Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries
Abstract
Lithium–sulfur (Li–S) batteries are enticing next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. Yet, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge–charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g–1 at 3 C rate), and long-life Li–S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and offers solutions for the development of high energy/power density Li–S batteries.
- Authors:
-
[1];
[4];
[6];
[6];
[6];
[2];
[3];
[8]
- Stanford Univ., CA (United States); Tsinghua Univ., Beijing (China)
- Curtin Univ., Perth, WA (Australia)
- Beihang Univ., Beijing (China)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Australian Nuclear Science and Technology Organisation (ANSTO), Melbourne, VIC (Australia). Australian Synchrotron
- Stanford Univ., CA (United States)
- Chinese Academy of Sciences, Shenyang (China)
- Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); Beijing Natural Science Foundation
- OSTI Identifier:
- 1617143
- Grant/Contract Number:
- AC02-76SF00515; NCET-12-0033; DP150102044; DP180100568; DP180100731; 11404017; 51872293
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 2; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Single-atom catalysts; lithium−sulfur batteries; catalytic conversion; graphene; density functional theory simulation
Citation Formats
Zhou, Guangmin, Zhao, Shiyong, Wang, Tianshuai, Yang, Shi-Ze, Johannessen, Bernt, Chen, Hao, Liu, Chenwei, Ye, Yusheng, Wu, Yecun, Peng, Yucan, Liu, Chang, Jiang, San Ping, Zhang, Qianfan, and Cui, Yi. Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries. United States: N. p., 2019.
Web. doi:10.1021/acs.nanolett.9b04719.
Zhou, Guangmin, Zhao, Shiyong, Wang, Tianshuai, Yang, Shi-Ze, Johannessen, Bernt, Chen, Hao, Liu, Chenwei, Ye, Yusheng, Wu, Yecun, Peng, Yucan, Liu, Chang, Jiang, San Ping, Zhang, Qianfan, & Cui, Yi. Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries. United States. https://doi.org/10.1021/acs.nanolett.9b04719
Zhou, Guangmin, Zhao, Shiyong, Wang, Tianshuai, Yang, Shi-Ze, Johannessen, Bernt, Chen, Hao, Liu, Chenwei, Ye, Yusheng, Wu, Yecun, Peng, Yucan, Liu, Chang, Jiang, San Ping, Zhang, Qianfan, and Cui, Yi. Mon .
"Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries". United States. https://doi.org/10.1021/acs.nanolett.9b04719. https://www.osti.gov/servlets/purl/1617143.
@article{osti_1617143,
title = {Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries},
author = {Zhou, Guangmin and Zhao, Shiyong and Wang, Tianshuai and Yang, Shi-Ze and Johannessen, Bernt and Chen, Hao and Liu, Chenwei and Ye, Yusheng and Wu, Yecun and Peng, Yucan and Liu, Chang and Jiang, San Ping and Zhang, Qianfan and Cui, Yi},
abstractNote = {Lithium–sulfur (Li–S) batteries are enticing next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. Yet, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge–charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g–1 at 3 C rate), and long-life Li–S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and offers solutions for the development of high energy/power density Li–S batteries.},
doi = {10.1021/acs.nanolett.9b04719},
journal = {Nano Letters},
number = 2,
volume = 20,
place = {United States},
year = {2019},
month = {12}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 265 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Li–O2 and Li–S batteries with high energy storage
journal, January 2012
- Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
- Nature Materials, Vol. 11, Issue 1, p. 19-29
Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes
journal, September 2016
- Pang, Quan; Liang, Xiao; Kwok, Chun Yuen
- Nature Energy, Vol. 1, Issue 9
Design of Complex Nanomaterials for Energy Storage: Past Success and Future Opportunity
journal, December 2017
