Covalently Grafted Polysulfur–Graphene Nanocomposites for Ultrahigh Sulfur-Loading Lithium–Polysulfur Batteries
Abstract
Although lithium–polysulfur (Li–polyS) batteries employing organic polymeric sulfur as a cathode material outperform the lithium–sulfur (Li–S) battery system, the relatively low sulfur loading (<2 mg cm–2) in the current Li–polyS batteries compromises the areal capacity, constraining their practicality. We present here a new cathode active material (a covalently grafted polysulfur–graphene nanocomposite (polySGN)) for ultrahigh-loading Li–polyS batteries. The new cathode active material polySGN offers several advantages: (i) the well-dispersed graphene sheets offer highly electrically conductive pathways for electrons to travel within the polySGN matrix; (ii) the intermediate organosulfide moieties alleviate irreversible sulfide deposition on electrodes; and (iii) the in situ formed coating layer on the cathode-side surface of the polymeric separator further reduces polysulfide migration. In conclusion, the Li–polyS batteries employing polySGN as the cathode active material accomplish the highest sulfur loading (up to 10.5 mg cm–2) and the highest areal capacity (~12 mA h cm–2) reported thus far in the literature.
- Authors:
-
- The Univ. of Texas at Austin, Austin, TX (United States)
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1487468
- Grant/Contract Number:
- EE0007218
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE
Citation Formats
Chang, Chi -Hao, and Manthiram, Arumugam. Covalently Grafted Polysulfur–Graphene Nanocomposites for Ultrahigh Sulfur-Loading Lithium–Polysulfur Batteries. United States: N. p., 2017.
Web. doi:10.1021/acsenergylett.7b01031.
Chang, Chi -Hao, & Manthiram, Arumugam. Covalently Grafted Polysulfur–Graphene Nanocomposites for Ultrahigh Sulfur-Loading Lithium–Polysulfur Batteries. United States. https://doi.org/10.1021/acsenergylett.7b01031
Chang, Chi -Hao, and Manthiram, Arumugam. Wed .
"Covalently Grafted Polysulfur–Graphene Nanocomposites for Ultrahigh Sulfur-Loading Lithium–Polysulfur Batteries". United States. https://doi.org/10.1021/acsenergylett.7b01031. https://www.osti.gov/servlets/purl/1487468.
@article{osti_1487468,
title = {Covalently Grafted Polysulfur–Graphene Nanocomposites for Ultrahigh Sulfur-Loading Lithium–Polysulfur Batteries},
author = {Chang, Chi -Hao and Manthiram, Arumugam},
abstractNote = {Although lithium–polysulfur (Li–polyS) batteries employing organic polymeric sulfur as a cathode material outperform the lithium–sulfur (Li–S) battery system, the relatively low sulfur loading (<2 mg cm–2) in the current Li–polyS batteries compromises the areal capacity, constraining their practicality. We present here a new cathode active material (a covalently grafted polysulfur–graphene nanocomposite (polySGN)) for ultrahigh-loading Li–polyS batteries. The new cathode active material polySGN offers several advantages: (i) the well-dispersed graphene sheets offer highly electrically conductive pathways for electrons to travel within the polySGN matrix; (ii) the intermediate organosulfide moieties alleviate irreversible sulfide deposition on electrodes; and (iii) the in situ formed coating layer on the cathode-side surface of the polymeric separator further reduces polysulfide migration. In conclusion, the Li–polyS batteries employing polySGN as the cathode active material accomplish the highest sulfur loading (up to 10.5 mg cm–2) and the highest areal capacity (~12 mA h cm–2) reported thus far in the literature.},
doi = {10.1021/acsenergylett.7b01031},
journal = {ACS Energy Letters},
number = 1,
volume = 3,
place = {United States},
year = {Wed Nov 29 00:00:00 EST 2017},
month = {Wed Nov 29 00:00:00 EST 2017}
}
Web of Science
Works referenced in this record:
The use of elemental sulfur as an alternative feedstock for polymeric materials
journal, April 2013
- Chung, Woo Jin; Griebel, Jared J.; Kim, Eui Tae
- Nature Chemistry, Vol. 5, Issue 6
Sulfur and Its Role In Modern Materials Science
journal, November 2016
- Boyd, Darryl A.
