Enhancing Chemical Interaction of Polysulfide and Carbon through Synergetic Nitrogen and Phosphorus Doping
Abstract
The shuttling effect of the polysulfide (PS) is the most detrimental factor that causes capacity fading of Li–S batteries. By substituting carbon atoms with heteroatoms, the host materials can provide a chemical interaction with PS to trap it within the electrochemically active range of the cathode. In this study, first-principles-based calculations identify the most stable nitrogen (N) and phosphorus (P) codoped atomic structures and their corresponding adsorption energy toward different PS species. Based on the simulated predictions, we introduce a glucosamine-derived carbon nanotube aerogel (CNA) with a secondary dopant of P during the synergetic polymerization and carbonization process. The N–P codoped CNA and S composite (NPCNA-S) renders a highly stable performance even at a sulfur loading of 3.5 mg cm–2. In conclusion, the specific capacity is >900 mAh g–1 and the stabilized capacity retention is >70% over 450 cycles at 0.2 C rate (1 C = 1675 mA g–1).
- Authors:
-
[1];
[3];
[1];
[1]
- Washington State Univ., Pullman, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Washington State Univ., Pullman, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1772336
- Grant/Contract Number:
- SC0014560
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Sustainable Chemistry & Engineering
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 2; Journal ID: ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS; Carbon nanotube aerogel; Li−S battery; Polysulfide; Nitrogen and phosphorus doping; Chemical interaction; Sulfur; Electrodes; Batteries; Doping; Materials
Citation Formats
Song, Junhua, Zheng, Jianming, Zhang, Renqin, Fu, Shaofang, Zhu, Chengzhou, Feng, Shuo, McEwen, Jean-Sabin, Du, Dan, Li, Xiaolin, and Lin, Yuehe. Enhancing Chemical Interaction of Polysulfide and Carbon through Synergetic Nitrogen and Phosphorus Doping. United States: N. p., 2019.
Web. doi:10.1021/acssuschemeng.9b04719.
Song, Junhua, Zheng, Jianming, Zhang, Renqin, Fu, Shaofang, Zhu, Chengzhou, Feng, Shuo, McEwen, Jean-Sabin, Du, Dan, Li, Xiaolin, & Lin, Yuehe. Enhancing Chemical Interaction of Polysulfide and Carbon through Synergetic Nitrogen and Phosphorus Doping. United States. https://doi.org/10.1021/acssuschemeng.9b04719
Song, Junhua, Zheng, Jianming, Zhang, Renqin, Fu, Shaofang, Zhu, Chengzhou, Feng, Shuo, McEwen, Jean-Sabin, Du, Dan, Li, Xiaolin, and Lin, Yuehe. Thu .
"Enhancing Chemical Interaction of Polysulfide and Carbon through Synergetic Nitrogen and Phosphorus Doping". United States. https://doi.org/10.1021/acssuschemeng.9b04719. https://www.osti.gov/servlets/purl/1772336.
@article{osti_1772336,
title = {Enhancing Chemical Interaction of Polysulfide and Carbon through Synergetic Nitrogen and Phosphorus Doping},
author = {Song, Junhua and Zheng, Jianming and Zhang, Renqin and Fu, Shaofang and Zhu, Chengzhou and Feng, Shuo and McEwen, Jean-Sabin and Du, Dan and Li, Xiaolin and Lin, Yuehe},
abstractNote = {The shuttling effect of the polysulfide (PS) is the most detrimental factor that causes capacity fading of Li–S batteries. By substituting carbon atoms with heteroatoms, the host materials can provide a chemical interaction with PS to trap it within the electrochemically active range of the cathode. In this study, first-principles-based calculations identify the most stable nitrogen (N) and phosphorus (P) codoped atomic structures and their corresponding adsorption energy toward different PS species. Based on the simulated predictions, we introduce a glucosamine-derived carbon nanotube aerogel (CNA) with a secondary dopant of P during the synergetic polymerization and carbonization process. The N–P codoped CNA and S composite (NPCNA-S) renders a highly stable performance even at a sulfur loading of 3.5 mg cm–2. In conclusion, the specific capacity is >900 mAh g–1 and the stabilized capacity retention is >70% over 450 cycles at 0.2 C rate (1 C = 1675 mA g–1).},
doi = {10.1021/acssuschemeng.9b04719},
journal = {ACS Sustainable Chemistry & Engineering},
number = 2,
volume = 8,
place = {United States},
year = {Thu Dec 12 00:00:00 EST 2019},
month = {Thu Dec 12 00:00:00 EST 2019}
}
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Works referenced in this record:
A Soft Approach to Encapsulate Sulfur: Polyaniline Nanotubes for Lithium-Sulfur Batteries with Long Cycle Life
journal, January 2012
- Xiao, Lifen; Cao, Yuliang; Xiao, Jie
- Advanced Materials, Vol. 24, Issue 9, p. 1176-1181
