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High-Mass-Loading Li-S Batteries Catalytically Activated by Cerium Oxide: Performance and Failure Analysis under Lean
Shuting Fu1,2, Hongmin Wang1, Yiren Zhong1
1Department of Chemistry and Energy Sciences Institute, Yale University, 810 West Campus Drive, West Haven, CT, 06516, USA.
Developing advanced lithium-sulfur (Li-S) batteries requires high sulfur loading and minimal electrolyte. This study introduces CeOx nanostructures in carbon hosts, achieving high capacity and revealing a unique failure mode caused by lithium dendrites under lean electrolyte conditions.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- High-energy-density lithium-sulfur (Li-S) batteries face challenges with increasing sulfur mass loading and minimizing electrolyte.
- Previous work identified the potential-limiting step in Li-S batteries under lean electrolyte conditions.
Purpose of the Study:
- To advance the understanding of Li-S batteries by extending previous findings to a new catalyst and high sulfur loading.
- To develop a multifunctional 3D network for enhanced Li-S battery performance.
Main Methods:
- Integration of cerium oxide (CeOx) nanostructures into cotton-derived carbon to create a 3D network.
- Electrochemical testing of the S/CeOx/C electrode at high sulfur loading and low electrolyte/sulfur ratio.
- Analysis of failure mechanisms in Li-S cells under lean electrolyte conditions.
Main Results:
- The S/CeOx/C electrode achieved a stable areal capacity of 9 mAh cm-2 with a high sulfur loading of 14 mg cm-2 at an electrolyte/sulfur ratio of 5 µL mg-1.
- A previously overlooked failure pattern was discovered: local short-circuiting due to lithium dendrite penetration through the separator during charging at high current density.
- The developed material facilitates high active material hosting, electron transport, and catalysis of the sulfur lithiation reaction.
Conclusions:
- The study highlights the critical importance of developing novel material structures for Li-S batteries.
- Understanding and mitigating failure mechanisms, such as lithium dendrite growth under lean electrolyte conditions, is crucial for advancing Li-S battery technology.
- The multifunctional 3D network shows promise for high-performance Li-S batteries.
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