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Title: An Ultrahigh Capacity Graphite/Li 2S Battery with Holey-Li 2S Nanoarchitectures

Abstract

The pairing of high-capacity Li 2S cathode (1166 mAh g -1) and lithium-free anode (LFA) provides an unparalleled potential in developing safe and energy-dense next-generation secondary batteries. However, the low utilization of the Li 2S cathode and the lack of electrolytes compatible to both electrodes are impeding the development. Here, a novel graphite/Li 2S battery system, which features a self-assembled, holey-Li 2S nanoarchitecture and a stable solid electrolyte interface (SEI) on the graphite electrode, is reported. The holey structure on Li 2S is beneficial in decomposing Li 2S at the first charging process due to the enhanced Li ion extraction and transfer from the Li 2S to the electrolyte. In addition, the concentrated dioxolane (DOL)-rich electrolyte designed lowers the irreversible capacity loss for SEI formation. By using the combined strategies, the graphite/holey-Li 2S battery delivers an ultrahigh discharge capacity of 810 mAh g -1 at 0.1 C (based on the mass of Li 2S) and of 714 mAh g -1 at 0.2 C. Moreover, it exhibits a reversible capacity of 300 mAh g -1 after a record lifecycle of 600 cycles at 1 C. These results suggest the great potential of the designed LFA/holey-Li 2S batteries for practical use.

Authors:
 [1];  [2];  [3]; ORCiD logo [1]
  1. Korea Advanced Inst. of Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemical and Biomolecular Engineering. KAIST Inst. for the NanoCentury. Advanced Battery Center
  2. Korea Advanced Inst. of Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemical and Biomolecular Engineering
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Electrochemical Materials & Systems Energy and Environment Directorate
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Korea Advanced Inst. of Science and Technology (KAIST), Daejeon (Korea, Republic of)
Sponsoring Org.:
USDOE; National Research Foundation of Korea (NRF)
OSTI Identifier:
1438222
Grant/Contract Number:  
AC05-76RL01830; NRF-2016M1B3A1A01937431
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; concentrated electrolytes; graphite/Li2S batteries; holey structures; Li2S cathodes; Li2S utilization

Citation Formats

Ye, Fangmin, Noh, Hyungjun, Lee, Hongkyung, and Kim, Hee-Tak. An Ultrahigh Capacity Graphite/Li2S Battery with Holey-Li2S Nanoarchitectures. United States: N. p., 2018. Web. doi:10.1002/advs.201800139.
Ye, Fangmin, Noh, Hyungjun, Lee, Hongkyung, & Kim, Hee-Tak. An Ultrahigh Capacity Graphite/Li2S Battery with Holey-Li2S Nanoarchitectures. United States. doi:10.1002/advs.201800139.
Ye, Fangmin, Noh, Hyungjun, Lee, Hongkyung, and Kim, Hee-Tak. Mon . "An Ultrahigh Capacity Graphite/Li2S Battery with Holey-Li2S Nanoarchitectures". United States. doi:10.1002/advs.201800139. https://www.osti.gov/servlets/purl/1438222.
@article{osti_1438222,
title = {An Ultrahigh Capacity Graphite/Li2S Battery with Holey-Li2S Nanoarchitectures},
author = {Ye, Fangmin and Noh, Hyungjun and Lee, Hongkyung and Kim, Hee-Tak},
abstractNote = {The pairing of high-capacity Li2S cathode (1166 mAh g-1) and lithium-free anode (LFA) provides an unparalleled potential in developing safe and energy-dense next-generation secondary batteries. However, the low utilization of the Li2S cathode and the lack of electrolytes compatible to both electrodes are impeding the development. Here, a novel graphite/Li2S battery system, which features a self-assembled, holey-Li2S nanoarchitecture and a stable solid electrolyte interface (SEI) on the graphite electrode, is reported. The holey structure on Li2S is beneficial in decomposing Li2S at the first charging process due to the enhanced Li ion extraction and transfer from the Li2S to the electrolyte. In addition, the concentrated dioxolane (DOL)-rich electrolyte designed lowers the irreversible capacity loss for SEI formation. By using the combined strategies, the graphite/holey-Li2S battery delivers an ultrahigh discharge capacity of 810 mAh g-1 at 0.1 C (based on the mass of Li2S) and of 714 mAh g-1 at 0.2 C. Moreover, it exhibits a reversible capacity of 300 mAh g-1 after a record lifecycle of 600 cycles at 1 C. These results suggest the great potential of the designed LFA/holey-Li2S batteries for practical use.},
doi = {10.1002/advs.201800139},
journal = {Advanced Science},
issn = {2198-3844},
number = 7,
volume = 5,
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
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Cited by: 1 work
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Figures / Tables:

