Freeze-Dried Sulfur-Graphene Oxide-Carbon Nanotube Nanocomposite for High Sulfur-Loading Lithium/Sulfur Cells

Yoon Hwa; Hyeon Kook Seo; Jong Min Yuk; Elton J. Cairns

doi:10.1021/acs.nanolett.7b03831

Freeze-Dried Sulfur-Graphene Oxide-Carbon Nanotube Nanocomposite for High Sulfur-Loading Lithium/Sulfur Cells

Yoon Hwa, Hyeon Kook Seo, Jong Min Yuk, Elton J. Cairns

Research output: Contribution to journal › Article › peer-review

95 Scopus citations

Abstract

The ambient-temperature rechargeable lithium/sulfur (Li/S) cell is a strong candidate for the beyond lithium ion cell since significant progress on developing advanced sulfur electrodes with high sulfur loading has been made. Here we report on a new sulfur electrode active material consisting of a cetyltrimethylammonium bromide-modified sulfur-graphene oxide-carbon nanotube (S-GO-CTA-CNT) nanocomposite prepared by freeze-drying. We show the real-time formation of nanocrystalline lithium sulfide (Li₂S) at the interface between the S-GO-CTA-CNT nanocomposite and the liquid electrolyte by in situ TEM observation of the reaction. The combination of GO and CNT helps to maintain the structural integrity of the S-GO-CTA-CNT nanocomposite during lithiation/delithiation. A high S loading (11.1 mgS/cm², 75% S) S-GO-CTA-CNT electrode was successfully prepared using a three-dimensional structured Al foam as a substrate and showed good S utilization (1128 mAh/g S corresponding to 12.5 mAh/cm²), even with a very low electrolyte to sulfur weight ratio of 4. Moreover, it was demonstrated that the ionic liquid in the electrolyte improves the Coulombic efficiency and stabilizes the morphology of the Li metal anode.

Original language	English (US)
Pages (from-to)	7086-7094
Number of pages	9
Journal	Nano Letters
Volume	17
Issue number	11
DOIs	https://doi.org/10.1021/acs.nanolett.7b03831
State	Published - Nov 8 2017
Externally published	Yes

Keywords

Lithium/sulfur cell
aluminum foam
energy storage
high sulfur loading
in situ TEM
ionic liquid

ASJC Scopus subject areas

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.7b03831

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title = "Freeze-Dried Sulfur-Graphene Oxide-Carbon Nanotube Nanocomposite for High Sulfur-Loading Lithium/Sulfur Cells",

abstract = "The ambient-temperature rechargeable lithium/sulfur (Li/S) cell is a strong candidate for the beyond lithium ion cell since significant progress on developing advanced sulfur electrodes with high sulfur loading has been made. Here we report on a new sulfur electrode active material consisting of a cetyltrimethylammonium bromide-modified sulfur-graphene oxide-carbon nanotube (S-GO-CTA-CNT) nanocomposite prepared by freeze-drying. We show the real-time formation of nanocrystalline lithium sulfide (Li2S) at the interface between the S-GO-CTA-CNT nanocomposite and the liquid electrolyte by in situ TEM observation of the reaction. The combination of GO and CNT helps to maintain the structural integrity of the S-GO-CTA-CNT nanocomposite during lithiation/delithiation. A high S loading (11.1 mgS/cm2, 75% S) S-GO-CTA-CNT electrode was successfully prepared using a three-dimensional structured Al foam as a substrate and showed good S utilization (1128 mAh/g S corresponding to 12.5 mAh/cm2), even with a very low electrolyte to sulfur weight ratio of 4. Moreover, it was demonstrated that the ionic liquid in the electrolyte improves the Coulombic efficiency and stabilizes the morphology of the Li metal anode.",

keywords = "Lithium/sulfur cell, aluminum foam, energy storage, high sulfur loading, in situ TEM, ionic liquid",

author = "Yoon Hwa and Seo, {Hyeon Kook} and Yuk, {Jong Min} and Cairns, {Elton J.}",

note = "Funding Information: The work at LBNL was sponsored by ZAF Energy Systems. We thank Tevye Kuykendall and the Molecular Foundry at the Lawrence Berkeley National Laboratory for supporting the X-ray diffractometer, X-ray photoelectron spectroscopy and scanning electron microscope. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The TEM research was supported by Nano·Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT, and Future Planning (2009-0082580). Dr. Hyo Won Kim and Hilda Buss are thanked for assistance with XPS analysis and freeze-drying, respectively. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

month = nov,

day = "8",

doi = "10.1021/acs.nanolett.7b03831",

language = "English (US)",

volume = "17",

pages = "7086--7094",

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T1 - Freeze-Dried Sulfur-Graphene Oxide-Carbon Nanotube Nanocomposite for High Sulfur-Loading Lithium/Sulfur Cells

