Film processing of Li6PS5Cl electrolyte using different binders and their combinations

Tron, Artur; Hamid, Raad; Zhang, Ningxin; Paolella, Andrea; Wulfert-Holzmann, Paul; Kolotygin, Vladislav; López-Aranguren, Pedro; Beutl, Alexander

doi:10.1016/j.est.2023.107480

Cited by 9 publications

(4 citation statements)

References 31 publications

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“…As we use a practical stack pressure of 2.5 MPa, the obtained ionic conductivities are lower than the theoretical value of LPSCl (∼1.0 × 10 −3 S cm −1 ) and some other reported values for similar systems, which are usually measured using impractical stack pressures (e.g. > 20 MPa) [34].…”

Section: Electrochemical Propertiescontrasting

confidence: 70%

“…TSEs prepared using both processing methods were found to show improved ionic conductivities with lower binder contents and higher densification pressures. As the binder is non-ionically conductive and would cover parts of the LPSCl particles, a higher proportion of it would reduce the overall conductivity of the TSEs while also reducing the effective contact area between the LPSCl particles and increasing the tortuosity of the Li + pathways [34]. On the other hand, the higher ionic conductivities with higher densification pressures arise from the reduced porosity, creating more ion-transport pathways and reducing the tortuosity across the TSEs.…”

Section: Electrochemical Propertiesmentioning

confidence: 99%

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Processing-structure-property relationships in practical thin solid-electrolyte separators for all-solid-state batteries

Li,

Kim,

Mezzomo

et al. 2024

J. Phys. Energy

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Scalable processing of thin and robust solid-electrolyte separators is key for the commercialization of high-energy all-solid-state batteries (ASSBs). Herein, we report the preparation of Li6PS5Cl-based thin solid-electrolyte separators incorporating suitable binders for potential use in ASSBs by two scalable wet processing techniques: tape-casting with nitrile-butadiene rubber (NBR) and calendering with carboxylated nitrile butadiene rubber (XNBR). By means of tensile testing and electrochemical impedance spectroscopy, the influence of processing on the mechanical as well as the electrochemical properties of the resulting thin solid-electrolyte separators is investigated. A trade-off between the mechanical and electrochemical properties is observed, which is due to the inextricably linked microstructures (particle size, binder content and distribution, and porosity) induced by the two different processes. Thin solid-electrolyte separators prepared using the tape-casting method with the more well-distributed binder network demonstrate superior tensile mechanical properties compared to the ones prepared by the calendering method. The results provide insights into the processing-structure-property relationships of the thin solid-electrolyte separators, which will contribute to advancing the application of practical thin solid electrolytes in ASSBs.

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Section: Electrochemical Propertiescontrasting

confidence: 70%

Section: Electrochemical Propertiesmentioning

confidence: 99%

Processing-structure-property relationships in practical thin solid-electrolyte separators for all-solid-state batteries

Li,

Kim,

Mezzomo

et al. 2024

J. Phys. Energy

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“…[27,28] Separator layers can be coated directly onto one electrode [8,13] or onto a release film to produce a free-standing sheet. [25,29,30] In this case, the separator has to be laminated onto one electrode by calendering, for example. [6] One benefit of this route over a direct coating onto one electrode is that a mutual dissolution of the binder by renewed contact with the solvent can be avoided.…”

Section: Introductionmentioning

confidence: 99%

Opportunities and Challenges of Calendering Sulfide‐Based Separators for Solid‐State Batteries

Heck,

Scharmann,

Osenberg

et al. 2024

Batteries & Supercaps

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Continuous densification procedures such as calendering are crucial for sulfide‐based solid‐state batteries to realize industry‐relevant processing. Therefore, this study investigates the impact of line load, roller circumferential speed and roll temperature on slurry‐based Li3PS4 and Li6PS5Cl separators compressed by a lab‐calender installed in an argon‐gas filled glovebox. While Li3PS4 layer become fragile in compressed state, the tested Li6PS5Cl separator is more suitable for calendering due to better mechanical stability. Next to basic analysis of, for example, density, length expansion, pore size distribution and specific ionic conductivity, 3D structures are generated based on images obtained by synchrotron tomography. All calendered separators showed particle breakage of the Li6PS5Cl. A slight decrease of the specific ionic conductivity with increased applied line load or pressure, respectively, is observed for both calendering and uniaxial pressing. However, expected increase of the conductivity was obtained for an increase of the stack pressure. Next to poorer contacting at low stack pressure, it is assumed that springback effect after densification could affect negatively the microstructure of the separator. These results highlight the opportunities and challenges in terms of calendering of sulfide‐based separators, as well as the complex correlations between densification, stack pressure and choice of material.

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“…Therefore, wet-chemical processing for the preparation of smalland large-scale cathodes, anodes, and electrolyte films is deemed to be more scalable than dry processing. However, the main issue related to films prepared via wet chemistry routes is the high chemical reactivity of sulfide electrolytes towards conventionally used solvents and binders, as previously reported [19,23,[28][29][30].…”

Section: Introductionmentioning

confidence: 99%

New Insights of Infiltration Process of Argyrodite Li6PS5Cl Solid Electrolyte into Conventional Lithium-Ion Electrodes for Solid-State Batteries

Tron,

Paolella,

Beutl

2023

Batteries

Self Cite

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All-solid-state lithium-ion batteries based on solid electrolytes are attractive for electric applications due to their potential high energy density and safety. The sulfide solid electrolyte (e.g., argyrodite) shows a high ionic conductivity (10−3 S cm−1). There is an open question related to the sulfide electrode’s fabrication by simply infiltrating methods applied for conventional lithium-ion battery electrodes via homogeneous solid electrolyte solutions, the structure of electrolytes after drying, chemical stability of binders and electrolyte, the surface morphology of electrolyte, and the deepening of the infiltrated electrolyte into the active materials to provide better contact between the active material and electrolyte and favorable lithium ionic conduction. However, due to the high reactivity of sulfide-based solid electrolytes, unwanted side reactions between sulfide electrolytes and polar solvents may occur. In this work, we explore the chemical and electrochemical properties of the argyrodite-based film produced by infiltration mode by combining electrochemical and structural characterizations.

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Film processing of Li6PS5Cl electrolyte using different binders and their combinations

Cited by 9 publications

References 31 publications

Processing-structure-property relationships in practical thin solid-electrolyte separators for all-solid-state batteries

Processing-structure-property relationships in practical thin solid-electrolyte separators for all-solid-state batteries

Opportunities and Challenges of Calendering Sulfide‐Based Separators for Solid‐State Batteries

New Insights of Infiltration Process of Argyrodite Li6PS5Cl Solid Electrolyte into Conventional Lithium-Ion Electrodes for Solid-State Batteries

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