Figure 1 Figure 1: Schematic illustration of the structural changes upon carbothermal conversion from Li2SO4 to Li2S and upon the initial charge process from Li2S to sulfur.

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Works referenced in this record:

Burning lithium in CS2 for high-performing compact Li2S–graphene nanocapsules for Li–S batteries
journal, June 2017


Li 2 S encapsulated by nitrogen-doped carbon for lithium sulfur batteries
journal, January 2014

  • Chen, Lin; Liu, Yuzi; Ashuri, Maziar
  • J. Mater. Chem. A, Vol. 2, Issue 42
  • DOI: 10.1039/C4TA04103H

A Conductive Molecular Framework Derived Li 2 S/N,P-Codoped Carbon Cathode for Advanced Lithium-Sulfur Batteries
journal, April 2017


Magnetic Field-Controlled Lithium Polysulfide Semiliquid Battery with Ferrofluidic Properties
journal, October 2015


A High-Performance Polymer Tin Sulfur Lithium Ion Battery
journal, February 2010

  • Hassoun, Jusef; Scrosati, Bruno
  • Angewandte Chemie International Edition, Vol. 49, Issue 13, p. 2371-2374
  • DOI: 10.1002/anie.200907324

High performance Li-ion sulfur batteries enabled by intercalation chemistry
journal, January 2015

  • Lv, Dongping; Yan, Pengfei; Shao, Yuyan
  • Chemical Communications, Vol. 51, Issue 70
  • DOI: 10.1039/C5CC05171A

Sulfur/polyacrylonitrile/carbon multi-composites as cathode materials for lithium/sulfur battery in the concentrated electrolyte
journal, January 2014

  • Zhang, Y. Z.; Liu, S.; Li, G. C.
  • J. Mater. Chem. A, Vol. 2, Issue 13
  • DOI: 10.1039/C3TA14914E

Inhibiting Polysulfide Shuttle in Lithium-Sulfur Batteries through Low-Ion-Pairing Salts and a Triflamide Solvent
journal, May 2017

  • Shyamsunder, Abhinandan; Beichel, Witali; Klose, Petra
  • Angewandte Chemie International Edition, Vol. 56, Issue 22
  • DOI: 10.1002/anie.201701026

A pre-lithiation method for sulfur cathode used for future lithium metal free full battery
journal, February 2017


Limited Stability of Ether-Based Solvents in Lithium–Oxygen Batteries
journal, September 2012

  • Ryan, Kate R.; Trahey, Lynn; Ingram, Brian J.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 37
  • DOI: 10.1021/jp306797s

An efficient Li2S-based lithium-ion sulfur battery realized by a bifunctional electrolyte additive
journal, October 2017


Exceptional Electrochemical Performance of Si-Nanowires in 1,3-Dioxolane Solutions: A Surface Chemical Investigation
journal, March 2012

  • Etacheri, Vinodkumar; Geiger, Uzi; Gofer, Yossi
  • Langmuir, Vol. 28, Issue 14
  • DOI: 10.1021/la300306v

Conversion from Li2SO4 to Li2S@C on carbon paper matrix: A novel integrated cathode for lithium-sulfur batteries
journal, November 2016