AU - Hwa, Yoon

AU - Seo, Hyeon Kook

AU - Yuk, Jong Min

AU - Cairns, Elton J.

N1 - Funding Information: The work at LBNL was sponsored by ZAF Energy Systems. We thank Tevye Kuykendall and the Molecular Foundry at the Lawrence Berkeley National Laboratory for supporting the X-ray diffractometer, X-ray photoelectron spectroscopy and scanning electron microscope. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The TEM research was supported by Nano·Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT, and Future Planning (2009-0082580). Dr. Hyo Won Kim and Hilda Buss are thanked for assistance with XPS analysis and freeze-drying, respectively. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/11/8

Y1 - 2017/11/8

N2 - The ambient-temperature rechargeable lithium/sulfur (Li/S) cell is a strong candidate for the beyond lithium ion cell since significant progress on developing advanced sulfur electrodes with high sulfur loading has been made. Here we report on a new sulfur electrode active material consisting of a cetyltrimethylammonium bromide-modified sulfur-graphene oxide-carbon nanotube (S-GO-CTA-CNT) nanocomposite prepared by freeze-drying. We show the real-time formation of nanocrystalline lithium sulfide (Li2S) at the interface between the S-GO-CTA-CNT nanocomposite and the liquid electrolyte by in situ TEM observation of the reaction. The combination of GO and CNT helps to maintain the structural integrity of the S-GO-CTA-CNT nanocomposite during lithiation/delithiation. A high S loading (11.1 mgS/cm2, 75% S) S-GO-CTA-CNT electrode was successfully prepared using a three-dimensional structured Al foam as a substrate and showed good S utilization (1128 mAh/g S corresponding to 12.5 mAh/cm2), even with a very low electrolyte to sulfur weight ratio of 4. Moreover, it was demonstrated that the ionic liquid in the electrolyte improves the Coulombic efficiency and stabilizes the morphology of the Li metal anode.

AB - The ambient-temperature rechargeable lithium/sulfur (Li/S) cell is a strong candidate for the beyond lithium ion cell since significant progress on developing advanced sulfur electrodes with high sulfur loading has been made. Here we report on a new sulfur electrode active material consisting of a cetyltrimethylammonium bromide-modified sulfur-graphene oxide-carbon nanotube (S-GO-CTA-CNT) nanocomposite prepared by freeze-drying. We show the real-time formation of nanocrystalline lithium sulfide (Li2S) at the interface between the S-GO-CTA-CNT nanocomposite and the liquid electrolyte by in situ TEM observation of the reaction. The combination of GO and CNT helps to maintain the structural integrity of the S-GO-CTA-CNT nanocomposite during lithiation/delithiation. A high S loading (11.1 mgS/cm2, 75% S) S-GO-CTA-CNT electrode was successfully prepared using a three-dimensional structured Al foam as a substrate and showed good S utilization (1128 mAh/g S corresponding to 12.5 mAh/cm2), even with a very low electrolyte to sulfur weight ratio of 4. Moreover, it was demonstrated that the ionic liquid in the electrolyte improves the Coulombic efficiency and stabilizes the morphology of the Li metal anode.

KW - Lithium/sulfur cell

KW - aluminum foam

KW - energy storage

KW - high sulfur loading

KW - in situ TEM

KW - ionic liquid

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DO - 10.1021/acs.nanolett.7b03831

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SN - 1530-6984

VL - 17

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EP - 7094

JO - Nano Letters

JF - Nano Letters

IS - 11

ER -

Freeze-Dried Sulfur-Graphene Oxide-Carbon Nanotube Nanocomposite for High Sulfur-Loading Lithium/Sulfur Cells

Abstract

Keywords

ASJC Scopus subject areas

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