Beyond Polymerization: In Situ Coupled Fluorination Enables More Stable Interfaces for Solid-State Lithium Batteries

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 23, 2025

In situ polymerization strategies hold great promise for enhancing the physical interfacial stability in solid-state batteries, yet (electro)chemical degradation of polymerized interfaces, especially at high voltages, remains a critical challenge. Herein, we find interphase engineering is crucial process and polymer pioneer an polymerization-fluorination (Poly-FR) strategy to create durable interfaces with excellent stabilities, achieved by designing bifunctional initiator both on-surface lithium donor reactions. The integrated fluorination converts Li2CO3 impurities on LiNi0.8Co0.1Mn0.1O2 (NCM811) surfaces into LiF-rich interphases, effectively inhibiting aggressive (de)lithiation intermediates protecting interface from underlying chemical degradation, thereby surpassing limitations alone. Furthermore, Poly-FR mediated symmetric Li|Li cells achieve impressive cycling up 12,000 h. Solid-state NCM811 cathodes Li metal anodes realize ultrastable performance 400 cycles 83.4% retention voltage 4.5 V. This work points toward advanced beyond.

Язык: Английский

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Leveraging polymer architecture design with acylamino functionalization for electrolytes to enable highly durable lithium metal batteries

Energy & Environmental Science, Год журнала: 2024, Номер 17(18), С. 6739 - 6754

Опубликована: Янв. 1, 2024

A novel polymer architecture design for GPEs is proposed via in situ copolymerization of VC and a new acylamino-crosslinker. This enables accelerated Li + transport dual-reinforced stable interfaces, contributing to long-lifespan LMBs.

Язык: Английский

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Tailored Engineering on the Interface Between Lithium Metal Anode and Solid‐State Electrolytes

Energy & environment materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 4, 2024

The replacement of non‐aqueous organic electrolytes with solid‐state (SSEs) in lithium metal batteries (SLMBs) is considered a promising strategy to address the constraints lithium‐ion batteries, especially terms energy density and reliability. Nevertheless, few SLMBs can deliver required cycling performance long‐term stability for practical use, primarily due suboptimal interface properties. Given diverse solidification pathways leading different characteristics, it crucial pinpoint source deterioration develop appropriate remedies. This review focuses on Li|SSE issues between anode SSE, discussing recent advancements understanding (electro)chemistry, impact defects, evolutions that vary among SSE species. state‐of‐the‐art strategies concerning modified SEI, artificial interlayer, surface architecture, composite structure are summarized delved into internal relationships characteristics enhancements. current challenges opportunities characterizing modifying suggested as potential directions achieving SLMBs.

Язык: Английский

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Isocyanurate‐Derivative Enables Highly Compatible Poly‐Dioxane Electrolyte for Dendrite‐Free Li Metal Batteries

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 30, 2024

Abstract The Li + transport kinetics and electrochemical stability of advanced solid‐state metal batteries (SLMBs) are seriously limited by the actual electrolyte compositions. Here, a novel polyether‐based (PTGDOX) is presented through in situ co‐polymerization integrating 1,3‐dioxane with multifunctional 1,3,5‐triglycidyl isocyanurate additive. group PTGDOX not only provides abundant coordinating sites for transfer restricts movement anions, but also prompts beneficial inorganic‐rich solid interface on electrode. As result, exhibits remarkably increased ionic conductivity 0.48 mS cm −1 at 30 °C reasonable Li‐ion transference number 0.68, enabling Li||Li symmetric cells to stably cycle over 2000 h 1 mAh −2 . Meanwhile, assembled Li||LiFePO 4 exhibit 97.4% capacity retention after 700 cycles 3 C excellent thermal stability. Moreover, demonstrates interfacial compatibility high‐voltage LiNi 0.8 Co 0.1 Mn O 2 cathode. such, this work facile accessible strategy designing interface‐stable polymer electrolytes achieving practical dendrite‐free SLMBs.

Язык: Английский

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Improving thermal stability and kinetical properties through polymer brushes towards wide-temperature solid-state lithium metal batteries

Composites Part B Engineering, Год журнала: 2025, Номер unknown, С. 112328 - 112328

Опубликована: Фев. 1, 2025

Язык: Английский

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Ultra-thin, Scalable, and MOF Network-Reinforced Composite Solid Electrolyte for All-Solid-State Lithium Metal Batteries

Journal of Membrane Science, Год журнала: 2025, Номер unknown, С. 124009 - 124009

Опубликована: Март 1, 2025

Язык: Английский

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Construction of solid-state lithium batteries with high energy density and high safety by in-situ polymerization

Chemical Engineering Journal, Год журнала: 2025, Номер 514, С. 163402 - 163402

Опубликована: Май 6, 2025

Язык: Английский

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Facilitating uniform lithium-ion transport via polymer-assisted formation of unique interfaces to achieve stable 4.7 V Li metal battery

National Science Review, Год журнала: 2025, Номер 12(6)

Опубликована: Май 5, 2025

ABSTRACT Achieving stable cycling of lithium metal batteries (LMBs) at high voltages presents a significant challenge due to interfacial instability and uneven lithium-ion transport, leading dendrite formation cathode degradation. Constructing solid-electrolyte interphase (SEI) that facilitates fast uniform ion transport is crucial for enhancing the stability electrode structures. However, current research mainly focuses on while neglecting which even more critical. In this study, we develop novel electrolyte system, PAFE, by incorporating aluminum ethoxide (Al(EtO)3), fluoroethylene carbonate (FEC), pentafluorocyclotriphosphazene (PFPN) into carbonate-based electrolyte. Al(EtO)3 serves as crosslinking agent, facilitating three-dimensional polymer network promotes deposition inorganic components such LiF, Li3N, Li3P Al2O3 within SEI cathode-electrolyte (CEI). These interphases lower activation energy thereby ensuring consistent flow reducing internal stress electrodes. As result, Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) cells with PAFE exhibit exceptional stability, retaining 80% capacity over 140 cycles cut-off voltage 4.7 V. Furthermore, 1 Ah pouch demonstrate excellent performance, highlighting potential system practical high-energy-density LMB applications.

Язык: Английский

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An oxygen-defective framework with intensified Lewis acidity reinforcing composite electrolyte for all-solid-state lithium metal batteries

Energy storage materials, Год журнала: 2024, Номер 73, С. 103847 - 103847

Опубликована: Окт. 18, 2024

Язык: Английский

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In situ polymerized ether-based polymer electrolytes towards practical lithium metal batteries

Chemical Communications, Год журнала: 2024, Номер unknown

Опубликована: Дек. 11, 2024

Commercial lithium-ion batteries that use flammable liquid electrolytes face significant safety risks, such as fires caused by electrolyte leaks. Solid polymer (SPEs) present a viable solution to this problem, with ether-based standing out due their superior stability and compatibility lithium metal. The

Язык: Английский

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