Solvation‐Tailored PVDF‐Based Solid‐State Electrolyte for High‐Voltage Lithium Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(18)

Опубликована: Март 12, 2024

Abstract Poly(vinylidene fluoride) (PVDF)‐based polymer electro‐lytes are attracting increasing attention for high‐voltage solid‐state lithium metal batteries because of their high room temperature ionic conductivity, adequate mechanical strength and good thermal stability. However, the presence highly reactive residual solvents, such as N, N‐dimethylformamide (DMF), severely jeopardizes long‐term cycling Herein, we propose a solvation‐tailoring strategy to confine solvent molecules by introducing low‐cost 3 Å zeolite molecular sieves fillers. The strong interaction between DMF sieve weakens ability participate in solvation Li + , leading more anions being involved solvation. Benefiting from tailored anion‐rich coordination environment, interfacial side reactions with anode NCM811 cathode effectively suppressed. As result, Li||Li symmetrical cells demonstrates ultra‐stable over 5100 h at 0.1 mA cm −2 Li||NCM811 full achieve excellent stability than 1130 250 cycles under charging cut‐off voltages 4.3 V 4.5 V, respectively. Our work is an innovative exploration address negative effects PVDF‐based electrolytes highlights importance modulating structures electrolytes.

Язык: Английский

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Visualizing and Regulating Dynamic Evolution of Interfacial Electrolyte Configuration during De‐solvation Process on Lithium‐Metal Anode

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)

Опубликована: Март 5, 2024

Abstract Acting as a passive protective layer, solid‐electrolyte interphase (SEI) plays crucial role in maintaining the stability of Li‐metal anode. Derived from reductive decomposition electrolytes (e.g., anion and solvent), SEI construction presents an interfacial process accompanied by dynamic de‐solvation during plating. However, typical electrolyte engineering related modification strategies always ignore evolution configuration at Li/electrolyte interface, which essentially determines architecture. Herein, employing advanced electrochemical situ FT‐IR MRI technologies, we directly visualize variations solvation environments involving Li + ‐solvent/anion. Remarkably, weakened ‐solvent interaction anion‐lean have been synchronously revealed, is difficult for fabrication anion‐derived layer. Moreover, simple regulation strategy, pulse protocol was introduced to effectively restore concentration, resulting enhanced LiF‐rich layer improved plating/stripping reversibility.

Язык: Английский

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Strong Lewis-acid coordinated PEO electrolyte achieves 4.8 V-class all-solid-state batteries over 580 Wh kg−1

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 23, 2024

Polyethylene oxide (PEO) based electrolytes critically govern the security and energy density of solid-state batteries, but typically suffer from poor oxidation resistance at high voltages, which limits batteries. Here, we report a Lewis-acid coordinated strategy to significantly improve cyclic stability 4.8 V-class PEO-based battery. The introduced Mg

Язык: Английский

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In Situ Structure Modulation of Cathode‐Electrolyte Interphase for High‐Performance Potassium‐Ion Battery

Advanced Functional Materials, Год журнала: 2024, Номер 34(19)

Опубликована: Янв. 9, 2024

Abstract Manganese‐based layered oxide cathodes, particularly K x MnO 2 (KMO), have shown great potential in potassium‐ion batteries (PIBs) due to their low cost, high theoretical capacities, and excellent thermal stability. However, Jahn‐Teller distortion, manganese dissolution, interface instability of electrode/electrolyte lead structural performance decay. Here, lithium difluoro(oxalate) borate (LiDFOB) is introduced as an electrolyte additive improve the electrochemical P3‐type KMO. LiDFOB creates a uniform, thin, robust cathode‐electrolyte interphase layer on cathode surface, enhancing reaction kinetics, preventing stabilizing structure. The P3‐KMO with basic exhibits significantly improved performance, such remarkable Coulombic efficiency ≈99.5% capacity retention 78.6% after 300 cycles at 100 mA g −1 . Moreover, full cell P3‐KMO||soft carbon demonstrates satisfactory specific energy density. This study emphasizes importance chemistry for PIBs.

