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In Operando X-ray Diffraction and Transmission X-ray Microscopy of Lithium Sulfur Batteries
⊥ Author Contributions
These authors contributed equally to this work.
Abstract
Rechargeable lithium–sulfur (Li–S) batteries hold great potential for high-performance energy storage systems because they have a high theoretical specific energy, low cost, and are eco-friendly. However, the structural and morphological changes during electrochemical reactions are still not well understood. In this Article, these changes in Li–S batteries are studied in operando by X-ray diffraction and transmission X-ray microscopy. We show recrystallization of sulfur by the end of the charge cycle is dependent on the preparation technique of the sulfur cathode. On the other hand, it was found that crystalline Li2S does not form at the end of discharge for all sulfur cathodes studied. Furthermore, during cycling the bulk of soluble polysulfides remains trapped within the cathode matrix. Our results differ from previous ex situ results. This highlights the importance of in operando studies and suggests possible strategies to improve cycle life.
Discussion of in operando XRD at rate of C/20, description of micrometer-sized sulfur particle preparation, SEM with EDS detector experimental information, ex situ XRD experimental information, image of in operando XRD setup, in operando XRD of sulfur/Super P composite electrode cycled at C/20, SEM and EDS images of the three cathode preparation methods, XRD of the alternative cathode preparation methods, in operando TXM mosaics, plot of cycle life of Li–S cell with sulfur/Super P composite cathode, high magnification ex situ SEM micrographs, and two movies of in operando TXM. This material is available free of charge via the Internet at http://pubs.acs.org.
Citing Articles
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This article has been cited by 23 ACS Journal articles (5 most recent appear below).
Insight into Sulfur Reactions in Li–S Batteries
Rui Xu, Ilias Belharouak, Xiaofeng Zhang, Rita Chamoun, Cun Yu, Yang Ren, Anmin Nie, Reza Shahbazian-Yassar, Jun Lu, James C.M. Li, and Khalil AmineACS Applied Materials & Interfaces2014 6 (24), 21938-21945Insight into Sulfur Reactions in Li–S Batteries
Rui Xu, Ilias Belharouak, Xiaofeng Zhang, Rita Chamoun, Cun Yu, Yang Ren, Anmin Nie, Reza Shahbazian-Yassar, Jun Lu, James C.M. Li, and Khalil AmineACS Applied Materials & Interfaces2014 6 (24), 21938-21945Understanding and controlling the sulfur reduction species (Li2Sx, 1 ≤ x ≤ 8) under realistic battery conditions are essential for the development of advanced practical Li–S cells that can reach their full theoretical capacity. However, it has been a ...
Rechargeable Lithium–Sulfur Batteries
Arumugam Manthiram, Yongzhu Fu, Sheng-Heng Chung, Chenxi Zu, and Yu-Sheng SuChemical Reviews2014 114 (23), 11751-11787Rechargeable Lithium–Sulfur Batteries
Arumugam Manthiram, Yongzhu Fu, Sheng-Heng Chung, Chenxi Zu, and Yu-Sheng SuChemical Reviews2014 114 (23), 11751-11787
Ab Initio Structure Search and in Situ 7Li NMR Studies of Discharge Products in the Li–S Battery System
Kimberly A. See, Michal Leskes, John M. Griffin, Sylvia Britto, Peter D. Matthews, Alexandra Emly, Anton Van der Ven, Dominic S. Wright, Andrew J. Morris, Clare P. Grey, and Ram SeshadriJournal of the American Chemical Society2014 136 (46), 16368-16377Ab Initio Structure Search and in Situ 7Li NMR Studies of Discharge Products in the Li–S Battery System
Kimberly A. See, Michal Leskes, John M. Griffin, Sylvia Britto, Peter D. Matthews, Alexandra Emly, Anton Van der Ven, Dominic S. Wright, Andrew J. Morris, Clare P. Grey, and Ram SeshadriJournal of the American Chemical Society2014 136 (46), 16368-16377The high theoretical gravimetric capacity of the Li–S battery system makes it an attractive candidate for numerous energy storage applications. In practice, cell performance is plagued by low practical capacity and poor cycling. In an effort to explore ...
Nanoscale Morphological and Chemical Changes of High Voltage Lithium–Manganese Rich NMC Composite Cathodes with Cycling
Feifei Yang, Yijin Liu, Surendra K. Martha, Ziyu Wu, Joy C. Andrews, Gene E. Ice, Piero Pianetta, and Jagjit NandaNano Letters2014 14 (8), 4334-4341Nanoscale Morphological and Chemical Changes of High Voltage Lithium–Manganese Rich NMC Composite Cathodes with Cycling
Feifei Yang, Yijin Liu, Surendra K. Martha, Ziyu Wu, Joy C. Andrews, Gene E. Ice, Piero Pianetta, and Jagjit NandaNano Letters2014 14 (8), 4334-4341Understanding the evolution of chemical composition and morphology of battery materials during electrochemical cycling is fundamental to extending battery cycle life and ensuring safety. This is particularly true for the much debated high energy density (...
High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene
Yongcai Qiu, Wanfei Li, Wen Zhao, Guizhu Li, Yuan Hou, Meinan Liu, Lisha Zhou, Fangmin Ye, Hongfei Li, Zhanhua Wei, Shihe Yang, Wenhui Duan, Yifan Ye, Jinghua Guo, and Yuegang ZhangNano Letters2014 14 (8), 4821-4827High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene
Yongcai Qiu, Wanfei Li, Wen Zhao, Guizhu Li, Yuan Hou, Meinan Liu, Lisha Zhou, Fangmin Ye, Hongfei Li, Zhanhua Wei, Shihe Yang, Wenhui Duan, Yifan Ye, Jinghua Guo, and Yuegang ZhangNano Letters2014 14 (8), 4821-4827Nitrogen-doped graphene (NG) is a promising conductive matrix material for fabricating high-performance Li/S batteries. Here we report a simple, low-cost, and scalable method to prepare an additive-free nanocomposite cathode in which sulfur nanoparticles ...
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History
- Published In Issue April 11, 2012
- Article ASAPMarch 30, 2012
- Just Accepted ManuscriptMarch 20, 2012
- Received: January 09, 2012
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