DataVXACS Energy LettersPaper
journal article·2026-05-08Open access

Early Onset Degradation Mechanism in All Solid-State Batteries Revealed by Operando Photoelectron Spectroscopy

Katherine A. Mazzio, Elmar Kataev, Francesco Piccolo, Florian Ruske, Raul Garcia-Diez, Regan Wilks, Marcus Bär, Philipp Adelhelm

ACS Energy Letters· Volume 11· Issue 5
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Abstract

High Resolution Image Download MS PowerPoint Slide Solid-state batteries (SSBs) promise enhanced safety and energy density, yet their long-term stability is limited by poorly understood interfacial degradation. Here, we perform operando hard X-ray photoelectron spectroscopy (HAXPES) on device-relevant structures, enabling depth-resolved probing of electrodes during cycling to follow lithiation and interfacial degradation processes in TiS 2 |Li 3 YCl 6 half cells. We identify a reduction process for Li 3 YCl 6 . Concurrently, oxygen-containing species are found to migrate toward the cathode current collector, where they react with TiS 2 to form an amorphous TiO x layer that contributes to capacity fade during extended cycling. Depth-dependent measurements confirm that oxygen enrichment is localized near the surface, establishing a kinetically driven degradation pathway linked to electron injection during discharge. These insights reveal how electrochemically induced migration of oxygen-containing species and interfacial redox can drive degradation in SSBs, providing a mechanistic basis for strategies to improve interfacial stability and cycling performance.
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Research context

Energy storage

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Chemical Technologies and Analytics, TU Wien, Getreidemarkt 9, Vienna, 1060, Austria

X-Ray Center, TU Wien, Lehargasse 4, Vienna, 1060, Austria

Department of Chemistry, Humboldt University of Berlin, Brook-Taylor-Str. 2, 12489 Berlin, Germany

Joint Research Group Operando Battery Analysis, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB), Hahn-Meitner-Platz 1, 14109 Berlin, Germany

Department of Interface Design, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB), Albert-Einstein-Str. 15, 12489 Berlin, Germany

Energy Materials In-Situ Laboratory Berlin (EMIL), Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB), Albert-Einstein-Str. 15, 12489 Berlin, Germany

Department of Active Materials and Interfaces for Stable Perovskite Solar Cells, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB), Kekuléstraße 5, 12489 Berlin, Germany

Department of X-ray Spectroscopy at Interfaces of Thin Films, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (HI-ERN), Albert-Einstein-Str. 15, 12489 Berlin, Germany

Department of Chemistry and Pharmacy, Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Egerlandstr. 3, 91058 Erlangen, Germany

Funding

Bundesministerium für Bildung und Forschung · Deutsche Forschungsgemeinschaft · Humboldt-Universität zu Berlin

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