Journal article
Chemo-Mechanical Hysteresis of Sulfur Conversion Electrodes via Operando Acoustic Transmission
Journal of the Electrochemical Society, v 171(10)
26 Sep 2024
Abstract
Abstract The chemo-mechanics of lithium-sulfur (Li-S) batteries are unique in lithium-based batteries as sulfur undergoes a solid-liquid-solid transition during each half-cycle. The dissolution of sulfurous species in liquid electrolytes is a primary degradation mode in Li-S systems. While this challenge is well known, tracking and measuring sulfur liquefaction requires ex-situ experiments or hard-to-parallelize X-ray techniques. Here, we show that operando acoustic analyses can track both physicochemical phase changes and the mechanical dynamics of sulfur. We show time-of-flight can monitor sulfur phase changes during density and effective elastic moduli dynamics. Acoustic wave damping is highly sensitive to the state-of-matter transitions of the sulfur electrode. By accounting for cell dilation from Li plating and stripping, we show sulfur’s chemo-mechanical phase changes dominate time-of-flight’s nonlinear, non-monotonic signatures. By utilizing inter-cycle and intra-cycle time-of-flight trends, we develop a semi-quantitative method that can be calibrated to measure the dissolution of sulfur into the electrolyte and verify this with ex-situ TGA and XRD. Lastly, we pair acoustics with voltammetry to observe slow chemo-mechanical dynamics alongside the sluggish kinetics of sulfur utilization. Operando acoustic analyses can elucidate the chemo-mechanical dynamics of the sulfur electrode noninvasively and aid development efforts to slow and mitigate S migration.
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Details
- Title
- Chemo-Mechanical Hysteresis of Sulfur Conversion Electrodes via Operando Acoustic Transmission
- Creators
- Kerry SunGunnar ThorsteinssonAlexandra StiberLibby KatzmanWesley ChangRichard MayDaniel Steingart
- Publication Details
- Journal of the Electrochemical Society, v 171(10)
- Publisher
- ELECTROCHEMICAL SOC INC; PENNINGTON
- Number of pages
- 10
- Grant note
We acknowledge financial support by ICL Group. We thank Bret Schumacher for his insightful advice. This research used the Center for Nano Initiative at Columbia University. This research used the Columbia Electrochemical Energy Center at Columbia University. K. Sun: Conceptualization, Methodology, Data curation, Formal analysis, Writing - Original Draft. G. Thorsteinsson: Software, Methodology, Data curation, Formal analysis, Writing - Original Draft. A. Stiber: Data Curation, Investigation. L. Katzman: Resources, Methodology. W. Chang: Writing - Review & Editing. R. May: Writing - Review & Editing. D. A. Steingart: Writing - Review & Editing, Supervision, Funding acquisition, Project administration, Conceptualization.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Mechanical Engineering and Mechanics
- Web of Science ID
- WOS:001328743600001
- Scopus ID
- 2-s2.0-85207658762
- Other Identifier
- 991021905615704721
InCites Highlights
Data related to this publication, from InCites Benchmarking & Analytics tool:
- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Electrochemistry
- Materials Science, Coatings & Films