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Title: Ultrathin dendrimer–graphene oxide composite film for stable cycling lithium–sulfur batteries

Abstract

Lithium–sulfur batteries (Li–S batteries) have attracted intense interest because of their high specific capacity and low cost, although they are still hindered by severe capacity loss upon cycling caused by the soluble lithium polysulfide intermediates. Although many structure innovations at the material and device levels have been explored for the ultimate goal of realizing long cycle life of Li–S batteries, it remains a major challenge to achieve stable cycling while avoiding energy and power density compromises caused by the introduction of significant dead weight/volume and increased electrochemical resistance. Here we introduce an ultrathin composite film consisting of naphthalimide-functionalized poly(amidoamine) dendrimers and graphene oxide nanosheets as a cycling stabilizer. Combining the dendrimer structure that can confine polysulfide intermediates chemically and physically together with the graphene oxide that renders the film robust and thin (<1% of the thickness of the active sulfur layer), the composite film is designed to enable stable cycling of sulfur cathodes without compromising the energy and power densities. As a result, our sulfur electrodes coated with the composite film exhibit very good cycling stability, together with high sulfur content, large areal capacity, and improved power rate.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [4];  [1];  [1];  [5];  [6];  [1];  [1];  [1]
  1. Yale Univ., West Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.
  2. Yale Univ., West Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.; Peking Univ., Beijing (China). College of Chemistry and Molecular Engineering
  3. Yale Univ., New Haven, CT (United States). Dept. of Mechanical Engineering and Materials Science
  4. Yale Univ., West Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.; Southeast Univ., Jiangsu (China). School of Chemistry and Chemical Engineering
  5. Yale Univ., New Haven, CT (United States). Dept. of Mechanical Engineering and Materials Science and Center for Research on Interface Structures and Phenomena
  6. Peking Univ., Beijing (China). College of Chemistry and Molecular Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1498104
Grant/Contract Number:  
FG02-07ER15909
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 14; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; lithium–sulfur battery; ultrathin composite film; dendrimer; graphene oxide; long cycle

Citation Formats

Liu, Wen, Jiang, Jianbing, Yang, Ke R., Mi, Yingying, Kumaravadivel, Piranavan, Zhong, Yiren, Fan, Qi, Weng, Zhe, Wu, Zishan, Cha, Judy J., Zhou, Henghui, Batista, Victor S., Brudvig, Gary W., and Wang, Hailiang. Ultrathin dendrimer–graphene oxide composite film for stable cycling lithium–sulfur batteries. United States: N. p., 2017. Web. doi:10.1073/pnas.1620809114.
Liu, Wen, Jiang, Jianbing, Yang, Ke R., Mi, Yingying, Kumaravadivel, Piranavan, Zhong, Yiren, Fan, Qi, Weng, Zhe, Wu, Zishan, Cha, Judy J., Zhou, Henghui, Batista, Victor S., Brudvig, Gary W., & Wang, Hailiang. Ultrathin dendrimer–graphene oxide composite film for stable cycling lithium–sulfur batteries. United States. doi:10.1073/pnas.1620809114.
Liu, Wen, Jiang, Jianbing, Yang, Ke R., Mi, Yingying, Kumaravadivel, Piranavan, Zhong, Yiren, Fan, Qi, Weng, Zhe, Wu, Zishan, Cha, Judy J., Zhou, Henghui, Batista, Victor S., Brudvig, Gary W., and Wang, Hailiang. Mon . "Ultrathin dendrimer–graphene oxide composite film for stable cycling lithium–sulfur batteries". United States. doi:10.1073/pnas.1620809114. https://www.osti.gov/servlets/purl/1498104.
@article{osti_1498104,
title = {Ultrathin dendrimer–graphene oxide composite film for stable cycling lithium–sulfur batteries},
author = {Liu, Wen and Jiang, Jianbing and Yang, Ke R. and Mi, Yingying and Kumaravadivel, Piranavan and Zhong, Yiren and Fan, Qi and Weng, Zhe and Wu, Zishan and Cha, Judy J. and Zhou, Henghui and Batista, Victor S. and Brudvig, Gary W. and Wang, Hailiang},
abstractNote = {Lithium–sulfur batteries (Li–S batteries) have attracted intense interest because of their high specific capacity and low cost, although they are still hindered by severe capacity loss upon cycling caused by the soluble lithium polysulfide intermediates. Although many structure innovations at the material and device levels have been explored for the ultimate goal of realizing long cycle life of Li–S batteries, it remains a major challenge to achieve stable cycling while avoiding energy and power density compromises caused by the introduction of significant dead weight/volume and increased electrochemical resistance. Here we introduce an ultrathin composite film consisting of naphthalimide-functionalized poly(amidoamine) dendrimers and graphene oxide nanosheets as a cycling stabilizer. Combining the dendrimer structure that can confine polysulfide intermediates chemically and physically together with the graphene oxide that renders the film robust and thin (<1% of the thickness of the active sulfur layer), the composite film is designed to enable stable cycling of sulfur cathodes without compromising the energy and power densities. As a result, our sulfur electrodes coated with the composite film exhibit very good cycling stability, together with high sulfur content, large areal capacity, and improved power rate.},
doi = {10.1073/pnas.1620809114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 14,
volume = 114,
place = {United States},
year = {2017},
month = {3}
}

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