Ultrafast Li‐Rich Transport in Composite Solid‐State Electrolytes

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 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.

Язык: Английский

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Host–Guest Inversion Engineering Induced Superionic Composite Solid Electrolytes for High-Rate Solid-State Alkali Metal Batteries

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Март 17, 2025

Abstract Composite solid electrolytes (CSEs) are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost expensive active ceramic fillers. Here, a host–guest inversion engineering strategy is proposed develop superionic CSEs using cost-effective SiO 2 nanoparticles as passive hosts poly(vinylidene fluoride-hexafluoropropylene) (PVH) microspheres polymer guests, forming an unprecedented “polymer guest-in-ceramic host” (i.e., PVH-in-SiO ) architecture differing the traditional “ceramic guest-in-polymer host”. The exhibits excellent Li-salt dissociation, achieving high-concentration free + . Owing low diffusion energy barriers coefficient, thermodynamically kinetically favorable migrate at /PVH interfaces. Consequently, delivers exceptional of 1.32 × 10 −3 S cm −1 25 °C (vs typically −5 –10 −4 high-cost ceramics), achieved under ultralow residual solvent content 2.9 wt% 8–15 in other CSEs). Additionally, electrochemically stable with anode various cathodes. Therefore, demonstrates high-rate cyclability LiFePO 4 |Li full cells (92.9% capacity-retention 3C after 300 cycles °C) outstanding stability high-mass-loading (9.2 mg high-voltage NCM622 (147.1 mAh g ). Furthermore, we verify versatility by fabricating Na-ion K-ion-based similarly promotions conductivity. Our offers simple, low-cost approach large-scale application beyond.

Язык: 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, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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.

Язык: 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, Год журнала: 2025, Номер unknown

Опубликована: Янв. 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.

Язык: 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, Год журнала: 2025, Номер unknown, С. 104210 - 104210

Опубликована: Март 1, 2025

Язык: 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, Год журнала: 2024, Номер 14(43)

Опубликована: Авг. 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.

Язык: 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, Год журнала: 2024, Номер 146(45), С. 31137 - 31149

Опубликована: Ноя. 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

Язык: 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, Год журнала: 2024, Номер 16(24), С. 31648 - 31656

Опубликована: Июнь 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.

Язык: Английский

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

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Янв. 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.

Язык: 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, Год журнала: 2025, Номер unknown

Опубликована: Янв. 17, 2025

Язык: Английский

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