current density (<200 mV at 5.0 mA cm-2) during Zn symmetric cell cycling. This HIC also allows solid-state Zn||covalent organic framework full cells to work at low temperatures, providing superior stability. More importantly, the HIC can even support zinc-ion hybrid supercapacitors to work, achieving extraordinary rate capability and a power density comparable to aqueous solution-based supercapacitors. This work provides a path for designing facilely prepared, low-cost, and environmentally friendly ionic conductors with extremely high ionic conductivity and excellent interface compatibility.

Zinc Chemistries of Hybrid Electrolytes in Zinc Metal Batteries: From Solvent Structure to Interfaces.

Along with the booming research on zinc metal batteries (ZMBs) in recent years, operational issues originated from inferior interfacial reversibility have become inevitable. Presently, single-component electrolytes represented by aqueous solution, "water-in-salt," solid, eutectic, ionic liquids, hydrogel, or organic solvent system are hard to undertake independently the task of guiding the practical application of ZMBs due to their specific limitations. The hybrid electrolytes modulate microscopic interaction mode between Zn2+ and other ions/molecules, integrating vantage of respective electrolyte systems. They even demonstrate original Zn2+ mobility pattern or interfacial chemistries mechanism distinct from single-component electrolytes, providing considerable opportunities for solving electromigration and interfacial problems in ZMBs. Therefore, it is urgent to comprehensively summarize the zinc chemistries principles, characteristics, and applications of various hybrid electrolytes employed in ZMBs. This review begins with elucidating the chemical bonding mode of Zn2+ and interfacial physicochemical theory, and then systematically elaborates the microscopic solvent structure, Zn2+ migration forms, physicochemical properties, and the zinc chemistries mechanisms at the anode/cathode interfaces in each type of hybrid electrolytes. Among of which, the scotoma and amelioration strategies for the current hybrid electrolytes are actively exposited, expecting to provide referenceable insights for further progress of future high-quality ZMBs.

Exploring the Impact of In Situ-Formed Solid-Electrolyte Interphase on the Cycling Performance of Aluminum Metal Anodes.

Unwanted processes in metal anode batteries, e.g., non-uniform metal electrodeposition, electrolyte decomposition, and/or short-circuiting, are not fully captured by the electrolyte bulk solvation structure but rather defined by the electrode-electrolyte interface and its changes induced by cycling conditions. Specifically, for aluminum-ion batteries (AIBs), the role of the solid-electrolyte interphase (SEI) on the Al0 electrodeposition mechanism and associated changes during resting or cycling remain unclear. Here, we investigated the current-dependent changes at the electrified aluminum anode/ionic liquid electrolyte interface to reveal the conditions of the SEI formation leading to irreversible cycling in the AIBs. We identified that the mechanism of anode failure depends on the nature of the counter electrode, where the areal capacity and cycling current for Al0 electrodeposition dictates the number of successful cycles. Notwithstanding the differences behind unstable aluminum anode cycling in symmetrical cells and AIBs, the uniform removal of electrochemically inactive SEI components, e.g., oxide-rich or solvent-derived organic-rich interphases, leads to more efficient cycling behavior. These understandings raise the importance of using specific conditioning protocols for efficient cycling of the aluminum anode in conjugation with different cathode materials.

Selective Methylation of Cyclic Ether Towards Highly Elastic Solid Electrolyte Interphase for Silicon-based Anodes.

Silicon (Si)-based anodes offer high theoretical capacity for lithium-ion batteries but suffer from severe volume changes and continuous solid electrolyte interphase (SEI) degradation. Here, we address these challenges by selective methylation of 1,3-dioxolane (DOL), thus shifting the unstable bulk polymerization to controlled interfacial reactions and resulting in a highly elastic SEI. Comparative studies of 2-methyl-1,3-dioxolane (2MDOL) and 4-methyl-1,3-dioxolane (4MDOL) reveal that 4MDOL, with its larger ring strain and more stable radical intermediates due to hyperconjugation effect, promotes the formation of high-molecular-weight polymeric species at the electrode-electrolyte interface. This elastic, polymer-rich SEI effectively accommodates volume changes of Si and inhibits continuous side reactions. Our designed electrolyte enables Si-based anode to achieve 85.4% capacity retention after 400 cycles at 0.5 C without additives, significantly outperforming conventional carbonate-based electrolytes. Full cells also demonstrate stable long-term cycling. This work provides new insights into molecular-level electrolyte design for high-performance Si anodes, offering a promising pathway toward next-generation lithium-ion batteries with enhanced energy density and longevity.

