Thin, flexible sulfide-based electrolyte film and its interface engineering for high performance solid-state lithium metal batteries

Liu, Hong; He, Pingge; Wang, Guoxu; Liang, Yuhao; Wang, Chao; Fan, Louzhen

doi:10.1016/j.cej.2021.132991

Cited by 56 publications

(27 citation statements)

References 48 publications

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“…[9,14] The other daunting challenge is the poor interface compatibility because SSEs are prone to (electro)chemical reduction from the Li metal anode. [15,16] Moreover, that reduction reaction would cause uneven Li + deposition and thus result in the formation of Li dendrite at anode interface, which would penetrate through the SSEs and deteriorate the performance and lifetime of batteries. [17] Therefore, there are rare reports that SSEs can be used to directly match Li metal to manufacture superior ASSLMBs.…”

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confidence: 99%

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

Liu

Zhu

Wang

et al. 2022

Adv Funct Materials

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Sulfide solid electrolytes (SSEs) for all‐solid‐state Li metal batteries (ASSLMBs) are attracting increasing attention due to their ultrahigh ionic conductivity and good machinability. However, current SSEs generally suffer from inferior Li metal compatibility and poor air‐stability, which severely impede their practical applications for ASSLMBs. Herein, novel argyrodite‐based SSEs of Li6+2xP1−xBixS5−1.5xO1.5xCl are synthesized via the Bi, O co‐doping the Li6PS5Cl for the first time. By adjusting the concentrations of dopant, the optimized Li6.04P0.98Bi0.02S4.97O0.03Cl presents an ultrahigh ionic conductivity (3.4 × 10−3 S cm−1). Moreover, such electrolyte displays splendid structural stability after exposure to humid air and chlorobenzene, demonstrating admirable air‐stability and solvent‐stability. The mechanism of the enhanced air‐stability of oxide‐doped SSEs is profoundly understood by conducting first‐principles density functional theory calculations. In addition, the Li6.04P0.98Bi0.02S4.97O0.03Cl electrolyte triggers the generation of LiBi alloy at the anode interface, which plays a crucial role in reducing Li+ diffusion energy barriers and improving interfacial compatibility, leading to an ultrahigh critical current density of 1.1 mA cm−2 and splendid cyclic stability in Li symmetric cell. As a result, ASSLMBs equipped with either pristine or air‐exposed Li6.04P0.98Bi0.02S4.97O0.03Cl can deliver satisfying discharge specific capacity at room temperature.

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confidence: 99%

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

Liu

Zhu

Wang

et al. 2022

Adv Funct Materials

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“…Owing to in situ-constructed LiF-rich multifunctional interface, the Li@LiF/LGPS/LiF@Li symmetric cell delivers increased critical current density of 1.9 mA cm -2 with a capacity of 1.9 mAh cm -2 , which is one of the highest values for the LGPS electrolyte-based symmetric cells among reported literatures (Table S1, Supporting Information). [21,41,44,45] The effects of the in situ-formed LiF-rich multifunctional interface on electrochemical performances of the all-solid-state cells were further evaluated at 25 °C. As shown in Figure 4a and Figure S7 in the Supporting Information, the Li@LiF/LGPS/ LiCoO 2 all-solid-state cell exhibits excellent rate performances with reversible discharge capacities of 121.2, 115, 105.8, and 91.9 mAh g -1 at 0.1 C, 0.2 C, 0.5 C, and 1 C, respectively.…”

Section: Resultsmentioning

confidence: 99%

In Situ‐Formed LiF‐Rich Multifunctional Interfaces toward Stable Li₁₀GeP₂S₁₂‐Based All‐Solid‐State Lithium Batteries

