Ultrafast Li‐Rich Transport in Composite Solid‐State Electrolytes

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 31, 2025

Solid-state lithium (Li) metal batteries (SSLMBs) have garnered considerable attention due to their potential for high energy density and intrinsic safety. However, widespread development has been hindered by the low ionic conductivity of solid-state electrolytes. In this contribution, a novel Li-rich transport mechanism is proposed achieve ultrafast Li-ion conduction in composite By incorporating cation-deficient dielectric nanofillers into polymer matrices, it found that negatively charged cation defects effectively intensify adsorption Li ions, resulting concentration enrichment on surface fillers. More importantly, these formed layers are interconnected establish continuous networks. The electrolyte exhibited remarkably ion activation (0.17 eV) achieved an unprecedented approaching 1 × 10⁻3 S cm⁻1 at room temperature. Li||LiNi0.8Co0.1Mo0.1O2 full cells demonstrated extended cycling life over 200 cycles with capacity retention 70.7%. This work provides fresh insight improving constructing networks, paving way high-performance SSLMBs.

Language: Английский

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Achieving Balanced Performance and Safety for Manufacturing All‐Solid‐State Lithium Metal Batteries by Polymer Base Adjustment

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 12, 2025

Abstract Organic–inorganic composite solid electrolytes (CSEs) have aroused intensive attention due to their balanced performance and environmental adaptability. However, high performance, e.g., the ionic conductivity, wide electrochemical window, excellent interfacial compatibility, is achieved by sacrificing mechanical strength, which increases possibility of short circuits thus poses serious safety hazards. Herein, a high‐performance rigid‐flexible PM polymer matrix synthesized simple process polymerization addition reaction between polyethylene oxide (PEO) methylene diphenyl diisocyanate (MDI), where PM‐based CSEs (denoted as PMPS@LATP‐NF) also prepared through porous non‐woven fabric (NF) dense filling process. The effect on properties, transport, interactions elucidated combined experimental theoretical methods, functional groups (─C─O─C, ─NCO, ─NH) contribute dissociation lithium salts, self‐healing, compatibility. Besides, PMPS@LATP‐NF can further mechanically regulate dendrites demonstrates ultra‐high thermal stability. Moreover, exhibits significantly enhanced cycling rate capability in all‐solid‐state Li/LiFePO 4 cells. This work emphasizes pivotal role properties electrolyte modification, stability, lifespan metal batteries, provides inspiration for development practical electrolytes.

Language: Английский

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Compatible Interfaces Constructed by Surficial Indiumization on Garnet Solid Electrolyte for Long‐Cycling All‐Solid‐State Lithium Metal Battery

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Composite solid electrolytes (CSEs) based on poly(vinylidene fluoride)-co-hexafluoropropylene (PVDF-HFP) and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) show great potential in building high energy density all-solid-state lithium metal batteries (ASSBs). Nevertheless, the Li2CO3 passivation layer formed LLZTO surface not only induces dehydrofluorination of PVDF-HFP but also blocks Li+ transport at interfaces PVDF-HFP/LLZTO CSE/electrodes. Herein, acetate-assisted surficial indiumization with a thickness 4 nm is carried out to convert detrimental into stable conductor LiInO2 (LIO) LLZTO. With this modification, air stability CSEs achieved which prevents regeneration effectively. Attributed unblocked paths LLZTO@LIO/PVDF-HFP (LIO-CSE) interface, ionic conductivity 3.1 × 10-4 S cm-1 transference number 0.673 are attained. The Li2CO3-free contributes constructing robust electrolyte interphase predominantly inorganic components, successfully decreases side reactions ultimately realizes good compatibility LLZTO/polymer electrolyte/electrode interfaces. assembled Li|LIO-CSE|Li cells exhibit excellent electrochemical for 3100 h 0.5 mA cm-2. Li/LIO-CSE/LiFePO4 ASSB delivers high-capacity retention 81.8% after 1000 cycles 25 °C. This work provides promising method toward remarkable interfacial ASSBs.

Language: Английский

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Creating electrostatic shielding effects through dual-salt strategy to regulate coordination environment of Li⁺ and realize high-performance all-solid-state lithium metal batteries

Energy storage materials, Journal Year: 2025, Volume and Issue: unknown, P. 104210 - 104210

Published: March 1, 2025

Language: Английский

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Ceramic Rich Composite Electrolytes: An Overview of Paradigm Shift toward Solid Electrolytes for High‐Performance Lithium‐Metal Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(43)

Published: Aug. 22, 2024

Abstract Exploiting the synergy between organic polymer electrolytes and inorganic via development of composite can suggest solutions to current challenges next‐generation solid‐state lithium‐metal batteries (SSLMBs). Depending upon a mass fraction fillers polymers, are broadly classified into “ceramic‐in‐polymer” (CIP) “polymer‐in‐ceramic” (PIC) categories, inheriting distinct structure electrochemical properties. Since stability characteristics phase superior those for lithium‐ion conduction, applying lithium‐enrich active filler in PIC seems more promising. The preserves primary migratory channels electrolyte, while viscoelastic properties attempt be introduced from binder or host. present work overviews studies on state‐of‐the‐art electrolytes, fundamental mechanism ionic preparation methods, progress materials SSLMBs. In addition, modification strategies improving electrode–electrolyte interface also emphasized. Moreover, it further prospects effective future PICs‐based CPEs accelerate practical application This review examines outlook PIC‐based lithium batteries.

