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Title: 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:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6];  [6]; ORCiD logo [6]; ORCiD logo [6];  [6];  [7]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [8]
  1. Stanford Univ., CA (United States); Tsinghua Univ., Beijing (China)
  2. Curtin Univ., Perth, WA (Australia)
  3. Beihang Univ., Beijing (China)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Australian Nuclear Science and Technology Organisation (ANSTO), Melbourne, VIC (Australia). Australian Synchrotron
  6. Stanford Univ., CA (United States)
  7. Chinese Academy of Sciences, Shenyang (China)
  8. 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 (NNSFC); 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. 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, & 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}
}

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