Nanoporous Li2S and MWCNT-linked Li2S powder cathodes for lithium-sulfur and lithium-ion battery chemistries
journal, January 2014

  • Wu, Feixiang; Magasinski, Alexandre; Yushin, Gleb
  • Journal of Materials Chemistry A, Vol. 2, Issue 17, p. 6064-6070
  • DOI: 10.1039/C3TA14161F

Li 2 S/carbon nanocomposite strips from a low-temperature conversion of Li 2 SO 4 as high-performance lithium–sulfur cathodes
journal, January 2018

  • Ye, Fangmin; Noh, Hyungjun; Lee, Jinhong
  • Journal of Materials Chemistry A, Vol. 6, Issue 15
  • DOI: 10.1039/C8TA00515J

In situ synthesized Li 2 S@porous carbon cathode for graphite/Li 2 S full cells using ether-based electrolyte
journal, December 2017


A Facile Layer-by-Layer Approach for High-Areal-Capacity Sulfur Cathodes
journal, January 2015


High-Performance Li/Dissolved Polysulfide Batteries with an Advanced Cathode Structure and High Sulfur Content
journal, August 2014


Rechargeable Lithium Sulfur Battery
journal, January 2003

  • Cheon, Sang-Eun; Ko, Ki-Seok; Cho, Ji-Hoon
  • Journal of The Electrochemical Society, Vol. 150, Issue 6
  • DOI: 10.1149/1.1571532

Smaller Sulfur Molecules Promise Better Lithium–Sulfur Batteries
journal, October 2012

  • Xin, Sen; Gu, Lin; Zhao, Na-Hong
  • Journal of the American Chemical Society, Vol. 134, Issue 45
  • DOI: 10.1021/ja308170k

Rechargeable Lithium Sulfur Battery
journal, May 2003

  • Cheon, Sang-Eun; Ko, Ki-Seok; Cho, Ji-Hoon
  • Journal of The Electrochemical Society, Vol. 150, Issue 6, p. A800-A805
  • DOI: 10.1149/1.1571533

In situ synthesis of lithium sulfide–carbon composites as cathode materials for rechargeable lithium batteries
journal, January 2013

  • Yang, Zichao; Guo, Juchen; Das, Shyamal K.
  • Journal of Materials Chemistry A, Vol. 1, Issue 4, p. 1433-1440
  • DOI: 10.1039/C2TA00779G

Promising Cell Configuration for Next-Generation Energy Storage: Li 2 S/Graphite Battery Enabled by a Solvate Ionic Liquid Electrolyte
journal, June 2016

  • Li, Zhe; Zhang, Shiguo; Terada, Shoshi
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 25
  • DOI: 10.1021/acsami.6b03736

High-Performance Lithium-Sulfur Batteries with a Self-Supported, 3D Li 2 S-Doped Graphene Aerogel Cathodes
journal, November 2015

  • Zhou, Guangmin; Paek, Eunsu; Hwang, Gyeong S.
  • Advanced Energy Materials, Vol. 6, Issue 2
  • DOI: 10.1002/aenm.201501355

Design of Battery Electrodes with Dual-Scale Porosity to Minimize Tortuosity and Maximize Performance
journal, December 2012

  • Bae, Chang-Jun; Erdonmez, Can K.; Halloran, John W.
  • Advanced Materials, Vol. 25, Issue 9
  • DOI: 10.1002/adma.201204055

Freestanding Flexible Li 2 S Paper Electrode with High Mass and Capacity Loading for High-Energy Li-S Batteries
journal, May 2017

  • Yu, Mingliang; Wang, Zhiyu; Wang, Yuwei
  • Advanced Energy Materials, Vol. 7, Issue 17
  • DOI: 10.1002/aenm.201700018

Formation of Reversible Solid Electrolyte Interface on Graphite Surface from Concentrated Electrolytes
journal, February 2017


