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Title: Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries

Abstract

We report that despite their high energy density and affordable cost compared to lithium-ion (Li-ion) batteries, lithium-sulfur (Li-S) batteries still endure from slow reaction kinetics and capacity loss induced by the insulating sulfur and severe polysulfide diffusion. To address these issues, we report here nickel nanoparticles filled in vertically grown carbon nanotubes on graphene sheets (graphene-carbon nanotube-nickel composite (Gr-CNT-Ni)) that are coated onto a polypropylene separator as a polysulfide trap for the construction of high-loading sulfur cathodes. The hierarchical porous framework of Gr-CNT physically entraps and immobilizes the active material sulfur, while the strong chemical interaction with Ni nanoparticles in Gr-CNT-Ni inhibits polysulfide diffusion. The covalently interconnected electron conduction channels and carbon shell-confined metal active sites provide feasible paths for the continual regeneration of active material during the charge/discharge process. Benefitting from these novel morphological and structural features, the Li-S cell with the Gr-CNT-Ni as a polysulfide trap demonstrates high specific capacity and good cycle life. Lastly, this work provides new avenues for synergistically combining the advantages of hierarchical porous carbon architectures and metal active sites for the development of high-performance cathodes for Li-S batteries.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [2]
  1. Madurai Kamaraj Univ., Tamil Nadu (India); Univ. of Texas, Austin, TX (United States). Texas Materials Inst.
  2. Univ. of Texas, Austin, TX (United States). Texas Materials Inst.
  3. Madurai Kamaraj Univ., Tamil Nadu (India)
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Science and Engineering Research Board
OSTI Identifier:
1598177
Grant/Contract Number:  
[SC0005397; EMR/2015/000912]
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 24]; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 3D hierarchical architecture; charge transfer; confined metal nanoparticles; lithium−sulfur batteries; tip growth

Citation Formats

Gnana kumar, G., Chung, Sheng-Heng, Raj kumar, T., and Manthiram, Arumugam. Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries. United States: N. p., 2018. Web. doi:10.1021/acsami.8b06054.
Gnana kumar, G., Chung, Sheng-Heng, Raj kumar, T., & Manthiram, Arumugam. Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries. United States. doi:10.1021/acsami.8b06054.
Gnana kumar, G., Chung, Sheng-Heng, Raj kumar, T., and Manthiram, Arumugam. Fri . "Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries". United States. doi:10.1021/acsami.8b06054. https://www.osti.gov/servlets/purl/1598177.
@article{osti_1598177,
title = {Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries},
author = {Gnana kumar, G. and Chung, Sheng-Heng and Raj kumar, T. and Manthiram, Arumugam},
abstractNote = {We report that despite their high energy density and affordable cost compared to lithium-ion (Li-ion) batteries, lithium-sulfur (Li-S) batteries still endure from slow reaction kinetics and capacity loss induced by the insulating sulfur and severe polysulfide diffusion. To address these issues, we report here nickel nanoparticles filled in vertically grown carbon nanotubes on graphene sheets (graphene-carbon nanotube-nickel composite (Gr-CNT-Ni)) that are coated onto a polypropylene separator as a polysulfide trap for the construction of high-loading sulfur cathodes. The hierarchical porous framework of Gr-CNT physically entraps and immobilizes the active material sulfur, while the strong chemical interaction with Ni nanoparticles in Gr-CNT-Ni inhibits polysulfide diffusion. The covalently interconnected electron conduction channels and carbon shell-confined metal active sites provide feasible paths for the continual regeneration of active material during the charge/discharge process. Benefitting from these novel morphological and structural features, the Li-S cell with the Gr-CNT-Ni as a polysulfide trap demonstrates high specific capacity and good cycle life. Lastly, this work provides new avenues for synergistically combining the advantages of hierarchical porous carbon architectures and metal active sites for the development of high-performance cathodes for Li-S batteries.},
doi = {10.1021/acsami.8b06054},
journal = {ACS Applied Materials and Interfaces},
number = [24],
volume = [10],
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 11 works
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