- Liu, Yayuan; Zhou, Guangmin; Liu, Kai
- Accounts of Chemical Research, Vol. 50, Issue 12
Rechargeable Lithium–Sulfur Batteries
journal, July 2014
- Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
- Chemical Reviews, Vol. 114, Issue 23
Nanowires for Electrochemical Energy Storage
journal, September 2019
- Zhou, Guangmin; Xu, Lin; Hu, Guangwu
- Chemical Reviews, Vol. 119, Issue 20
Suppressing Polysulfide Dissolution via Cohesive Forces by Interwoven Carbon Nanofibers for High-Areal-Capacity Lithium–Sulfur Batteries
journal, December 2017
- Yun, Jong Hyuk; Kim, Joo-Hyung; Kim, Do Kyung
- Nano Letters, Vol. 18, Issue 1
Powering Lithium–Sulfur Battery Performance by Propelling Polysulfide Redox at Sulfiphilic Hosts
journal, December 2015
- Yuan, Zhe; Peng, Hong-Jie; Hou, Ting-Zheng
- Nano Letters, Vol. 16, Issue 1
Catalytic Effects in Lithium-Sulfur Batteries: Promoted Sulfur Transformation and Reduced Shuttle Effect
journal, September 2017
- Liu, Donghai; Zhang, Chen; Zhou, Guangmin
- Advanced Science, Vol. 5, Issue 1
Free-standing TiO2 nanowire-embedded graphene hybrid membrane for advanced Li/dissolved polysulfide batteries
journal, March 2015
- Zhou, Guangmin; Zhao, Yubao; Zu, Chenxi
- Nano Energy, Vol. 12
Enhancing Catalytic Activity of Titanium Oxide in Lithium–Sulfur Batteries by Band Engineering
journal, May 2019
- Wang, Yuankun; Zhang, Ruifang; Chen, Jie
- Advanced Energy Materials, Vol. 9, Issue 24
Catalytic oxidation of Li 2 S on the surface of metal sulfides for Li−S batteries
journal, January 2017
- Zhou, Guangmin; Tian, Hongzhen; Jin, Yang
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 5
A highly efficient polysulfide mediator for lithium–sulfur batteries
journal, January 2015
- Liang, Xiao; Hart, Connor; Pang, Quan
- Nature Communications, Vol. 6, Issue 1
Propelling polysulfides transformation for high-rate and long-life lithium–sulfur batteries
journal, March 2017
- Zheng, Cheng; Niu, Shuzhang; Lv, Wei
- Nano Energy, Vol. 33
Carbon@titanium nitride dual shell nanospheres as multi-functional hosts for lithium sulfur batteries
journal, January 2019
- Wang, Yuankun; Zhang, Ruifang; Pang, Yuan-chao
- Energy Storage Materials, Vol. 16
Promoting the Transformation of Li 2 S 2 to Li 2 S: Significantly Increasing Utilization of Active Materials for High‐Sulfur‐Loading Li–S Batteries
journal, April 2019
- Yang, Xiaofei; Gao, Xuejie; Sun, Qian
- Advanced Materials, Vol. 31, Issue 25
Conductive porous vanadium nitride/graphene composite as chemical anchor of polysulfides for lithium-sulfur batteries
journal, March 2017
- Sun, Zhenhua; Zhang, Jingqi; Yin, Lichang
- Nature Communications, Vol. 8, Issue 1
Phosphorene as a Polysulfide Immobilizer and Catalyst in High-Performance Lithium-Sulfur Batteries
journal, October 2016
- Li, Lu; Chen, Long; Mukherjee, Sankha
- Advanced Materials, Vol. 29, Issue 2
Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis
journal, April 2013
- Yang, Xiao-Feng; Wang, Aiqin; Qiao, Botao
- Accounts of Chemical Research, Vol. 46, Issue 8
Catalysis by Supported Single Metal Atoms
journal, November 2016
- Liu, Jingyue
- ACS Catalysis, Vol. 7, Issue 1
Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011
- Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng
- Nature Chemistry, Vol. 3, Issue 8
Single-Atom Electrocatalysts
journal, October 2017
- Zhu, Chengzhou; Fu, Shaofang; Shi, Qiurong
- Angewandte Chemie International Edition, Vol. 56, Issue 45
Heterogeneous single-atom catalysis
journal, May 2018
- Wang, Aiqin; Li, Jun; Zhang, Tao
- Nature Reviews Chemistry, Vol. 2, Issue 6
A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018
- Xu, Haoxiang; Cheng, Daojian; Cao, Dapeng
- Nature Catalysis, Vol. 1, Issue 5
Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations
journal, March 2012
- Kyriakou, Georgios; Boucher, Matthew B.; Jewell, April D.
