Journal Article

PUBDB-2026-01702

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Effect of Stack Pressure on the Microstructure and Ionic Conductivity of the Slurry‐Processed Solid Electrolyte $Li_7SiPS_8$

Nguyen, D. H.Extern* ; Osenberg, M.Extern* ; Schneider, C. ; Moosmann, J.HZG*Hereon* ; Beckmann, F.HZG*Hereon* ; Manke, I.Extern* ; Lotsch, B. V.

2025
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/admi.202500845

Abstract: All-solid-state batteries (ASSBs) have gained much interest in recent yearsbecause they promise higher energy and power densities as well as improvedsafety over lithium-ion batteries (LIBs). This is achieved by using nonflammablesolid electrolytes (SEs) together with lithium metal or high-capacitysilicon anodes. One major hurdle to overcome is the permanent intimatecontact of all cell components to enable long-term cycling stability. This studyinvestigates the macroscopic (microstructure) and microscopic (atomistic)effects of uniaxial stack pressure on the transport properties of free-standing,slurry-processed tetragonal Li7SiPS8 (t-Li7SiPS8) sheets, containing differentsolid electrolyte (SE)-to-binder ratios (SE:B) and particle size fractions.The results demonstrate that binder content and particle size significantlyinfluence the morphology as evidenced by synchrotron-radiation computedtomography (CT), pressure response, and ionic conductivity of the sheets.Notably, while compression mechanics are consistent across samples, relativedensities, and ionic conductivities are more dependent on binder content thanparticle size. Larger particles and lower binder contents generally led to higherionic conductivities. The study also reveals that activation volumes appearto increase with binder content, suggesting that extrinsic factors, particularlythe binder, may obscure the calculation of the intrinsic activation volumesof t-Li7SiPS8. Thus, the obtained values for binder-containing sheets may beconsidered apparent values. Contrary to expectations, repeated compressioncycles led to a decreased ionic conductivity and relative density, likely due tomicrostructural damage and increased (apparent) activation volumes. Overall,the study serves as a reminder to the community to carefully interpret intrinsicvalues, such as the activation volume, and by extension the activationenergy, in the increasingly popular binder-containing SE sheet systems.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. Helmholtz-Zentrum Hereon (Hereon)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)

Experiment(s):

1. PETRA Beamline P07 (PETRA III)

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Database coverage:
; ; ; Article Processing Charges ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; DOAJ Seal ; Essential Science Indicators ; Fees ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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