High-conductivity free-standing Li6PS5Cl/poly(vinylidene difluoride) composite solid electrolyte membranes for lithium-ion batteries

Wang, Shuo; Zhang, Xue; Liu, Sijie; Xin, Chengzhou; Xue, Chuanjiao; Richter, Felix H.; Li, Liangliang; Fan, Li‐Zhen; Lin, Yuanhua; Shen, Yang; Janek, Jürgen; Chen, Nan

doi:10.1016/j.jmat.2019.12.010

Cited by 60 publications

(59 citation statements)

References 19 publications

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“…It can be seen that all of the three samples show the main peaks of LPSCl. No characteristic peaks of PEO and LiTFSI were detected, which can be attributed to the formation of amorphous phases in the synthesis process [40]. The temperature-dependent ionic conductivities of sulfide-based CSEs with different LPSCl:PEO ratios were illustrated in Fig.…”

Section: Resultsmentioning

confidence: 98%

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

Zhou

Liang

et al. 2021

Journal of Energy Chemistry

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Section: Resultsmentioning

confidence: 98%

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

Zhou

Liang

et al. 2021

Journal of Energy Chemistry

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“…[1][2][3] Most ASSB concepts rely on replacing the (flammable) liquid electrolyte by solid electrolyte and the graphite anode by lithium metal, while retaining a layered transition metal oxide as cathode material. [4][5][6][7][8][9][10] Additionally, the introduction of conversion-type <1 mAh cm −2 ) owing to low active material loading. [13][14][15][25][26][27][28][29][30][31] Several ASSBs with conversion-type cathodes exhibit high areal capacities (up to 4 mAh cm −2 ), but these degrade rapidly during cycling.…”

Section: Introductionmentioning

confidence: 99%

“…[43][44][45] Moreover, only few reports try to elucidate the complex electrochemical reaction mechanism. [38,[41][42][43][44][45] For example, it has recently been reported that in the Li 6 PS 5 Cl-C composite cathode Li 6 PS 5 Cl decomposes upon initial reduction into LiCl, Li 2 S and Li 3 P, which could be then oxidized into S and P 2 S 7 4− during a full charge step. [45] Moreover, in situ pressure measurements have been utilized to monitor lithiation/delithiation of intercalation-type cathodes.…”

Section: Introductionmentioning

confidence: 99%

Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid‐State Batteries with Long Cycle Life

Wang

Tang

Zhang

et al. 2021

Advanced Energy Materials

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All‐solid‐state batteries with conversion‐type cathodes promise to exceed the performance of lithium‐ion batteries due to their high theoretical specific energy and potential safety. However, the reported performance of solid‐state batteries is still unsatisfactory due to poor electronic and ionic conduction in the composite cathodes. Here, in situ formation of active material as well as highly effective ion‐ and electron‐conducting paths via electrochemical decomposition of Li6PS5Cl0.5Br0.5 (LPSCB)/multiwalled carbon nanotube mixtures during cycling is reported. Effectively, the LPSCB electrolyte forms a multiphase conversion‐type cathode by partial decomposition during the first discharge. Comprehensive characterization, especially operando pressure monitoring, reveals a co‐redox process of two redox‐active elements during cycling. The monolithic LPSCB‐based cell shows stable cycling over 1000 cycles with a very high capacity retention of 94% at high current density (0.885 mA cm−2, ≈0.7 C) at room temperature and a high areal capacity of 12.56 mAh cm−2 is achieved.

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“…[1,2] The solid electrolyte (SE) is the key component in ASSBs and has been extensively explored for several decades. [3,4] Among the different types of solid electrolytes, lithium thiophosphates have attracted ever-increasing attention for ASSBs due to their very high ionic conductivity and facile processing at room temperature. [5,6] Recent theoretical simulations suggest that the ionic conductivity of SEs in ASSB cathodes needs to reach at least 10 -2 S cm -1 in order to obtain comparable performance with commercial lithium-ion batteries with liquid electrolytes-a target that may only be achieved with thiophosphate electrolytes.…”

mentioning

confidence: 99%

Influence of Crystallinity of Lithium Thiophosphate Solid Electrolytes on the Performance of Solid‐State Batteries

Wang

Zhang

Chen

et al. 2021

Advanced Energy Materials

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achieve high safety and competitive energy and power density. [1,2] The solid electrolyte (SE) is the key component in ASSBs and has been extensively explored for several decades. [3,4] Among the different types of solid electrolytes, lithium thiophosphates have attracted ever-increasing attention for ASSBs due to their very high ionic conductivity and facile processing at room temperature. [5,6] Recent theoretical simulations suggest that the ionic conductivity of SEs in ASSB cathodes needs to reach at least 10 -2 S cm -1 in order to obtain comparable performance with commercial lithium-ion batteries with liquid electrolytes-a target that may only be achieved with thiophosphate electrolytes. [7] Therefore, significant research effort is spent on improving the ionic conductivity of thiophosphate SEs. [8,9] Glasses in the quasi-binary system xLi 2 S•yP 2 S 5 prepared by mechanical ball milling exhibit a conductivity of up to 10 -4 S cm -1 (e.g., 75Li 2 S•25P 2 S 5 glass [7525-glass], 70Li 2 S•30P 2 S 5 glass [7030-glass]) at room temperature. [10] The conductivity is enhanced by the precipitation of metastable phases upon heating, forming glass-ceramic dispersions: crystalline phases in an amorphous matrix, in this work denoted as "gc". [11] Although very high ionic conductivities above 10 mS cm -1 have been achieved in some Solid electrolytes (SEs) largely define the properties of all-solid-state batteries (ASSBs) and are expected to improve their safety, stability, and performance. Their ionic conductivity has much improved in recent years, enabling higher power and energy density. However, more subtle parameters, such as crystallinity, may also influence the electrochemical performance of cells. In this work, the correlation between the performance of ASSBs and thiophosphate SEs having the same stoichiometry, but different crystallinity is investigated. In In/InLi | SE | LiCoO 2 @ LiNb 0.5 Ta 0.5 O 3 model cells, better cycling and rate performance is achieved when using glass/glass-ceramic SEs (e.g., 75Li 2 S•25P 2 S 5 glass, 70Li 2 S•30P 2 S 5 glass, and Li 6 PS 5 Cl glass-ceramic). This can be mostly attributed to the mitigation of contact loss by the glass/glass-ceramic SEs compared to their crystalline SE counterparts. Furthermore, the SE decomposition at typical cathode potentials is investigated by using SE and carbon composites as cathodes. Larger volume changes and more severe decomposition are observed with crystalline SEs in the SE/carbon composite cathode after cycling. The crystalline SEs show higher electronic partial conductivity which results in more degradation in the composite cathode. This work sheds light on optimized composite cathode design for ASSB by carefully choosing solid electrolytes with appropriate mechanical and (electro-)chemical properties.

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High-conductivity free-standing Li6PS5Cl/poly(vinylidene difluoride) composite solid electrolyte membranes for lithium-ion batteries

Cited by 60 publications

References 19 publications

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid‐State Batteries with Long Cycle Life

Influence of Crystallinity of Lithium Thiophosphate Solid Electrolytes on the Performance of Solid‐State Batteries

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