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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

DOI: 10.1039/C8CP01968A DOI Help

Authors: Christian Dietrich (Justus-Liebig-University Giessen) , Raimund Koerver (Justus-Liebig-University Giessen) , Michael W. Gaultois (University of Liverpool) , Gregor Kieslich (Technical University of Munich) , Giannantonio Cibin (Diamond Light Source) , Juergen Janek (Justus-Liebig-University Giessen; Karlsruhe Institute of Technology) , Wolfgang G. Zeier (Justus-Liebig-University Giessen)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Physical Chemistry Chemical Physics

State: Published (Approved)
Published: July 2018
Diamond Proposal Number(s): 13861

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 (LiS)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.

Subject Areas: Chemistry, Materials

Instruments: B18-Core EXAFS