Unlocking Failure Mechanisms and Improvement of Practical Li–S Pouch Cells through In Operando Pressure Study

Chinnam, Parameswara R.; Xu, Leidong; Cai, Lu; Cordes, Nikolaus L.; Kim, Sangwook; Efaw, Corey Michael; Murray, Daniel J.; Dufek, Eric J.; Xu, Hongyi; Li, Bin

doi:10.1002/aenm.202103048

Unlocking Failure Mechanisms and Improvement of Practical Li–S Pouch Cells through In Operando Pressure Study

Journal Article · Tue Dec 07 00:00:00 EST 2021 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202103048· OSTI ID:1923024

Chinnam, Parameswara R. ^[1]; Xu, Leidong ^[2]; Cai, Lu ^[1]; ^[1]; Kim, Sangwook ^[1]; ^[1]; ^[1]; ^[1]; Xu, Hongyi ^[2]; ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)
University of Connecticut, Storrs, CT (United States)

For Lithium-sulfur (Li-S) battery commercialization, the study at a pouch cell level is essential, as some problems ignored or deemed minimal at the smaller level could have a greater effect on the performance of the larger pouch cell. Herein, the failure mechanisms of Li-S pouch cells are deeply investigated via in operando pressure analysis. It is found that highly porous structures of cathodes/separators and slow electrolyte diffusion through cathodes/separators can both lead to poor initial wetting. Additionally, Li-metal anode dominates the thickness variation of the whole pouch cell, which is verified by in situ measured pressure variation. Consequently, a real-time approach that combined normalized pressure with dP/dV analysis is proposed and validated to diagnose the morphology evolution of Li-metal anode. Moreover, applied pressure and porosity/tortuosity ratio of the cathode are both identified as independent factors that influence anode performance. In addition to stabilizing anodes, high pressure is proven to improve the cathode connectivity and avoid cathode cracking over cycling, which improves the possibility of developing cathodes with high sulfur mass loading. Here, this work provides insights into Li-S pouch cell design (e.g., cathode and separator) and highlights pathways to improve cell capacity and cycling performance with applied and monitored pressure.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1923024

Alternate ID(s):: OSTI ID: 23124011

Report Number(s):: INL/JOU-21-64698

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 7 Vol. 12; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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