- Angewandte Chemie International Edition, Vol. 55, Issue 50
Polymerizations with elemental sulfur: A novel route to high sulfur content polymers for sustainability, energy and defense
journal, July 2016
- Griebel, Jared J.; Glass, Richard S.; Char, Kookheon
- Progress in Polymer Science, Vol. 58
The use of polymers in Li-S batteries: A review
journal, March 2017
- Dirlam, Philip T.; Glass, Richard S.; Char, Kookheon
- Journal of Polymer Science Part A: Polymer Chemistry, Vol. 55, Issue 10
Rechargeable Lithium–Sulfur Batteries
journal, July 2014
- Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
- Chemical Reviews, Vol. 114, Issue 23
Recent Approaches for the Direct Use of Elemental Sulfur in the Synthesis and Processing of Advanced Materials
journal, January 2015
- Lim, Jeewoo; Pyun, Jeffrey; Char, Kookheon
- Angewandte Chemie International Edition, Vol. 54, Issue 11
Sulfur-sulfur bond lengths, or can a bond length be estimated from a single parameter?
journal, October 1988
- Knop, Osvald.; Boyd, Russell J.; Choi, S. C.
- Journal of the American Chemical Society, Vol. 110, Issue 22
Inverse Vulcanization of Elemental Sulfur to Prepare Polymeric Electrode Materials for Li–S Batteries
journal, February 2014
- Simmonds, Adam G.; Griebel, Jared J.; Park, Jungjin
- ACS Macro Letters, Vol. 3, Issue 3
Elemental-Sulfur-Mediated Facile Synthesis of a Covalent Triazine Framework for High-Performance Lithium-Sulfur Batteries
journal, January 2016
- Talapaneni, Siddulu Naidu; Hwang, Tae Hoon; Je, Sang Hyun
- Angewandte Chemie International Edition, Vol. 55, Issue 9
Immobilization of sulfur in microgels for lithium–sulfur battery
journal, January 2016
- Chang, Aiping; Wu, Qingshi; Du, Xue
- Chemical Communications, Vol. 52, Issue 24
Copolymerization of Polythiophene and Sulfur To Improve the Electrochemical Performance in Lithium–Sulfur Batteries
journal, October 2015
- Oschmann, Bernd; Park, Jungjin; Kim, Chunjoong
- Chemistry of Materials, Vol. 27, Issue 20
Cardanol benzoxazine-Sulfur Copolymers for Li-S batteries: Symbiosis of Sustainability and Performance
journal, March 2016
- Shukla, Swapnil; Ghosh, Arnab; Sen, Uttam Kumar
- ChemistrySelect, Vol. 1, Issue 3
A new configured lithiated silicon–sulfur battery built on 3D graphene with superior electrochemical performances
journal, January 2016
- Li, Bin; Li, Songmei; Xu, Jingjing
- Energy & Environmental Science, Vol. 9, Issue 6
Inverse vulcanization of elemental sulfur and styrene for polymeric cathodes in Li‐S batteries
journal, September 2016
- Zhang, Yueyan; Griebel, Jared J.; Dirlam, Philip T.
- Journal of Polymer Science Part A: Polymer Chemistry, Vol. 55, Issue 1
Solution processible hyperbranched inverse-vulcanized polymers as new cathode materials in Li–S batteries
journal, January 2015
- Wei, Yangyang; Li, Xiang; Xu, Zhen
- Polymer Chemistry, Vol. 6, Issue 6
Inverse vulcanization of elemental sulfur with 1,4-diphenylbutadiyne for cathode materials in Li–S batteries
journal, January 2015
- Dirlam, Philip T.; Simmonds, Adam G.; Kleine, Tristan S.
- RSC Advances, Vol. 5, Issue 31
A Sulfur-Rich Copolymer@CNT Hybrid Cathode with Dual-Confinement of Polysulfides for High-Performance Lithium-Sulfur Batteries
journal, December 2016
- Hu, Guangjian; Sun, Zhenhua; Shi, Chao
- Advanced Materials, Vol. 29, Issue 11
Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium–sulfur batteries
journal, June 2015
- Kim, Hoon; Lee, Joungphil; Ahn, Hyungmin
- Nature Communications, Vol. 6, Issue 1
A new approach for recycling waste rubber products in Li–S batteries
journal, January 2017
- Yu, Byeong-Chul; Jung, Ji-Won; Park, Kyusung
- Energy & Environmental Science, Vol. 10, Issue 1
Graphene-based composite materials
journal, July 2006
- Stankovich, Sasha; Dikin, Dmitriy A.; Dommett, Geoffrey H. B.
- Nature, Vol. 442, Issue 7100, p. 282-286
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications
journal, September 2012
- Georgakilas, Vasilios; Otyepka, Michal; Bourlinos, Athanasios B.
