Regulating Interfacial Chemistry to Boost Ionic Transport and Interface Stability of Composite Solid‐State Electrolytes for High‐Performance Solid‐State Lithium Metal Batteries

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 2, 2025

Abstract Composite solid‐state electrolytes (CSSEs) that combine the benefits of inorganic and polymer hold great potential for lithium metal batteries (SSLMBs) due to their high ionic conductivity superior mechanical properties. However, overall performance is severely hindered by several practical challenges, including component aggregation, poor interface behavior, limited Li + transport. Here, a unique ultrathin coating triaminopropyl triethoxysilane with bifunctional structure introduced effectively bridges fillers (Li 1+x Al x Ti 2‐x (PO 4 ) 3 , LATP) polyvinylidene fluoride hexafluoropropylene /polyethylene oxide matrix, thereby enabling high‐performance CSSEs (referred as SLPH). This design prevents LATP particle agglomeration, improves interfacial compatibility, ensures enrichment fast transport within SLPH. Consequently, SLPH exhibits low conduction energy barrier ( E = 0.462 eV), desirable (4.19 × 10 −4 S cm −1 at 60 °C), transference number 0.694). As result, SSLMBs SLPH, Li| |Li symmetric cells, LiFePO | coin‐type, pouch demonstrate rate capability long‐time cycling stability. work underscores significance surface functionalization create stable solid‐solid enhance conduction, paving way in SSLMBs.

Язык: Английский

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Toward High‐Performance, Flexible, Photo‐Assisted All‐Solid‐State Sodium‐Metal Batteries: Screening of Solid‐Polymer‐Based Electrolytes Coupled with Photoelectrochemical Storage Cathodes

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 18, 2025

Abstract The advancement of photo‐assisted rechargeable sodium‐metal batteries with high energy efficiency, lightweight structure, and simplified design is crucial for the growing demand in portable electronics. However, addressing intrinsic safety concerns liquid electrolytes sluggish reaction kinetics existing photoelectrochemical storage cathodes (PSCs) remains a significant challenge. In this work, functionalized light‐driven composite solid electrolyte (CSE) fillers are systematically screened, optimized PSC materials employed to construct advanced solid‐state battery (PSSMB). To further enhance mechanical properties poly(ethylene oxide) compatibility CSE, natural lignocellulose incorporated, enabling fabrication flexible PSSMBs. situ tests density functional theory calculations reveal that electric field facilitated sodium salt dissociation, reduced interfacial resistance, improved ionic conductivity (0.1 mS cm −1 ). Meanwhile, energy‐level matching maximized utilization photogenerated carriers, accelerating enhancing interface between cathode. resulting pouch‐type PSSMB demonstrates remarkable discharge capacity 117 mAh g outstanding long‐term cycling stability, retaining 89.1% its achieving an efficiency 96.8% after 300 cycles at 1 C. This study highlights versatile strategy advancing safe, high‐performance batteries.

Язык: Английский

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Tailoring Multiple Interactions in Poly (Urethane‐Urea)‐Based Solid‐State Polymer Electrolytes for Long‐Term Cycling Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 10, 2025

Abstract Polyethylene oxide (PEO)‐based solid polymer electrolytes (SPEs) are considered as one of the most promising candidates for next‐generation lithium metal batteries. However, their application is limited by poor electrode/electrolyte interfacial stability, low Li‐ions transference number, and weak mechanical strength. Herein, poly (urethane‐urea)‐based SPEs developed to enhance improve transport kinetics, provide superior properties. The (urethane‐urea) structure integrates abundant polar groups rigid conjugated moieties, which facilitate interactions with anions salt in SPEs, promoting number supporting formation a LiF‐rich electrolyte interphase (SEI) guide uniform deposition suppress dendrite growth. Furthermore, supramolecular crosslinked network formed through multiple hydrogen bonds π‐π stacking interactions, enhancing strength toughness SPEs. As result, Li//Li solid‐state symmetric cells assembled this SPE demonstrate stable cycling over 3000 h, while LiFePO 4 retain 93.6% initial capacity after 500 cycles at rate 1C. This work presents feasible design strategy developing highly functional materials.

Язык: Английский

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Stabilizing Sodium Metal Anodes by Functional Polymers

Materials Today Energy, Год журнала: 2024, Номер 45, С. 101664 - 101664

Опубликована: Авг. 10, 2024

Язык: Английский

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Thermal stability of PVDF-HFP based gel electrolyte for high performance and safe lithium metal batteries

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 157725 - 157725

Опубликована: Ноя. 1, 2024

Язык: Английский

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A Thermally Robust Biopolymeric Separator Conveys K⁺ Transport and Interfacial Chemistry for Longevous Potassium Metal Batteries

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 15, 2025

Potassium metal batteries (KMBs) hold promise for stationary energy storage with certain cost and resource merits. Nevertheless, their practicability is greatly handicapped by dendrite-related anodes, the target design of specialized separators to boost anode safety in its nascent stage. Here, we develop a thermally robust biopolymeric separator customized via solvent-exchange amino-siloxane decoration strategy render durable safe KMBs. Through experimental investigation theoretical computation, reveal that optimized porosity surface functionalization could manage ion transport interfacial chemistry, thereby enabling efficient K+ diffusion favorable solid electrolyte interphase achieve prolonged cycling stability (over 3000 h). The thus-assembled full cell retains 80% initial capacity after 400 cycles at 0.5 A g–1. heat-proof property designed further demonstrated. Our separator, affording multifunctional features, provides an appealing solution circumvent instability issues associated potassium batteries.