Language: Английский

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Constructing an Artificial Interface as a Bifunctional Promoter for the Li Anode and the NCM Cathode in Lithium Metal Batteries

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(45), P. 31137 - 31149

Published: Nov. 1, 2024

The bottleneck of Li metal batteries toward practical applications lies at inferior cyclability as well dendrite issues. As a promising solution, an interface engineering strategy is proposed herein for the anode through constructing hybrid artificial interface. It assembled onto using photocontrolled free radical polymerization (photo-CRP) polyethylene glycol diacrylate-hexafluorobutyl methacrylate and hexafluorobutyl methacrylate-trifluoroethyl carbonate (PEGDA-HFMBA@HFMBA-FEMC or PH@HF layer). Among such interfaces, interior layer PEGDA-HFMBA exists protective shield with flexibility fracture resistance, while exterior HFMBA-FEMC plays role LiF reservoir to promote mass transfer its even electrodeposition. In meantime, some excess HFMBA FEMC monomers further dissolve into electrolyte molecular additives, followed by in situ generation thin robust LiF-rich cathode (CEI). With resulting anode, Li/NCM811 full cells showcase multifold amplification comparison Bare-Li, covering durable capacity retention 81.8% after 400 cycles. When cutoff voltage elevated 4.5 V working temperature 45 °C, still maintain stable operation extending 300

Language: Английский

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Improving the Ionic Conductivity and Anode Interface Compatibility of LLZO/PVDF Composite Polymer Electrolytes by Compositional Tuning

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(24), P. 31648 - 31656

Published: June 5, 2024

Utilizing aluminum-doped nano LLZO (Li6.28La3Zr2Al0.24O12) as the ceramic filler, we synthesized and optimized LLZO/PVDF/LiClO4 composite polymer electrolytes (CPEs) to achieve high ionic conductivity good interfacial stability with metallic lithium. The research examines how PVDF grade mass ratio of LiClO4 affect conductivity, lithium metal compatibility, overall performance CPEs. CPE using Kynar 741 a PVDF-to-LiClO4 2:1 emerged superior, displaying at room temperature (0.12 mS/cm), lowest activation energy (0.247 eV), an extensive electrochemical window (approximately 4.9 V), robust mechanical strength. In tests symmetric cells, membrane facilitated over 1000 h stable cycling 0.1 mA cm–2 mAh cm–2. Furthermore, when integrated into full solid-state lithium–metal batteries LiFePO4 cathodes, it sustained more than 80% capacity retention across 500 charge/discharge cycles rate 0.5 C constantly Coulombic efficiencies above 99.8%, underscoring its exceptional durability efficiency. This provides practical framework benchmarks for developing LLZO/PVDF-based CPEs enhanced against metals.

Language: Английский

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Regulating Lithium-Ion Transport in PEO-Based Solid-State Electrolytes through Microstructures of Clay Minerals

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 11, 2025

Clay minerals show significant potential as fillers in polymer composite solid electrolytes (CSEs), whereas the influence of their microstructures on lithium-ion (Li+) transport properties remains insufficiently understood. Herein, we design advanced poly(ethylene oxide) (PEO)-based CSEs incorporating clay with diverse including 1D halloysite nanotubes, 2D Laponite (Lap) nanosheets, and 3D porous diatomite. These form distinct Li+ pathways at clay-PEO interfaces due to varied structural configurations. Among them, Lap nanosheets exhibit most improvements conductivity (1.67 × 10–4 ± 0.02 S cm–1 30 °C), transference number (0.72), oxidative stability (4.7 V). Consequently, a solid-state Li|LiFePO4 battery PEO/Lap CSE exhibits high reversible capacity superior cycling (with 90.2% retention after 250 cycles 1.0 °C). Furthermore, pouch batteries an integrated LiFePO4 cathode safety performance, even under extreme damage. This work provides valuable theoretical insights for application mineral CSEs.

Language: Английский

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Three-Dimensionally Printed Ionogel-Coated Ceramic Electrolytes for Solid-State Lithium Batteries

ACS Nano, Journal Year: 2025, Volume and Issue: 19(5), P. 5789 - 5800

Published: Jan. 31, 2025

Stereolithography three-dimensional (3D) printing technology enables the customization of ceramic-based solid electrolyte structures with desired electrochemical properties; however, formulating slurries that both are highly ceramic-loaded and have low viscosity for poses a challenge. Here, we propose an ionogel-coated ceramic approach to prepare shear-thinning fast-ion conductor (Li6.5La3Zr1.5Ta0.5O12) slurry, which possesses high content 50 wt % 1.53 Pa·s. Utilizing this 3D symmetric honeycomb briquette-like films printed, solid-state lithium batteries easily fabricated by filling cathode anode into respective honeycombs. The atomic-level interaction between ceramic/ionogel interfaces integrated electrode/electrolyte interface facilitates rapid Li+ transport across multiscale interphases in batteries. Additionally, interactions nanoparticles ionic liquids Li salt substantially increase concentration free Li+, enhance conductivity ensure stable efficiency. Solid-state can cycle stably 500 times without obvious degradation at 0.5 C °C. strategy offers feasible solution customized electrolytes.

Language: Английский

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In situ preparation of composite gel electrolytes with high room-temperature ionic conductivity and homogeneous Na+ flux for sodium metal batteries

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 17, 2025

Language: Английский

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