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Spectroscopic characterization of lithium thiophosphates by XPS and XAS – a model to help monitor interfacial reactions in all-solid-state batteries

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Abstract

Inspired by reports of redox active interphases in all-solid-state batteries employing fast conducting lithium thiophosphate solid-state electrolytes, we investigated the compositional depolymerization of interconnected PS4 tetrahedra in (Li2S)x(P2S5)100−x glasses (50 < x < 80) by X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS). Based on the observed energy shifts with composition, we present a structural model of the three different bonding types describing the structures of either crystalline or amorphous thiophosphates. This model and reference data characterizes amorphous thiophosphates based on their inter-tetrahedral connectivity and helps to distinguish malign decomposition reactions from reversible redox reactions at the cathode active material/solid-state electrolyte interface. This work highlights the importance of a combined analytical approach and appropriate reference compounds to elucidate the interface reactions in all-solid-state battery systems.

Graphical abstract: Spectroscopic characterization of lithium thiophosphates by XPS and XAS – a model to help monitor interfacial reactions in all-solid-state batteries

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Publication details

The article was received on 27 Mar 2018, accepted on 12 Jul 2018 and first published on 13 Jul 2018


Article type: Paper
DOI: 10.1039/C8CP01968A
Citation: Phys. Chem. Chem. Phys., 2018, Advance Article
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    Spectroscopic characterization of lithium thiophosphates by XPS and XAS – a model to help monitor interfacial reactions in all-solid-state batteries

    C. Dietrich, R. Koerver, M. W. Gaultois, G. Kieslich, G. Cibin, J. Janek and W. G. Zeier, Phys. Chem. Chem. Phys., 2018, Advance Article , DOI: 10.1039/C8CP01968A

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