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Fibrous Hybrid of Graphene and Sulfur Nanocrystals for High-Performance Lithium–Sulfur Batteries
journal, May 2013
- Zhou, Guangmin; Yin, Li-Chang; Wang, Da-Wei
- ACS Nano, Vol. 7, Issue 6
Dual-Confined Flexible Sulfur Cathodes Encapsulated in Nitrogen-Doped Double-Shelled Hollow Carbon Spheres and Wrapped with Graphene for Li-S Batteries
journal, February 2015
- Zhou, Guangmin; Zhao, Yubao; Manthiram, Arumugam
- Advanced Energy Materials, Vol. 5, Issue 9
Nitrogen- and phosphorus-co-doped carbons with tunable enhanced surface areas promoted by the doping additives
journal, January 2013
- Paraknowitsch, Jens Peter; Zhang, Yuanjian; Wienert, Björn
- Chemical Communications, Vol. 49, Issue 12
Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium–Sulfur Battery Cathode Material with High Capacity and Cycling Stability
journal, July 2011
- Wang, Hailiang; Yang, Yuan; Liang, Yongye
- Nano Letters, Vol. 11, Issue 7, p. 2644-2647
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Tailoring Pore Size of Nitrogen-Doped Hollow Carbon Nanospheres for Confining Sulfur in Lithium-Sulfur Batteries
journal, January 2015
- Zhou, Weidong; Wang, Chongmin; Zhang, Qinglin
- Advanced Energy Materials, Vol. 5, Issue 16
Heteroatom doped carbons prepared by the pyrolysis of bio-derived amino acids as highly active catalysts for oxygen electro-reduction reactions
journal, January 2011
- Choi, Chang Hyuck; Park, Sung Hyeon; Woo, Seong Ihl
- Green Chem., Vol. 13, Issue 2
Hydrophilic Hierarchical Nitrogen-Doped Carbon Nanocages for Ultrahigh Supercapacitive Performance
journal, April 2015
- Zhao, Jin; Lai, Hongwei; Lyu, Zhiyang
- Advanced Materials, Vol. 27, Issue 23
Review—The Importance of Chemical Interactions between Sulfur Host Materials and Lithium Polysulfides for Advanced Lithium-Sulfur Batteries
journal, January 2015
- Pang, Quan; Liang, Xiao; Kwok, C. Y.
- Journal of The Electrochemical Society, Vol. 162, Issue 14
Improved lithium–sulfur cells with a treated carbon paper interlayer
journal, January 2013
- Zu, Chenxi; Su, Yu-Sheng; Fu, Yongzhu
- Physical Chemistry Chemical Physics, Vol. 15, Issue 7
Template-directed synthesis of nitrogen- and sulfur-codoped carbon nanowire aerogels with enhanced electrocatalytic performance for oxygen reduction
journal, December 2016
- Fu, Shaofang; Zhu, Chengzhou; Song, Junhua
- Nano Research, Vol. 10, Issue 6
Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts
journal, February 2017
- Zhu, Chengzhou; Fu, Shaofang; Song, Junhua
- Small, Vol. 13, Issue 15
Sulphur–TiO2 yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries
journal, January 2013
- Wei Seh, Zhi; Li, Weiyang; Cha, Judy J.
- Nature Communications, Vol. 4, Article No. 1331
Operando Spectromicroscopy of Sulfur Species in Lithium-Sulfur Batteries
journal, June 2017
- Miller, Elizabeth C.; Kasse, Robert M.; Heath, Khloe N.
- Journal of The Electrochemical Society, Vol. 165, Issue 1
How to Obtain Reproducible Results for Lithium Sulfur Batteries?
journal, January 2013
- Zheng, Jianming; Lv, Dongping; Gu, Meng
- Journal of The Electrochemical Society, Vol. 160, Issue 11
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
journal, January 2012
- Su, Yu-Sheng; Manthiram, Arumugam
- Nature Communications, Vol. 3, Article No. 1166
Thermodynamic stability of nitrogen functionalities and defects in graphene and graphene nanoribbons from first principles
journal, November 2019
- Ayiania, Michael; Hensley, Alyssa J. R.; Groden, Kyle
- Carbon, Vol. 152
Enhancing lithium–sulphur battery performance by strongly binding the discharge products on amino-functionalized reduced graphene oxide
journal, September 2014
- Wang, Zhiyu; Dong, Yanfeng; Li, Hongjiang
- Nature Communications, Vol. 5, Issue 1
High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene
journal, July 2014
- Qiu, Yongcai; Li, Wanfei; Zhao, Wen
- Nano Letters, Vol. 14, Issue 8
Kinetically Controlled Synthesis of Pt-Based One-Dimensional Hierarchically Porous Nanostructures with Large Mesopores as Highly Efficient ORR Catalysts
journal, December 2016
- Fu, Shaofang; Zhu, Chengzhou; Song, Junhua
- ACS Applied Materials & Interfaces, Vol. 8, Issue 51
The characterization of nitrogen-enriched activated carbons by IR, XPS and LSER methods
journal, August 2002
- Burg, Philippe; Fydrych, Peggy; Cagniant, Denise
- Carbon, Vol. 40, Issue 9
Long-life Li/polysulphide batteries with high sulphur loading enabled by lightweight three-dimensional nitrogen/sulphur-codoped graphene sponge
journal, July 2015
- Zhou, Guangmin; Paek, Eunsu; Hwang, Gyeong S.
