A novel asymmetrical multilayered composite electrolyte for high-performance ambient-temperature all-solid-state lithium batteries

Wang, Zhen; Tan, Jiewen; Cui, Jiawu; Xie, Keyu; Bai, Yunfei; Jia, Zhanhui; Gao, Xiangwen; Wu, Yuping; Tang, Wei

doi:10.1039/d3ta07352a

Cited by 6 publications

(2 citation statements)

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“…It was observed that previous XPS peaks of the LFP correspond to the O 1s, Li 1s, P 2p, and Fe 2p peaks. 32,33 The fitting of the Li 1s spectra, as presented in Fig. 4a, revealed two peaks at 55.3 and 57.3 eV, which were attributed to Fe 3p and lattice lithium, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…Despite these advantages for the LFP cathode, the low inferior electric conductivity (10 −9 –10 −10 S cm −1 ) along with sluggish Li diffusion (10 −14 –10 −16 cm 2 s −1 ) resulting from the absence of a continuous coplanar octahedral network of FePO 4 and a PO 4 tetrahedron across the two-phase boundary are the primary limitations for practical applications of high-rate batteries. 32,33 As a result, numerous approaches have been considered to tackle the aforementioned drawbacks, such as coating with conductive carbonaceous materials, doping with metal ions, and optimizing particle size. 34–36 Among these strategies, the integration of LFP with unique conductive carbon material coatings has emerged as the most economical and efficient method for increasing the rate efficiency of LFP.…”

Section: Introductionmentioning

confidence: 99%

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Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄

Wang,

Li,

Zhu

et al. 2024

New J. Chem.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄

Wang,

Li,

Zhu

et al. 2024

New J. Chem.

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In situ Triggered Rich‐LiF/Mg Multifunctional Passivation Layer for Modifying the Anode Interface of All‐Solid‐State Lithium Metal Batteries

Wang,

Wu,

Hao

et al. 2024

Adv Funct Materials

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Lithium (Li) is a promising anode material for all‐solid‐state Li metal batteries (ASSLMBs) due to its high energy density. However, the interface incompatibility of Li/solid electrolyte and uneven Li deposition induces the penetration of Li dendrites. Herein, a multifunctional rich‐LiF/Mg artificial solid electrolyte interphase (SEI) layer is constructed from a MgF2‐PVDF‐HFP film to passivate the Li anode and achieve effective inhibition of Li dendrites. Notably, the triggered LixMg alloys rivet the Li6PS5Cl (LPSCl) electrolyte and Li anode together well, producing satisfactory interface contact and reducing overpotential. The mechanism of LiF and LixMg alloys to enhance the stability of the Li/LPSCl interface is further elucidated by density functional theory (DFT). Moreover, the synergistic interaction of LiF with high interfacial energy and LixMg alloys with low diffusion barrier promotes uniform deposition of Li during plating/stripping and structural stability. Therefore, the modified Li‐symmetric cell exhibits ultra‐high critical current density (2.0 mA cm−2) and considerable cyclic stability (more than 1000 h at 0.5 mA cm−2). Remarkably, NCM//LPSCl//3% MgF2‐PVDF‐HFP@Li ASSLMBs exhibit considerable long‐term cycle stability (86.9% capacity retention after 100 cycles at 0.2 C). This work highlights the critical role of the intermediate passivating layer in mitigating side reactions and preventing Li penetration.

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Lithium Dendrite Deflection at Mixed Ionic–Electronic Conducting Interlayers in Solid Electrolytes

Yu,

Gan,

Mijailovic

et al. 2024

Advanced Energy Materials

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Solid state lithium metal batteries using garnet solid electrolytes such as LLZTO (Li6.4La3Zr1.5Ta0.5O12) promise substantial improvements in energy density and safety. However, practical implementation is hindered by lithium dendrite penetration at high current densities. Recent work shows that internal electrochemically induced mechanical stresses are large enough to propagate lithium dendrites and subsequently fracture solid electrolytes. This study builds on this understanding and demonstrates that stress‐driven dendrite propagation can be controlled via deflection at weakly bonded internal interfaces. This approach, based on a fracture‐mechanics analysis of multilayered composites, is investigated with a variety of interlayer materials that are embedded into LLZTO. The viability and effectiveness of dendrite deflection are most clearly evident with reduced graphene oxide where the critical current density increased from 0.6 to 3.8 mA cm−2. In this material, both the weak interface with LLZTO and the mixed ionic–electronic conducting nature of the interlayer appear to contribute to the improved performance. Additional insight into the mechanics of multilayered electrolytes is also obtained with finite element modeling. The overall results present a promising proof‐of‐concept demonstration along with important generalized design guidelines for creating multilayered solid electrolyte architectures that can enable high‐performance solid‐state batteries.

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A novel asymmetrical multilayered composite electrolyte for high-performance ambient-temperature all-solid-state lithium batteries

Abstract: All-solid-state lithium batteries are considered promising next-generation devices for energy storage, but their application still faces various interfacial issues. In this work, an innovative asymmetric multi-layered solid composite electrolyte design...

Cited by 6 publications

References 57 publications

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄

In situ Triggered Rich‐LiF/Mg Multifunctional Passivation Layer for Modifying the Anode Interface of All‐Solid‐State Lithium Metal Batteries

Lithium Dendrite Deflection at Mixed Ionic–Electronic Conducting Interlayers in Solid Electrolytes

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A novel asymmetrical multilayered composite electrolyte for high-performance ambient-temperature all-solid-state lithium batteries

Abstract: All-solid-state lithium batteries are considered promising next-generation devices for energy storage, but their application still faces various interfacial issues. In this work, an innovative asymmetric multi-layered solid composite electrolyte design...

Cited by 6 publications

References 57 publications

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO4 cathode materials from spent LiFePO4

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO4 cathode materials from spent LiFePO4

In situ Triggered Rich‐LiF/Mg Multifunctional Passivation Layer for Modifying the Anode Interface of All‐Solid‐State Lithium Metal Batteries

Lithium Dendrite Deflection at Mixed Ionic–Electronic Conducting Interlayers in Solid Electrolytes

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Product

Resources

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Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄

Sustainable and facile synthesis of high-performance nitrogen-doped carbon/graphene@LiFePO₄ cathode materials from spent LiFePO₄