Hygroscopic Nature of Lithium Ions: A Simple Key to Super Tough Atmosphere-Stable Hydrogel Electrolytes.

Gel electrolytes have emerged as a versatile solution to address numerous limitations associated with liquid electrolytes in electrical energy storage (EES) devices, in terms of safety, flexibility, and affordability. Aqueous gel electrolytes, in particular, exhibit exceptional features by offering one of the highest ion solvation capacities and ionic conductivities. The two main challenges with hydrogel electrolytes are their easy freezing at subzero temperatures and rapid dehydration under open conditions, leading to the failure of the EES device. In response, we present an uncomplicated and quick-to-make hydrogel electrolyte system offering impressive mechanical properties (205.5 kPa tensile strength, 2880 kJ/m3 toughness, and 3030% strain at the break), along with antifreezing and antiflammability attributes. Notably, the hydrogel electrolyte demonstrates high ionic conductivity and superior performance in supercapacitor cells over a wide range of temperatures (-40 to 80 °C) and under various deformations. The hydrogel electrolyte maintains its capabilities under open conditions over an extended period of time, even at 50 °C, showcased by powering a wristwatch. The atmospheric stability of the hydrogel electrolyte demonstrated in this study introduces promising prospects for the future of EES devices spanning from production to end-user consumption.

Cutting-Edge Progress in Aqueous Zn-S Batteries: Innovations in Cathodes, Electrolytes, and Mediators.

Rechargeable aqueous zinc-sulfur batteries (AZSBs) are emerging as prominent candidates for next-generation energy storage devices owing to their affordability, non-toxicity, environmental friendliness, non-flammability, and use of earth-abundant electrodes and aqueous electrolytes. However, AZSBs currently face challenges in achieving satisfied electrochemical performance due to slow kinetic reactions and limited stability. Therefore, further research and improvement efforts are crucial for advancing AZSBs technology. In this comprehensive review, it is delved into the primary mechanisms governing AZSBs, assess recent advancements in the field, and analyse pivotal modifications made to electrodes and electrolytes to enhance AZSBs performance. This includes the development of novel host materials for sulfur (S) cathodes, which are capable of supporting higher S loading capacities and the refinement of electrolyte compositions to improve ionic conductivity and stability. Moreover, the potential applications of AZSBs across various energy platforms and evaluate their market viability based on recent scholarly contributions is explored. By doing so, this review provides a visionary outlook on future research directions for AZSBs, driving continuous advancements in stable AZSBs technology and deepening the understanding of their charge-discharge dynamics. The insights presented in this review signify a significant step toward a sustainable energy future powered by renewable sources.

High-Performance Pure Polymer Electrolytes with Enhanced Ionic Conductivity for Room-Temperature Applications.

All-solid-state lithium metal batteries (ASSLMBs) are renowned for their high energy density and safety, positioning them as leading candidates for next-generation energy storage solutions. In this study, pure polymer solid-state electrolytes are developed using the solution casting method, optimized for room temperature operation. The base material, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), is enhanced with succinonitrile (SN) and polyacrylonitrile (PAN) to improve its electrochemical performance at room temperature. The optimized electrolyte, PSP-0.05, demonstrated superior characteristics, including an ionic conductivity (σ) of 3.2 × 10-4 S cm-1 and a wide voltage window of up to 5 V. When integrated into full batteries, PSP-0.05 exhibited exceptional performance in multiplicative cycling tests at room temperature, achieving discharge specific capacities of 132 and 113 mAh g-1 at 3 and 5 C rates, respectively. Additionally, long-term cycling at 1 C rate resulted in an initial discharge-specific capacity of 145.2 mAh g-1 with over 94.9% capacity retention after 1000 cycles. Given the simplicity of the preparation process and its impressive electrochemical properties, the PSP-0.05 electrolyte holds significant potential for practical applications in safer ASSLMBs.

Surface Coordination of Garnet Fillers Improves the Organic-Inorganic Interfacial Compatibility of Composite Solid Electrolyte.

