skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Following the Transient Reactions in Lithium-Sulfur Batteries Using In an In Situ Nuclear Magnetic Resonance Technique

Abstract

Li-S batteries hold great potential for next-generation, large-format power source applications; yet, the fundamental understanding of the electrochemical reaction pathways remains lacking to enable their functionality as promised. Here, in situ NMR technique employing a specially designed cylindrical micro battery was used to monitor the chemical environments around Li+ ions during repetitive charge-discharge process and track the transient electrochemical and chemical reactions occurring in the whole Li-S system. The in situ NMR provides real time, quantitative information related to the temporal concentration variations of the polysulfides with various chain lengths, providing important clues for the reaction pathways during both discharge and charge processes. The in-situ technique also reveals that redox reactions may involve transient species that are difficult to detect in ex-situ NMR study. Intermediate species such as charged free radicals may play an important role in the formation of the polysulfide products. Additionally, in situ NMR measurement simultaneously reveals vital information on the 7Li chemical environments in the electrochemical and parasitic reactions on the lithium anode that promotes the understanding of the failure mechanism in the Li-S system. These new insights could help design effective strategies to accelerate the development of Li-S battery technology.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1182937
Report Number(s):
PNNL-SA-101779
44591; KC0208010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nano Letters, 15(5):3309-3316
Additional Journal Information:
Journal Name: Nano Letters, 15(5):3309-3316
Country of Publication:
United States
Language:
English
Subject:
Lithium Sulpher Batteries; In Situ NMR; Environmental Molecular Sciences Laboratory

Citation Formats

Xiao, Jie, Hu, Jian Z., Chen, Honghao, Vijayakumar, M., Zheng, Jianming, Pan, Huilin, Walter, Eric D., Hu, Mary Y., Deng, Xuchu, Feng, Ju, Liaw, Bor Yann, Gu, Meng, Deng, Zhiqun, Lu, Dongping, Xu, Suochang, Wang, Chong M., and Liu, Jun. Following the Transient Reactions in Lithium-Sulfur Batteries Using In an In Situ Nuclear Magnetic Resonance Technique. United States: N. p., 2015. Web. doi:10.1021/acs.nanolett.5b00521.
Xiao, Jie, Hu, Jian Z., Chen, Honghao, Vijayakumar, M., Zheng, Jianming, Pan, Huilin, Walter, Eric D., Hu, Mary Y., Deng, Xuchu, Feng, Ju, Liaw, Bor Yann, Gu, Meng, Deng, Zhiqun, Lu, Dongping, Xu, Suochang, Wang, Chong M., & Liu, Jun. Following the Transient Reactions in Lithium-Sulfur Batteries Using In an In Situ Nuclear Magnetic Resonance Technique. United States. doi:10.1021/acs.nanolett.5b00521.
Xiao, Jie, Hu, Jian Z., Chen, Honghao, Vijayakumar, M., Zheng, Jianming, Pan, Huilin, Walter, Eric D., Hu, Mary Y., Deng, Xuchu, Feng, Ju, Liaw, Bor Yann, Gu, Meng, Deng, Zhiqun, Lu, Dongping, Xu, Suochang, Wang, Chong M., and Liu, Jun. Wed . "Following the Transient Reactions in Lithium-Sulfur Batteries Using In an In Situ Nuclear Magnetic Resonance Technique". United States. doi:10.1021/acs.nanolett.5b00521.
@article{osti_1182937,
title = {Following the Transient Reactions in Lithium-Sulfur Batteries Using In an In Situ Nuclear Magnetic Resonance Technique},
author = {Xiao, Jie and Hu, Jian Z. and Chen, Honghao and Vijayakumar, M. and Zheng, Jianming and Pan, Huilin and Walter, Eric D. and Hu, Mary Y. and Deng, Xuchu and Feng, Ju and Liaw, Bor Yann and Gu, Meng and Deng, Zhiqun and Lu, Dongping and Xu, Suochang and Wang, Chong M. and Liu, Jun},
abstractNote = {Li-S batteries hold great potential for next-generation, large-format power source applications; yet, the fundamental understanding of the electrochemical reaction pathways remains lacking to enable their functionality as promised. Here, in situ NMR technique employing a specially designed cylindrical micro battery was used to monitor the chemical environments around Li+ ions during repetitive charge-discharge process and track the transient electrochemical and chemical reactions occurring in the whole Li-S system. The in situ NMR provides real time, quantitative information related to the temporal concentration variations of the polysulfides with various chain lengths, providing important clues for the reaction pathways during both discharge and charge processes. The in-situ technique also reveals that redox reactions may involve transient species that are difficult to detect in ex-situ NMR study. Intermediate species such as charged free radicals may play an important role in the formation of the polysulfide products. Additionally, in situ NMR measurement simultaneously reveals vital information on the 7Li chemical environments in the electrochemical and parasitic reactions on the lithium anode that promotes the understanding of the failure mechanism in the Li-S system. These new insights could help design effective strategies to accelerate the development of Li-S battery technology.},
doi = {10.1021/acs.nanolett.5b00521},
journal = {Nano Letters, 15(5):3309-3316},
number = ,
volume = ,
place = {United States},
year = {2015},
month = {5}
}