Lin

Zhao

Weng

et al. 2022

Adv Materials Inter

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Li10GeP2S12 (LGPS) solid electrolyte with extremely high ionic conductivity is a promising candidate for all‐solid‐state lithium batteries. However, continued LGPS reduction at Li/LGPS interface is huge challenge. Thus, developing a simple and effective strategy to improve Li/LGPS interfacial stability is highly urgent. Herein, LiF‐rich multifunctional interfaces on Li metal (Li@LiF), consisting of three functional components of LiF, carbon particles, and thin CF bond top‐layer, are in situ constructed on the Li metal surface by spontaneous reaction between Li metal and poly(tetrafluoroethylene) at room temperature. LiF, as the main component, significantly suppresses the interfacial reaction due to low electronic conductivity and promotes smooth lithium plating on the Li metal surface arising from high interfacial energy against Li. Meanwhile, carbon particles with excellent Li+ affinity and thin strong polar CF bond top‐layer enable homogenous Li+ flux as well as fast Li+ migration across the LiF‐rich interface, respectively. Consequently, the LGPS‐based symmetric lithium cell possesses significantly prolonged cycling stability and increased critical current density. The LGPS‐based all‐solid‐state lithium cells employing LiCoO2 cathode and Li@LiF anode exhibit excellent rate capability and impressive cycling stability, achieving a high capacity retention of 80.9% over 300 cycles at 0.1 C under 25 °C.

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“…As a result, the as‐prepared SE–NW–SE and NW–SE–NW films are both free‐standing with a thin thickness of ~70 μm (Figure 15G). 372 Recently, Liu et al 384 shared a similar protocol by direct casting LGPS–PEO‐based slurry on a nylon mesh to fabricate sheet‐type SE membrane. After cold pressing, the SE membrane with a thickness of 60 μm exhibited sufficient mechanical strength and flexibility.…”

Section: Processing Strategiesmentioning

confidence: 99%

Challenges, interface engineering, and processing strategies toward practical sulfide‐based all‐solid‐state lithium batteries

Liang

Liu

Wang

et al. 2022

InfoMat

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All‐solid‐state lithium batteries have emerged as a priority candidate for the next generation of safe and energy‐dense energy storage devices surpassing state‐of‐art lithium‐ion batteries. Among multitudinous solid‐state batteries based on solid electrolytes (SEs), sulfide SEs have attracted burgeoning scrutiny due to their superior ionic conductivity and outstanding formability. However, from the perspective of their practical applications concerning cell integration and production, it is still extremely challenging to constructing compatible electrolyte/electrode interfaces and developing available scale processing technologies. This review presents a critical overview of the current underlying understanding of interfacial issues and analyzes the main processing challenges faced by sulfide‐based all‐solid‐state batteries from the aspects of cost‐effective and energy‐dense design. Besides, the corresponding approaches involving interface engineering and processing protocols for addressing these issues and challenges are summarized. Fundamental and engineering perspectives on future development avenues toward practical application of high energy, safety, and long‐life sulfide‐based all‐solid‐state batteries are ultimately provided.

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Thin, flexible sulfide-based electrolyte film and its interface engineering for high performance solid-state lithium metal batteries

Cited by 56 publications

References 48 publications

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

In Situ‐Formed LiF‐Rich Multifunctional Interfaces toward Stable Li₁₀GeP₂S₁₂‐Based All‐Solid‐State Lithium Batteries

Challenges, interface engineering, and processing strategies toward practical sulfide‐based all‐solid‐state lithium batteries

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Thin, flexible sulfide-based electrolyte film and its interface engineering for high performance solid-state lithium metal batteries

Cited by 56 publications

References 48 publications

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

High Air Stability and Excellent Li Metal Compatibility of Argyrodite‐Based Electrolyte Enabling Superior All‐Solid‐State Li Metal Batteries

In Situ‐Formed LiF‐Rich Multifunctional Interfaces toward Stable Li10GeP2S12‐Based All‐Solid‐State Lithium Batteries

Challenges, interface engineering, and processing strategies toward practical sulfide‐based all‐solid‐state lithium batteries

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In Situ‐Formed LiF‐Rich Multifunctional Interfaces toward Stable Li₁₀GeP₂S₁₂‐Based All‐Solid‐State Lithium Batteries