Composite solid electrolytes (CSEs) have become one of the most promising solid-state electrolytes due to their favorable safety and flexibility. However, the weak interaction between inorganic fillers and polymer matrix leads to poor organic-inorganic interfacial compatibility, which degrades the electrochemical performance of CSEs. Herein, it is demonstrated that Li6.4La3Zr1.4Ta0.6O12 (LLZTO) can be chemically bonded to the polymer matrix by surface coordination of the 1,2-dithiolane group of lipoic acid (LA) with metal atoms on the surface of LLZTO through a combination of experimental investigations and theoretical calculations. The surface coordination not only enhances the interfacial compatibility between LLZTO and the polymer matrix, but also facilitates rapid Li+ transport, which leads to the ionic conductivity of the prepared CSE (P-V-M@LLZTO) as high as 6.1 × 10-4 S cm-1 at 30 °C. The excellent interface compatibility ensures a stable cycle of Li/P-V-M@LLZTO/Li symmetrical cell for more than 3500 h. As a result, LiFePO4/P-V-M@LLZTO/Li cell delivers the discharge capacity of 161 mAh g-1 after 5 cycles with a capacity retention of 81% after 500 cycles at 0.5C under 30 °C. This work demonstrates that surface coordination is an effective strategy to solve the inherent interfacial incompatibility problem in CSEs.

Confined Polyethylene Glycol Anchored in Kaolinite as High Ionic Conductivity Solid-State Electrolyte for Lithium Batteries.

Solid-state electrolytes (SSEs) have garnered significant attention as critical materials for enabling safer, energy-dense, and reversible electrochemical energy storage in batteries. Among the various types of solid electrolytes developed, composite polymer electrolytes (CPEs) have stood out as some of the most promising candidates due to their well-rounded performance. In this study, we choose polyethylene glycol (PEG) as the covalent grafting intercalant and lithium perchlorate as carrier source to prepare a fast lithium ion conductor, K-PEG-Li doped with clay-based active filler as a CPE. The CPE exhibits excellent lithium conduction (4.36 × 10-3 S cm-1 at 25 °C and 3.32 × 10-2 S cm-1 at 115 °C), great mechanical performance with good tensile strength (6.07 MPa) and toughness (strain 313%), and convincing flame-retardancy. These outstanding conducting and mechanical functionalities indicate that such a clay-based active filler doped composite polymer electrolyte will find promising application in solid-state lithium batteries.

Nonflammable Ether and Phosphate-Based Liquid Electrolytes for Sodium-Ion Batteries.

This study investigates a group of electrolytes containing NaPF6 or NaBF4 salts in phosphate- and ether-based solvents for high-mass loading sodium-ion batteries. It explores physicochemical properties such as ionic conductivity, dynamic viscosities, and nonflammability. The combination of experimental with computational studies reveals detailed insights into the physicochemical properties of the nonflammable liquid electrolytes. Diglyme-based electrolytes become nonflammable with 50 vol % phosphate solvents, while tetraglyme-based electrolytes require 70 vol %. The solvation structure has been investigated using NMR and is combined with computational studies to provide information about properties such as solvation structure, ionic conductivity, and viscosity. The molecular dynamic simulations confirm the enhanced solvation in diglyme-based liquid electrolytes observed experimentally by 23Na-NMR. Despite lacking sufficient electrochemical stability, this work provides a fundamental understanding of the solvation structure and physicochemical properties of a novel electrolyte system. This is an important contribution to be applied in future electrolyte design rationale.

Li-Fe-Cl Families as Novel Solid Electrolytes for All-Solid-State Batteries.

The halides have attracted much attention as novel solid electrolytes because of their easy synthesis, high electrochemical stability, and high ionic conductivities. However, the reported halides for solid electrolytes are still understudied compared with the oxides and sulfides. Here, we studied the Li-Fe-Cl phases that include Li2FeCl4 and Li6FeCl8. Using the self-doping approach, a maximum ionic conductivity of 2.0 × 10-4 S cm-1 at 50 °C was achieved for Li1.8Fe1.1Cl4. It was improved by 3 orders of magnitude compared with that of Li2FeCl4 (8.27 × 10-7 S cm-1 at 50 °C). For the Li|Li1.8Fe1.1Cl4|Li half-cell, it cycled for 2000 h at 50 °C under a current density of 0.01 mA cm-2, indicating an acceptable compatibility between Li2FeCl4 and Li. Finally, an all-solid-state battery was successfully assembled with Li1.8Fe1.1Cl4@LFP as the cathode, Li1.8Fe1.1Cl4 as the electrolyte, and a Li sheet as the anode. The initial specific charge capacity of the battery was 76.36 mAh g-1 at 0.1C and 50 °C. The initial Coulombic efficiency was 73.06%. This study suggests Li2FeCl4 as a new solid electrolyte, and the introduction of Li vacancies into the Li site is an efficient way to improve the electrochemical properties of halides.

Enhanced Critical Current Density in the Garnet Oxide Electrolyte by a Silver Interlayer.