Язык: Английский

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Advancements and Challenges in Organic–Inorganic Composite Solid Electrolytes for All-Solid-State Lithium Batteries

Nano-Micro Letters, Год журнала: 2024, Номер 17(1)

Опубликована: Сен. 20, 2024

To address the limitations of contemporary lithium-ion batteries, particularly their low energy density and safety concerns, all-solid-state lithium batteries equipped with solid-state electrolytes have been identified as an up-and-coming alternative. Among various SEs, organic-inorganic composite solid (OICSEs) that combine advantages both polymer inorganic materials demonstrate promising potential for large-scale applications. However, OICSEs still face many challenges in practical applications, such ionic conductivity poor interfacial stability, which severely limit This review provides a comprehensive overview recent research advancements OICSEs. Specifically, influence fillers on main functional parameters OICSEs, including conductivity, Li

Язык: Английский

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An All-Solid-State fluorinated Ion-Conductive elastomer with outstanding mechanical properties and high environmental stability for flexible electronics

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159437 - 159437

Опубликована: Янв. 1, 2025

Язык: Английский

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Dual-Anion-Rich Polymer Electrolytes for High-Voltage Solid-State Lithium Metal Batteries

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Solid polymer electrolytes (SPEs) are promising candidates for lithium metal batteries (LMBs) owing to their safety features and compatibility with anodes. However, the inferior ionic conductivity electrochemical stability of SPEs hinder application in high-voltage solid-state LMBs (HVSSLMBs). Here, a strategy is proposed develop dual-anion-rich solvation structure by implementing ferroelectric barium titanate (BTO) nanoparticles (NPs) dual salts into poly(vinylidene fluoride) (PVDF)-based HVSSLMBs. The BTO NPs regulate spatial PVDF segments, enhancing local built-in electric field SPEs, which, turn, facilitates dissolution dissociation salts. This contributes an enhanced steric effect, which significantly improves Li+ transport kinetics stability. designed PVDF-based SPE achieves high 4.1 × 10–4 S cm–1 transference number 0.70 at 25 °C. Li//Li symmetric cells deliver excellent critical current density 2.4 mA cm–2 maintain stable Li plating/stripping process over 5000 h. After 1000 cycles 2C, LiFePO4//Li achieve discharge capacity 108.3 mAh g–1. Furthermore, LiNi0.8Co0.1Mn0.1O2 (NCM811)//Li present retention after 300 1C cutoff voltage 4.4 V. NCM811/Graphite pouch exhibit cycling performance. work illustrates that synergistic integration functional multiple holds significant potential development SPEs.

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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Recent progress in ultra-thin solid polymeric electrolytes for next-generation lithium batteries

Energy storage materials, Год журнала: 2024, Номер 67, С. 103329 - 103329

Опубликована: Март 1, 2024

Язык: Английский

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Non‐Resonant Structure Induces N‐Rich Solid Electrolyte Interface toward Ultra‐Stable Solid‐State Lithium‐Metal Batteries

Advanced Functional Materials, Год журнала: 2024, Номер 34(36)

Опубликована: Март 19, 2024

Abstract The practical application of all‐solid‐state lithium metal batteries (ASSLMBs) is limited by (Li) anode instability including Li dendrite formation and deteriorating interface with electrolytes. Here, a functional additive, isosorbide mononitrate (ISMN) non‐resonant structure (O 2 −N−O−) reported, which improves its reactivity utilized to build stable N‐rich solid electrolyte interface, effectively alleviating side reactions for poly(vinylidene fluoride) (PVDF)‐lithium bis(trifluoromethane sulfonyl) imide (LiTFSI)‐based (PLE‐ISMN). In addition, the ion‐dipole interaction between ISMN ions facilitates dissociation LiTFSI form carrier ions, improving ionic conductivity (4.4 × 10 −4 S cm −1 ) transference number (0.50) PLE‐ISMN. Consequently, Li/Li symmetric cell delivers high critical current density 2.0 mA −2 stripping/plating cycling over 5000 h capacity 1.0 mAh . Moreover, Li|LiFePO 4 an excellent initial discharge 154.0 g outstanding retention 88.9% after 500 cycles at 0.5 C. Li|LiNi 0.8 Co 0.1 Mn O also exhibits good performance 4.4 V 1

Язык: Английский

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