- Nature Communications, Vol. 6, Issue 1
A porous nitrogen and phosphorous dual doped graphene blocking layer for high performance Li–S batteries
journal, January 2015
- Gu, Xingxing; Tong, Chuan-jia; Lai, Chao
- Journal of Materials Chemistry A, Vol. 3, Issue 32
Nitrogen and Phosphorus Dual-Doped Graphene/Carbon Nanosheets as Bifunctional Electrocatalysts for Oxygen Reduction and Evolution
journal, June 2015
- Li, Rong; Wei, Zidong; Gou, Xinglong
- ACS Catalysis, Vol. 5, Issue 7
Rechargeable Lithium–Sulfur Batteries
journal, July 2014
- Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
- Chemical Reviews, Vol. 114, Issue 23
Investigation of the Self-Discharge Behavior of Lithium-Sulfur Batteries
journal, January 2016
- Knap, V.; Stroe, D. -I.; Swierczynski, M.
- Journal of The Electrochemical Society, Vol. 163, Issue 6
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Designing high-energy lithium–sulfur batteries
journal, January 2016
- Seh, Zhi Wei; Sun, Yongming; Zhang, Qianfan
- Chemical Society Reviews, Vol. 45, Issue 20
Opportunities and challenges for a sustainable energy future
journal, August 2012
- Chu, Steven; Majumdar, Arun
- Nature, Vol. 488, Issue 7411, p. 294-303
Nitrogen-containing carbons from phenol–formaldehyde resins and their catalytic activity in NO reduction with NH3
journal, January 2003
- Huang, Mei-Chiung; Teng, Hsisheng
- Carbon, Vol. 41, Issue 5
Potential for widespread electrification of personal vehicle travel in the United States
journal, August 2016
- Needell, Zachary A.; McNerney, James; Chang, Michael T.
- Nature Energy, Vol. 1, Issue 9
A metal-free bifunctional electrocatalyst for oxygen reduction and oxygen evolution reactions
journal, April 2015
- Zhang, Jintao; Zhao, Zhenghang; Xia, Zhenhai
- Nature Nanotechnology, Vol. 10, Issue 5
Yolk–Shell Structure of Polyaniline-Coated Sulfur for Lithium–Sulfur Batteries
journal, October 2013
- Zhou, Weidong; Yu, Yingchao; Chen, Hao
- Journal of the American Chemical Society, Vol. 135, Issue 44
Strong Lithium Polysulfide Chemisorption on Electroactive Sites of Nitrogen-Doped Carbon Composites For High-Performance Lithium-Sulfur Battery Cathodes
journal, February 2015
- Song, Jiangxuan; Gordin, Mikhail L.; Xu, Terrence
- Angewandte Chemie International Edition, Vol. 54, Issue 14
Transport Properties of Polysulfide Species in Lithium–Sulfur Battery Electrolytes: Coupling of Experiment and Theory
journal, July 2016
- Safari, M.; Kwok, C. Y.; Nazar, L. F.
- ACS Central Science, Vol. 2, Issue 8
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Long-Life and High-Areal-Capacity Li–S Batteries Enabled by a Light-Weight Polar Host with Intrinsic Polysulfide Adsorption
journal, March 2016
- Pang, Quan; Nazar, Linda F.
- ACS Nano, Vol. 10, Issue 4
High-Level Doping of Nitrogen, Phosphorus, and Sulfur into Activated Carbon Monoliths and Their Electrochemical Capacitances
journal, June 2015
- Hasegawa, George; Deguchi, Takeru; Kanamori, Kazuyoshi
- Chemistry of Materials, Vol. 27, Issue 13
Phosphorus-Doped Graphite Layers with High Electrocatalytic Activity for the O2 Reduction in an Alkaline Medium
journal, March 2011
- Liu, Zi-Wu; Peng, Feng; Wang, Hong-Juan
- Angewandte Chemie International Edition, Vol. 50, Issue 14