In Situ Formed Lithium Sulfide/Microporous Carbon Cathodes for Lithium-Ion Batteries
journal, November 2013

  • Zheng, Shiyou; Chen, Yvonne; Xu, Yunhua
  • ACS Nano, Vol. 7, Issue 12
  • DOI: 10.1021/nn404601h

Vapor-Phase Atomic-Controllable Growth of Amorphous Li 2 S for High-Performance Lithium–Sulfur Batteries
journal, October 2014

  • Meng, Xiangbo; Comstock, David J.; Fister, Timothy T.
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn505480w

Li-S Batteries with Li 2 S Cathodes and Si/C Anodes
journal, January 2015

  • Jha, Himendra; Buchberger, Irmgard; Cui, Xueyin
  • Journal of The Electrochemical Society, Vol. 162, Issue 9
  • DOI: 10.1149/2.0681509jes

Two-dimensional layered transition metal disulphides for effective encapsulation of high-capacity lithium sulphide cathodes
journal, September 2014

  • Seh, Zhi Wei; Yu, Jung Ho; Li, Weiyang
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6017

A superconcentrated ether electrolyte for fast-charging Li-ion batteries
journal, January 2013

  • Yamada, Yuki; Yaegashi, Makoto; Abe, Takeshi
  • Chemical Communications, Vol. 49, Issue 95, p. 11194-11196
  • DOI: 10.1039/c3cc46665e

Si/Li<sub>2</sub>S Battery with Solvate Ionic Liquid Electrolyte
journal, January 2016


Polysulfide dissolution control: the common ion effect
journal, January 2013

  • Shin, Eon Sung; Kim, Keon; Oh, Si Hyoung
  • Chem. Commun., Vol. 49, Issue 20
  • DOI: 10.1039/C2CC36986A

Nanostructured Li 2 S–C Composites as Cathode Material for High-Energy Lithium/Sulfur Batteries
journal, February 2012

  • Cai, Kunpeng; Song, Min-Kyu; Cairns, Elton J.
  • Nano Letters, Vol. 12, Issue 12
  • DOI: 10.1021/nl303965a

A high energy density Li 2 S@C nanocomposite cathode with a nitrogen-doped carbon nanotube top current collector
journal, January 2015

  • Zhang, Su; Liu, Meinan; Ma, Fei
  • Journal of Materials Chemistry A, Vol. 3, Issue 37
  • DOI: 10.1039/C5TA05819H

Novel dual-salts electrolyte solution for dendrite-free lithium-metal based rechargeable batteries with high cycle reversibility
journal, December 2014


Preparation of electrochemically active lithium sulfide–carbon composites using spark-plasma-sintering process
journal, May 2010

  • Takeuchi, Tomonari; Sakaebe, Hikari; Kageyama, Hiroyuki
  • Journal of Power Sources, Vol. 195, Issue 9, p. 2928-2934
  • DOI: 10.1016/j.jpowsour.2009.11.011

Fabrication of mesoporous Li 2 S–C nanofibers for high performance Li/Li 2 S cell cathodes
journal, January 2015


A Graphite-Polysulfide Full Cell with DME-Based Electrolyte
journal, January 2016

  • Bhargav, Amruth; Wu, Min; Fu, Yongzhu
  • Journal of The Electrochemical Society, Vol. 163, Issue 8
  • DOI: 10.1149/2.0151608jes

Synthesis of highly electrochemically active Li 2 S nanoparticles for lithium–sulfur-batteries
journal, January 2015

  • Kohl, M.; Brückner, J.; Bauer, I.
  • Journal of Materials Chemistry A, Vol. 3, Issue 31
  • DOI: 10.1039/C5TA04504E

Ultrasmall Li2S Nanoparticles Anchored in Graphene Nanosheets for High-Energy Lithium-Ion Batteries
journal, September 2014

  • Zhang, Kai; Wang, Lijiang; Hu, Zhe
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06467

