Observation of Dynamic Interfacial Layers in Li-Ion and Li-O2 Batteries by Scanning Electrochemical Microscopy

Bülter, Heinz; Schwager, Patrick; Fenske, Daniela; Wittstock, Günther

doi:10.1016/j.electacta.2016.02.212

Cited by 29 publications

(38 citation statements)

References 90 publications

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“…Figure a–c shows a series of SECM feedback images of an identical region of the HOPG basal plane using DBDMB as redox mediator at a ME–sample distance of d =7 μm. In contrast to earlier studies on graphite composites, metallic Li, and Si from this laboratory, we used Au MEs here because, as Pt MEs approached the HOPG, deactivation of the ME occurred instantaneously. This was prevented by the use of Au MEs.…”

Section: Resultssupporting

confidence: 55%

“…These observations of long‐term changes of SEI passivity over hours were also reported for graphite composite and Li . The complexity of long‐term SEI passivity changes as indicated in Figure was similar to the reported complexity at graphite composite electrodes …”

Section: Resultsmentioning

confidence: 99%

“…(i) Rather unlikely was a malfunction of the positioning system. Although positioning systems are susceptible to thermal drift, the thermal drift did not cause height changes in the μm range during 1–2 h in previous studies . (ii) More likely was an expansion and/or restructuring of the lithiated HOPG.…”

Section: Resultsmentioning

confidence: 99%

“…The solid–electrolyte interphase (SEI) on highly oriented pyrolytic graphite (HOPG) with a state of charge (SOC) of 18 % was investigated by the feedback mode of scanning electrochemical microscopy (SECM) using 2,5‐di‐ tert ‐butyl‐1,4‐dimethoxy benzene (DBDMB) as redox mediator. The local SEI passivity changed or remained constant on the timescale of hours as previously reported for SEI‐covered metallic Li and graphite composite electrodes . In addition, only a few short‐term changes of the SEI passivity between a few seconds and minutes were observed similar to metallic Li and in contrast to graphite composite electrodes.…”

Section: Discussionmentioning

confidence: 99%

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Scanning Electrochemical Microscopy for the In Situ Characterization of Solid–Electrolyte Interphases: Highly Oriented Pyrolytic Graphite versus Graphite Composite

2016

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The solid–electrolyte interphase (SEI) is of key importance for the performance and safety of lithium‐ion batteries. Recently, scanning electrochemical microscopy (SECM) has been used to study in situ the SEI. Here, we compare the SEI of graphite composite electrodes to the SEI at macroscopic samples of binder‐free, highly oriented pyrolytic graphite (HOPG) where effects of mechanical processing and particle–particle as well as electrolyte–binder interactions should be absent. Both, short‐term changes of SEI passivity on the timescale of seconds and minutes and long‐term changes over hours are found on HOPG as well as on graphite composite electrodes, but the SEI at HOPG is more stable compared to graphite composite electrodes. In addition, the microelectrode probe of the SECM is used to induce local SEI damage to monitor its reformation. Subsequently, secondary processes such as local crack formation, gas formation due to electrolyte reduction, and HOPG expansion are studied.

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Section: Resultssupporting

confidence: 55%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

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Scanning Electrochemical Microscopy for the In Situ Characterization of Solid–Electrolyte Interphases: Highly Oriented Pyrolytic Graphite versus Graphite Composite

2016

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“…Deviations between forward and reverse line scans at identical locations we denote as “short‐term events”. An example of a strong local increase of i T (solid curve) compared with the previous line scan is shown in Figure a, b (dotted curve) . The increase of i T was equivalent to a decrease of SEI passivity and could be as large as the i T value of the pristine graphite electrodes .…”

Section: Sei Investigation By the Feedback Mode Of Scanning Electrocmentioning

confidence: 99%

Review of Local In Situ Probing Techniques for the Interfaces of Lithium‐Ion and Lithium–Oxygen Batteries

et al. 2016

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Electrodes in lithium‐ion and post‐lithium‐ion batteries are made of composite materials exposing a variety of different surfaces towards the electrolyte. This causes a distribution of current densities and consequently locally different changes of interfaces and bulk materials that might be critical for the performance and durability of secondary batteries. The optimization of local structures of battery materials is hindered by a lack of local techniques that provide in situ reactivity information from such hidden interfaces. A variety of new electrochemical scanning probe techniques are currently adapted to the investigation of battery materials under near‐realistic environmental conditions. The review provides a critical assessment of this development with a particular emphasis on the assessment of the passivating properties of solid–electrolyte interphases, the extension of the concepts to lithium–oxygen cells, and attempts to image ion intercalation reactions.

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Korrelative elektrochemische Mikroskopie zur Aufklärung der lokalen ionischen und elektronischen Eigenschaften der Festkörper‐Elektrolyt Zwischenphase in Li‐Ionen‐Batterien

et al. 2022

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Die Festkörper-Elektrolyt-Zwischenphase (SEI) spielt eine Schlüsselrolle für die Stabilität von Lithium-Ionen-Batterien (LIB), da die SEI den kontinuierlichen Abbau des Elektrolyten an der Anode verhindert. Die SEI fungiert als isolierende Schicht für den Elektronentransfer und ermöglicht dennoch den Ionenfluss durch die Schicht. Wir kombinieren zum ersten Mal die Rückkopplungs-und Multifrequenz-Wechselstrommodi der elektrochemischen Rastermikroskopie (SECM), um die lokalen elektronischen und ionischen Eigenschaften der SEI quantitativ zu bewerten, indem wir die SEI-Bildungsbedingungen und die verwendeten Elektrolyte der Li-Ionen-Batterien variieren. Korrelationen zwischen den elektronischen und ionischen Eigenschaften der resultierenden SEI auf einer Modell-Cu-Elektrode zeigen die Machbarkeit der vorgeschlagenen Strategie, um die beiden wesentlichen Eigenschaften einer SEI zu quantifizieren: ionische und elektronische Leitfähigkeit in Abhängigkeit von den Bildungsbedingungen; Ergebnisse, die voraussichtlich einen signifikanten Einfluss auf den Bereich der LIBs haben werden.

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Observation of Dynamic Interfacial Layers in Li-Ion and Li-O2 Batteries by Scanning Electrochemical Microscopy

Cited by 29 publications

References 90 publications

Scanning Electrochemical Microscopy for the In Situ Characterization of Solid–Electrolyte Interphases: Highly Oriented Pyrolytic Graphite versus Graphite Composite

Scanning Electrochemical Microscopy for the In Situ Characterization of Solid–Electrolyte Interphases: Highly Oriented Pyrolytic Graphite versus Graphite Composite

Review of Local In Situ Probing Techniques for the Interfaces of Lithium‐Ion and Lithium–Oxygen Batteries

Korrelative elektrochemische Mikroskopie zur Aufklärung der lokalen ionischen und elektronischen Eigenschaften der Festkörper‐Elektrolyt Zwischenphase in Li‐Ionen‐Batterien

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