Surface modification of garnet fillers with a polymeric sacrificial agent enables compatible interfaces of composite solid-state electrolytes

Luo, Bin; Wu, Jintian; Zhang, Ming; Zhang, Zhihao; Zhang, Xingwei; Fang, Zixuan; Xu, Ziqiang; Wu, Mengqiang

doi:10.1039/d3sc04710e

Chem. Sci.

2023

DOI: 10.1039/d3sc04710e

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Surface modification of garnet fillers with a polymeric sacrificial agent enables compatible interfaces of composite solid-state electrolytes

Bin Luo,

Jintian Wu,

Ming Zhang

et al.

Abstract: The poly (vinylidene fluoride) (PVDF)-based composite solid-state electrolyte (CSE) has garnered attention due to its excellent comprehensive performance. However, challenges persist in the structural design and preparation process of the...

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2024

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Cited by 4 publications

References 55 publications

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Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte

Wang,

Yuan,

Liu

et al. 2024

Adv Funct Materials

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Composite solid electrolytes (CSEs) integrate the fast ion conductivity of inorganic electrolytes and the excellent interfacial compatibility of polymer electrolytes. Typically, fluoropolymers and garnets are promising individuals to formulate cutting‐edge CSEs owing to their unique properties. However, the alkaline garnets can induce the dehydrofluorination of fluoropolymers, deteriorating their CSEs performance. Here, for the first time, NH4HCO3 is proposed as a sacrificial inhibitor to effectively prevent the garnet‐induced dehydrofluorination, using Li6.4La3Zr1.4Ta0.6O12 (LLZTO) and poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVH) as symbolic garnets and fluoropolymers, respectively. Various findings demonstrate that NH4HCO3 can buffer the alkalinity of LLZTO, thereby inhibiting the dehydrofluorination of PVH. In addition, NH4HCO3 can completely decompose to volatiles upon drying without compromising the properties of LLZTO and PVH. Additionally, a polymer‐in‐salt strategy is further introduced by adding high‐concentration LiTFSI salt to the above system, resulting in the PVH/LiTFSI/LLZTO (PLL) CSEs. Benefiting from the synergetic coupling of the sacrificial inhibitor and polymer‐in‐salt strategies, the PLL exhibits an exceptionally high ionic conductivity of 1.2 mS cm−1 at 25 °C and stable voltage of 5.09 V, outperforming other reported CSEs. Consequently, the PLL delivers impressive high‐rate cyclability in solid‐state lithium‐metal batteries with an outstanding capacity retention of 95.4% after 240 cycles at 1 C (25 °C).

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Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte

Wang,

Yuan,

Liu

et al. 2024

Adv Funct Materials

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Understanding Li6.24La3Zr2Al0.24O11.98 effect on poly(ionic liquid)-based electrolytes for high voltage solid-state lithium batteries working at room temperature

Villacis-Segovia,

Del Olmo,

Olmedo Martínez

et al. 2024

Chemical Engineering Journal

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Improving the interfacial stability of ultrahigh-nickel cathodes with PEO-based electrolytes by targeted chemical reactions

Dai,

Hou,

Luo

et al. 2024

Chem. Sci.

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Surface modification of garnet fillers with a polymeric sacrificial agent enables compatible interfaces of composite solid-state electrolytes

Abstract: The poly (vinylidene fluoride) (PVDF)-based composite solid-state electrolyte (CSE) has garnered attention due to its excellent comprehensive performance. However, challenges persist in the structural design and preparation process of the...

Cited by 4 publications

References 55 publications

Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte

Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte

Understanding Li6.24La3Zr2Al0.24O11.98 effect on poly(ionic liquid)-based electrolytes for high voltage solid-state lithium batteries working at room temperature

Improving the interfacial stability of ultrahigh-nickel cathodes with PEO-based electrolytes by targeted chemical reactions

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Surface modification of garnet fillers with a polymeric sacrificial agent enables compatible interfaces of composite solid-state electrolytes

Abstract: The poly (vinylidene fluoride) (PVDF)-based composite solid-state electrolyte (CSE) has garnered attention due to its excellent comprehensive performance. However, challenges persist in the structural design and preparation process of the...

Cited by 4 publications

References 55 publications

Sacrificial NH4HCO3 Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm−1 and 5V‐Level Composite Solid Electrolyte

Sacrificial NH4HCO3 Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm−1 and 5V‐Level Composite Solid Electrolyte

Understanding Li6.24La3Zr2Al0.24O11.98 effect on poly(ionic liquid)-based electrolytes for high voltage solid-state lithium batteries working at room temperature

Improving the interfacial stability of ultrahigh-nickel cathodes with PEO-based electrolytes by targeted chemical reactions

Contact Info

Product

Resources

About

Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte

Sacrificial NH₄HCO₃ Inhibits Fluoropolymer/Garnet Interfacial Reactions Toward 1mS cm⁻¹ and 5V‐Level Composite Solid Electrolyte