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Interfacial studies between polymer and inorganic solid electrolytes for lithium solid-state batteries

Solid-state batteries (SSBs) have attracted considerable attention in recent years due to their potential advantages over conventional lithium-ion batteries, including higher energy density and enhanced safety. This is primarily achieved by replacing the flammable liquid electrolyte (LE) with a solid-state electrolyte (SSE). SSEs are broadly classified into inorganic solid electrolytes (SEs) and polymer electrolytes (PEs), each offering unique advantages and drawbacks. SEs generally exhibit high ionic conductivity but suffer from mechanical brittleness, whereas PEs provide superior mechanical flexibility and ease of processing, albeit with lower ionic conductivity.

To harness the complementary benefits of both, hybrid electrolytes (HEs), comprising both SE and PE phases have been developed. These systems aim to simultaneously achieve high ionic conductivity and mechanical compliance. However, the large interfacial resistance at the PE|ISE junction remains a major challenge, significantly impacting the performance of HEs. Despite its importance, this interface has not been extensively studied in the literature.

Our research focuses on developing a fundamental understanding of the PE|SE interface. We employ a four-electrode cell configuration to isolate and study interfacial phenomena via electrochemical impedance spectroscopy (EIS). To further investigate the chemical characteristics of the interface, we utilize surface-sensitive techniques such as time-of-flight secondary ion mass spectrometry (TOF-SIMS) and X-ray photoelectron spectroscopy (XPS). Our investigations explore the formation and evolution of interphases at unstable PE|SE interfaces and assess how factors such as the surface properties of different SEs and salt concentration in the polymer electrolyte influence interfacial resistance and degradation behavior.

Dieses Bild wurde eingereicht von Ujjawal Sigar (AG Dr. Felix Richter).

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