Язык: Английский

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Fluorinated Functional Units for Li⁺ Flux Homogenization in Silica Framework‐Based Zwitterionic Single Ion Conductors for Stable Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 31, 2025

Abstract Progress in commercializing solid polymer electrolytes (SPEs) for lithium metal batteries (LMBs) has been impeded by challenges, like concentration polarization, non‐uniform Li + flux, and an unstable electrolyte interface (SEI), which contribute to dendrite formation. To address these issues, silica framework (SF)‐based single‐ion conductors are proposed, featuring a unique solvation channel composed of fluorinated segment, high‐dipole zwitterion, rotation‐motion‐driven ion‐hopping medium. This design promotes low resistance at the cathode/electrode interface, suppresses growth anode/electrolyte maintains uniform flux. results show that continuous ion channels within robust enhance Li‐ion dissociation transport, achieving high ionic conductivity (σ DC = 8.8 × 10 −4 S cm −1 ), modulus 0.9 GPa, transference number (≈0.83), extended electrochemical stability window (up 5.2 V) 25 °C. fosters formation hybrid organic/inorganic SEI layer 2 CO 3 , LiF, O, enabling ultra‐stable plating/stripping over 4000 h 0.1 mA −2 . Furthermore, full cells demonstrate excellent rate performance long‐term cycling capacity retention (81% Li||LFP 86% Li||NCM811 after 400 cycles 1 C) coulombic efficiency, offering promising strategy stable LMBs.

Язык: Английский

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Solid polymer electrolyte supported by an asymmetric porous polymer membrane for thermally stable and high-energy lithium metal batteries

Journal of Power Sources, Год журнала: 2025, Номер 633, С. 236441 - 236441

Опубликована: Фев. 7, 2025

Язык: Английский

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A Zwitterion Coupled All‐Solid‐State Single Ion Conducting Polymer Electrolyte via Photoinitiated Thiol‐Ene Click Polymerization

Macromolecular Rapid Communications, Год журнала: 2025, Номер unknown

Опубликована: Фев. 7, 2025

The all-solid-state single ion conducting polymer electrolyte has a bottleneck in ionic conductivity even though it can prevent concentration polarization. Here, lithium 3,3'-(diallylammonio)bis(propane-1-sulfonyl(trifluoromethyl sulfonyl)imide) (LiDAA(PSI)2) with symmetrical "one positive, two negative" structure and unsaturated double bonds for propagation, is synthesized. LiDAA(PSI)2 copolymerized 1,2-ethanedithiol poly(ethylene glycol) diacrylate via photoinitiated thiol-ene click polymerization forms random copolymer, SPZ short. For comparison, 3-(diallylamino)propane-1-sulfonyl(trifluoromethyl (LiDAAPSI) corresponding copolymer SP are 7Li resonance peak position of shifts to low-field compared that LiDAAPSI, indicating weaker electrostatic attraction. responsible the shift, taking effect charge conjugation. Unsurprisingly, 1.69e-5 S cm-1 at 60 °C, which 1.9 times SP. Lithium electroplating stripping 0.0125 mA [email protected] mAh cm-2 °C performed. An metal secondary battery demonstrated. Zwitterion coupled possesses structure, conjugation weaken interaction, inspires design synthesis electrolytes zwitterion effect.

Язык: Английский

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Surface‐Confined Disordered Hydrogen Bonds Enable Efficient Lithium Transport in All‐Solid‐State PEO‐Based Lithium Battery

Angewandte Chemie, Год журнала: 2025, Номер unknown

Опубликована: Фев. 17, 2025

Abstract Polyethylene oxide (PEO)‐based electrolytes are essential to advance all‐solid‐state lithium batteries (ASSLBs) with high safety/energy density due their inherent flexibility and scalability. However, the inefficient Li + transport in PEO often leads poor rate performance diminished stability of ASSLBs. The regulation intermolecular H‐bonds is regarded as one most effective approaches enable efficient transport, while practical performances hindered by electrochemical instability free H‐bond donors constrained mobility highly ordered H‐bonding structures. To overcome these challenges, we develop a surface‐confined disordered system stable donor‐acceptor interactions construct loosened chain segments/ions arrangement bulk phase PEO‐based electrolytes, realizing crystallization inhibition PEO, weak coordination entrapment anions, which conducive deposition. rationally designed LiFePO 4 ‐based ASSLB demonstrates long cycle‐life over 400 cycles at 1.0 C 65 °C capacity retention 87.5 %, surpassing currently reported polymer‐based This work highlights importance confined on an battery system, paving way for future design

Язык: Английский

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