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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]
+ Show Author Affiliations
  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 Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
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.
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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. https://doi.org/10.1073/pnas.1620809114
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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. https://doi.org/10.1073/pnas.1620809114. https://www.osti.gov/servlets/purl/1498104.
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@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 = {Mon Mar 20 00:00:00 EDT 2017},
month = {Mon Mar 20 00:00:00 EDT 2017}
}
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https://doi.org/10.1073/pnas.1620809114
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Cited by: 82 works
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Figures / Tables:

Figure 1 Figure 1: Illustration of Naph-Den synthesis and sulfur cathode fabrication. (A) Molecular structure illustration of Naph-Den. (B) Digital photos of Naph-Den DMF solution, mGO DMF suspension, and NaphDen–mGO slurry. (C) A thin Naph-Den–mGO film on a glass slide, prepared by casting the slurry on copper foil and then transferring themore » film. (D) AFM image and height profile for the Naph-Den–mGO film, showing an average thickness of 97 nm with thicker folded edges. (E) Digital photo of a GO–S electrode coated with the Naph-Den–mGO layer. (F) SEM image of the surface of the Naph-Den–mGO/GO–S electrode. (G) SEM side views of the Naph-Den– mGO/GO–S electrode, with the enlarged image showing the thickness of the Naph-Den–mGO film.« less
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    Works referencing / citing this record:

    Graphene in Lithium-Ion/Lithium-Sulfur Batteries
    book, January 2019

    Sulfur Immobilization by “Chemical Anchor” to Suppress the Diffusion of Polysulfides in Lithium-Sulfur Batteries
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