Prelithiation of Nanostructured Sulfur Cathode by an “On-Sheet” Solid-State Reaction
journal, April 2016


Recent Advances in Electrolytes for Lithium-Sulfur Batteries
journal, April 2015

  • Zhang, Shiguo; Ueno, Kazuhide; Dokko, Kaoru
  • Advanced Energy Materials, Vol. 5, Issue 16
  • DOI: 10.1002/aenm.201500117

PVP-Assisted Synthesis of Uniform Carbon Coated Li 2 S/CB for High-Performance Lithium–Sulfur Batteries
journal, November 2015

  • Chen, Lin; Liu, Yuzi; Zhang, Fan
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 46
  • DOI: 10.1021/acsami.5b07331

Synergistically Assembled Li 2 S/FWNTs@Reduced Graphene Oxide Nanobundle Forest for Free-Standing High-Performance Li 2 S Cathodes
journal, May 2017

  • Chen, Yan; Lu, Songtao; Zhou, Jia
  • Advanced Functional Materials, Vol. 27, Issue 25
  • DOI: 10.1002/adfm.201700987

Model Membrane-Free Li-S Batteries for Enhanced Performance and Cycle Life
journal, April 2015


New Nanostructured Li2S/Silicon Rechargeable Battery with High Specific Energy
journal, April 2010

  • Yang, Yuan; McDowell, Matthew T.; Jackson, Ariel
  • Nano Letters, Vol. 10, Issue 4, p. 1486-1491
  • DOI: 10.1021/nl100504q

Facile synthesis of Li2S–polypyrrole composite structures for high-performance Li2S cathodes
journal, January 2014

  • Seh, Zhi Wei; Wang, Haotian; Hsu, Po-Chun
  • Energy & Environmental Science, Vol. 7, Issue 2
  • DOI: 10.1039/c3ee43395a

Micro-scale Li2S–C composite preparation from Li2SO4 for cathode of lithium ion battery
journal, November 2015


High-Capacity Micrometer-Sized Li2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries
journal, September 2012

  • Yang, Yuan; Zheng, Guangyuan; Misra, Sumohan
  • Journal of the American Chemical Society, Vol. 134, Issue 37, p. 15387-15394
  • DOI: 10.1021/ja3052206

Chemical routes toward long-lasting lithium/sulfur cells
journal, January 2016


A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries
journal, February 2013

  • Suo, Liumin; Hu, Yong-Sheng; Li, Hong
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2513

Capacity Fade Analysis of Sulfur Cathodes in Lithium-Sulfur Batteries
journal, July 2016


Slurryless Li 2 S/Reduced Graphene Oxide Cathode Paper for High-Performance Lithium Sulfur Battery
journal, February 2015


Durable Carbon-Coated Li 2 S Core–Shell Spheres for High Performance Lithium/Sulfur Cells
journal, March 2014

  • Nan, Caiyun; Lin, Zhan; Liao, Honggang
  • Journal of the American Chemical Society, Vol. 136, Issue 12
  • DOI: 10.1021/ja412943h

Correlation Between Cointercalation of Solvents and Electrochemical Intercalation of Lithium into Graphite in Propylene Carbonate Solution
journal, January 2003

  • Abe, Takeshi; Kawabata, Naoki; Mizutani, Yasuo
  • Journal of The Electrochemical Society, Vol. 150, Issue 3
  • DOI: 10.1149/1.1541004

Sulfur-Infiltrated Micro- and Mesoporous Silicon Carbide-Derived Carbon Cathode for High-Performance Lithium Sulfur Batteries
journal, June 2013

  • Lee, Jung Tae; Zhao, Youyang; Thieme, Sören
  • Advanced Materials, Vol. 25, Issue 33
  • DOI: 10.1002/adma.201301579

Improving lithium–sulphur batteries through spatial control of sulphur species deposition on a hybrid electrode surface
journal, May 2014

  • Yao, Hongbin; Zheng, Guangyuan; Hsu, Po-Chun
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4943

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.