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Title: Large-diameter and heteroatom-doped graphene nanotubes decorated with transition metals as carbon hosts for lithium–sulfur batteries

Abstract

This work addresses here performance issues of lithium–sulfur (Li–S) batteries via retaining the polysulfide intermediates within a novel cathode nanocarbon host. Herein, we report a series of nitrogen and oxygen co-doped and transition metal-decorated large size (200–500 nm in diameter) graphene nanotubes (M-GNTs) (M = Co, Ni, and/or Fe) as effective carbon hosts for sulfur cathodes (S@M-GNTs) in Li–S batteries. The exceptionally large diameters of the graphene tubes allow facile diffusion of sulfur inside the tubes with sufficient loadings, yet leaving room for volume expansion during the lithiation process. The GNTs with the largest diameter and abundant N and O doping along with FeCoNi alloy decoration (FeCoNi-GNTs) exhibit the best sulfur cathode performance. In addition to the unique nanocarbon structures, the heteroatom dopants and transition metal nanoparticles likely also play promotional roles in retaining long-chain polysulfide discharge intermediates within the carbon host, therefore improving rate capability and cycle stability. In particular, a S@FeCoNi-GNT cathode with a high sulfur loading (~4.5 mgS cm-2) exhibits discharge capacities up to 1234.7 mA h g-1 at C/20 and 909.0 mA h g-1 at C/5. A discharge capacity of 554.4 mA h g-1 at 1C after 500 cycles was retained, further demonstrating its encouraging potentialmore » in Li–S batteries.« less

Authors:
 [1];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  3. Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1515154
Alternate Identifier(s):
OSTI ID: 1514729
Report Number(s):
BNL-211690-2019-JAAM
Journal ID: ISSN 2050-7488
Grant/Contract Number:  
SC0012704; CBET-1604392
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Carbon hosts; large size graphene tube; ultra-high sulfur loading; sulfur cathodes; Li-S batteries

Citation Formats

Ogoke, Ogechi, Hwang, Sooyeon, Hultman, Benjamin, Chen, Mengjie, Karakalos, Stavros, He, Yanghua, Ramsey, Adam, Su, Dong, Alexandridis, Paschalis, and Wu, Gang. Large-diameter and heteroatom-doped graphene nanotubes decorated with transition metals as carbon hosts for lithium–sulfur batteries. United States: N. p., 2019. Web. doi:10.1039/C9TA02889G.
Ogoke, Ogechi, Hwang, Sooyeon, Hultman, Benjamin, Chen, Mengjie, Karakalos, Stavros, He, Yanghua, Ramsey, Adam, Su, Dong, Alexandridis, Paschalis, & Wu, Gang. Large-diameter and heteroatom-doped graphene nanotubes decorated with transition metals as carbon hosts for lithium–sulfur batteries. United States. doi:10.1039/C9TA02889G.
Ogoke, Ogechi, Hwang, Sooyeon, Hultman, Benjamin, Chen, Mengjie, Karakalos, Stavros, He, Yanghua, Ramsey, Adam, Su, Dong, Alexandridis, Paschalis, and Wu, Gang. Mon . "Large-diameter and heteroatom-doped graphene nanotubes decorated with transition metals as carbon hosts for lithium–sulfur batteries". United States. doi:10.1039/C9TA02889G. https://www.osti.gov/servlets/purl/1515154.
@article{osti_1515154,
title = {Large-diameter and heteroatom-doped graphene nanotubes decorated with transition metals as carbon hosts for lithium–sulfur batteries},
author = {Ogoke, Ogechi and Hwang, Sooyeon and Hultman, Benjamin and Chen, Mengjie and Karakalos, Stavros and He, Yanghua and Ramsey, Adam and Su, Dong and Alexandridis, Paschalis and Wu, Gang},
abstractNote = {This work addresses here performance issues of lithium–sulfur (Li–S) batteries via retaining the polysulfide intermediates within a novel cathode nanocarbon host. Herein, we report a series of nitrogen and oxygen co-doped and transition metal-decorated large size (200–500 nm in diameter) graphene nanotubes (M-GNTs) (M = Co, Ni, and/or Fe) as effective carbon hosts for sulfur cathodes (S@M-GNTs) in Li–S batteries. The exceptionally large diameters of the graphene tubes allow facile diffusion of sulfur inside the tubes with sufficient loadings, yet leaving room for volume expansion during the lithiation process. The GNTs with the largest diameter and abundant N and O doping along with FeCoNi alloy decoration (FeCoNi-GNTs) exhibit the best sulfur cathode performance. In addition to the unique nanocarbon structures, the heteroatom dopants and transition metal nanoparticles likely also play promotional roles in retaining long-chain polysulfide discharge intermediates within the carbon host, therefore improving rate capability and cycle stability. In particular, a S@FeCoNi-GNT cathode with a high sulfur loading (~4.5 mgS cm-2) exhibits discharge capacities up to 1234.7 mA h g-1 at C/20 and 909.0 mA h g-1 at C/5. A discharge capacity of 554.4 mA h g-1 at 1C after 500 cycles was retained, further demonstrating its encouraging potential in Li–S batteries.},
doi = {10.1039/C9TA02889G},
journal = {Journal of Materials Chemistry. A},
number = ,
volume = 7,
place = {United States},
year = {2019},
month = {5}
}

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