Ta-doped Li6.4La3Zr1.4Ta0.6O12 (LLZTO) for solid-state lithium batteries demonstrates encouraging performance; however, they encounter issues with lithium dendrite formation that impede their widespread use. Herein, we design a LLZTO ceramic with an interlayer containing a mixed dense layer of Ag and LLZTO, prepared by one-step sintering. The Ag-rich interlayer in LLZTO can hinder the growth and the penetration of lithium dendrites though the reaction between Ag and lithium metal. Compared with the Ag-free counterpart, a higher critical current density of 0.6 mA cm-2, in addition to a longer life span under a current density of 0.2 mA cm-2, is achieved by adopting the interlayer in LLZTO. This research offers novel insights into the engineering of garnet-based solid electrolytes, tailored for the advancement of high-rate lithium metal batteries.

Visible and near-infrared modulating tungsten suboxide nanorods electrochromic films in acidic aqueous electrolytes.

Proton-based aqueous electrolytes can be used to achieve high performance electrochromic nanocrystal thin films due to their small ion size. However, acidic aqueous electrolyte systems have not yet been explored in near-infrared (NIR) absorbing plasmonic tungsten oxide nanocrystal films. Here, we demonstrate tungsten suboxide nanorod films with excellent visible and NIR modulation performance in the H+-based aqueous electrolytes, thanks to their mesoporous structure, nanosized domains, and open tunnel structure. Colloidally synthesized WO2.83 nanorods with an average width of 6 nm and length of 48 nm were converted to WO2.90 nanorod film via annealing in air, while still preserving open tunnels. These films exhibit fast switching speed (tc = 0.9 s, tb = 2.1 s), excellent cycling stability over 2500 cycles, wide optical modulation up to ΔT = 53.8 % in the NIR region, and a high coloration efficiency (CE) of 167 cm2 C⁻1 at 1300 nm. Additionally, introducing a thin spacer (25 µm) reduced intrinsic NIR absorption from water, thereby enhancing the NIR modulation properties. These highly performing aqueous proton-electrolytes-based electrochromic devices open new possibilities for implementing visible and NIR electrochromism.

Dipole Moment Dictates the Preferential Immobilization in Gel Electrolytes for Ah-level Aqueous Zinc-Metal Batteries.

Aqueous Zn-metal batteries are of great interest due to their high material abundance, low production cost, and excellent safety. However, they suffer from severe side reactions and notorious dendrite growth closely related to electrolytes. Here, in-situ generated zwitterionic polymers are used as gel electrolytes to overcome these problems. It is shown that anions and H2O, but not anions and cations, are preferentially immobilized at different sites of zwitterionic polymers, facilitating the free migration of Zn2+ and reducing the side reactions. This immobilization can be associated with the dipole moment of zwitterionic polymers. As a result, poly[3-dimethyl(methacryloyl oxyethyl) ammonium propane sulfonate] (PDMAPS) stands out from a series of zwitterionic polymers and outperforms the other candidates in electrochemical performance. The symmetric cells using PDMAPS smoothly operate ~9000 h at 0.5 mA cm-2 for 0.5 mAh cm-2, much better than the controls. Moreover, PDMAPS enables an Ah-level pouch cell for continuous cycling. These results not only benefit the rational molecular design of advanced electrolytes, but also demonstrate the promising potential of zwitterionic polymers in aqueous Zn-metal batteries.

Microwave-assisted solvothermal synthesis of nanostructured Ga-Doped Li7La3Zr2O12 solid electrolyte with enhanced densification and Li-ion conductivity.

Garnet-type Li7La3Zr2O12 (LLZO) Li-ion solid electrolytes are promising candidates for safe, next-generation solid-state batteries. In this study, we synthesize Ga-doped LLZO (Ga-LLZO) electrolytes using a microwave-assisted solvothermal method followed by low-temperature heat treatment. The nanostructured precursor (<50 nm) produced by the microwave-assisted solvothermal process has a high surface energy, facilitating the reaction for preparing garnet-type Ga-LLZO powders (<800 nm) within a short time (<5 h) at a low calcination temperature (<700 °C). Additionally, the calcined nanostructured Ga-LLZO powder can be sintered to produce a high-density pellet with minimized grain boundaries under moderate sintering conditions (temperature: 1150 °C, duration: 10 h). The optimal doping concentration was determined to be 0.4 mol% Ga, which resulted significantly increased the ionic conductivity (1.04 × 10-3 S cm-1 at 25 °C) and stabilized the cycling performance over 1700 h at 0.4 mA cm-2. This approach demonstrates the potential to synthesize oxide-type solid electrolyte materials with improved properties for solid-state batteries.