- Chemical Reviews, Vol. 112, Issue 11
The chemistry of graphene oxide
journal, January 2010
- Dreyer, Daniel R.; Park, Sungjin; Bielawski, Christopher W.
- Chem. Soc. Rev., Vol. 39, Issue 1
High-performance polystyrene/graphene-based nanocomposites with excellent anti-corrosion properties
journal, January 2014
- Yu, Yuan-Hsiang; Lin, Yan-Yu; Lin, Chia-Hsuan
- Polym. Chem., Vol. 5, Issue 2
Oligoanilines as a suppressor of polysulfide shuttling in lithium–sulfur batteries
journal, January 2017
- Chang, Chi-Hao; Chung, Sheng-Heng; Han, Pauline
- Materials Horizons, Vol. 4, Issue 5
Bifunctional Separator with a Light-Weight Carbon-Coating for Dynamically and Statically Stable Lithium-Sulfur Batteries
journal, June 2014
- Chung, Sheng-Heng; Manthiram, Arumugam
- Advanced Functional Materials, Vol. 24, Issue 33
Works referencing / citing this record:
A 3D Nitrogen-Doped Graphene/TiN Nanowires Composite as a Strong Polysulfide Anchor for Lithium-Sulfur Batteries with Enhanced Rate Performance and High Areal Capacity
journal, September 2018
- Li, Zhaohuai; He, Qiu; Xu, Xu
- Advanced Materials, Vol. 30, Issue 45
Recent Advances in Applying Vulcanization/Inverse Vulcanization Methods to Achieve High-Performance Sulfur-Containing Polymer Cathode Materials for Li-S Batteries
journal, August 2018
- Zhao, Fulai; Li, Yu; Feng, Wei
- Small Methods, Vol. 2, Issue 11
Facile preparation of ultrafine Ti 4 O 7 nanoparticle-embedded porous carbon for high areal capacity lithium–sulfur batteries
journal, January 2018
- Chen, Ao; Liu, Weifang; Hu, Hang
- Journal of Materials Chemistry A, Vol. 6, Issue 41
Structural Design of Lithium–Sulfur Batteries: From Fundamental Research to Practical Application
journal, June 2018
- Yang, Xiaofei; Li, Xia; Adair, Keegan
- Electrochemical Energy Reviews, Vol. 1, Issue 3
Progress on the Critical Parameters for Lithium-Sulfur Batteries to be Practically Viable
journal, May 2018
- Chung, Sheng-Heng; Chang, Chi-Hao; Manthiram, Arumugam
- Advanced Functional Materials, Vol. 28, Issue 28
Elucidating the reaction kinetics of lithium–sulfur batteries by operando XRD based on an open-hollow S@MnO 2 cathode
journal, January 2019
- Huang, Shaozhuan; Liu, Lixiang; Wang, Ye
- Journal of Materials Chemistry A, Vol. 7, Issue 12
A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries
journal, January 2019
- Li, Yun; Murphy, Ian A.; Chen, Ying
- Journal of Materials Chemistry A, Vol. 7, Issue 21
2D MXene nanosheets enable small-sulfur electrodes to be flexible for lithium–sulfur batteries
journal, January 2019
- Zhao, Qian; Zhu, Qizhen; Miao, Jiawei
- Nanoscale, Vol. 11, Issue 17
Wet-spinning assembly of continuous and macroscopic graphene oxide/polyacrylonitrile reinforced composite fibers with enhanced mechanical properties and thermal stability: Wet-spinning assembly of continuous and macroscopic graphene oxide/polyacrylonitrile
journal, July 2018
- Zhao, Renhai; Tian, Mingwei; Qu, Lijun
- Journal of Applied Polymer Science, Vol. 136, Issue 3
Synthesis and Applications of Polymers Made by Inverse Vulcanization
journal, May 2019
- Chalker, Justin M.; Worthington, Max J. H.; Lundquist, Nicholas A.
- Topics in Current Chemistry, Vol. 377, Issue 3
Trapping of Polysulfides with Sulfur‐Rich Poly Ionic Liquid Cathode Materials for Ultralong‐Life Lithium–Sulfur Batteries
journal, January 2020
- Liu, Xu; Lu, Yu; Zeng, Qinghui
- ChemSusChem, Vol. 13, Issue 4
Current Status and Future Prospects of Metal–Sulfur Batteries
journal, May 2019
- Chung, Sheng‐Heng; Manthiram, Arumugam
- Advanced Materials, Vol. 31, Issue 27