- Science, Vol. 335, Issue 6073
Single-atom catalyst boosts electrochemical conversion reactions in batteries
journal, March 2019
- Wang, Jian; Jia, Lujie; Zhong, Jun
- Energy Storage Materials, Vol. 18
Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium–Sulfur Batteries
journal, February 2019
- Du, Zhenzhen; Chen, Xingjia; Hu, Wei
- Journal of the American Chemical Society, Vol. 141, Issue 9
Implanting Atomic Cobalt within Mesoporous Carbon toward Highly Stable Lithium–Sulfur Batteries
journal, September 2019
- Xie, Jin; Li, Bo‐Quan; Peng, Hong‐Jie
- Advanced Materials, Vol. 31, Issue 43
Single Nickel Atoms on Nitrogen‐Doped Graphene Enabling Enhanced Kinetics of Lithium–Sulfur Batteries
journal, August 2019
- Zhang, Linlin; Liu, Daobin; Muhammad, Zahir
- Advanced Materials, Vol. 31, Issue 40
Computational understanding of Li-ion batteries
journal, March 2016
- Urban, Alexander; Seo, Dong-Hwa; Ceder, Gerbrand
- npj Computational Materials, Vol. 2, Issue 1
An Analogous Periodic Law for Strong Anchoring of Polysulfides on Polar Hosts in Lithium Sulfur Batteries: S- or Li-Binding on First-Row Transition-Metal Sulfides?
journal, March 2017
- Chen, Xiang; Peng, Hong-Jie; Zhang, Rui
- ACS Energy Letters, Vol. 2, Issue 4
A Universal Seeding Strategy to Synthesize Single Atom Catalysts on 2D Materials for Electrocatalytic Applications
journal, November 2019
- Zhao, Shiyong; Chen, Guangxu; Zhou, Guangmin
- Advanced Functional Materials, Vol. 30, Issue 6
Understanding the Anchoring Effect of Two-Dimensional Layered Materials for Lithium–Sulfur Batteries
journal, May 2015
- Zhang, Qianfan; Wang, Yapeng; Seh, Zhi Wei
- Nano Letters, Vol. 15, Issue 6
Energy efficient synthesis of highly ordered mesoporous carbon nitrides with uniform rods and their superior CO 2 adsorption capacity
journal, January 2017
- Lakhi, Kripal S.; Park, Dae-Hwan; Singh, Gurwinder
- Journal of Materials Chemistry A, Vol. 5, Issue 31
Identification of catalytic sites for oxygen reduction and oxygen evolution in N-doped graphene materials: Development of highly efficient metal-free bifunctional electrocatalyst
journal, April 2016
- Yang, Hong Bin; Miao, Jianwei; Hung, Sung-Fu
- Science Advances, Vol. 2, Issue 4
Local structural order in the disordered vanadium tetracyanoethylene room-temperature molecule-based magnet
journal, August 2004
- Haskel, D.; Islam, Z.; Lang, J.
- Physical Review B, Vol. 70, Issue 5
Lithium/Sulfur Cell Discharge Mechanism: An Original Approach for Intermediate Species Identification
journal, April 2012
- Barchasz, Céline; Molton, Florian; Duboc, Carole
- Analytical Chemistry, Vol. 84, 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 Graphene-Pure-Sulfur Sandwich Structure for Ultrafast, Long-Life Lithium-Sulfur Batteries
journal, November 2013
- Zhou, Guangmin; Pei, Songfeng; Li, Lu
- Advanced Materials, Vol. 26, Issue 4