Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries

Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithi...

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Main Authors: Zhou, G., Zhao, Shiyong, Wang, T., Yang, S.Z., Johannessen, B., Chen, H., Liu, C., Ye, Y., Wu, Y., Peng, Y., Jiang, San Ping, Zhang, Q., Cui, Y.
Format: Journal Article
Language:English
Published: AMER CHEMICAL SOC 2020
Subjects:
Online Access:http://purl.org/au-research/grants/arc/DP150102044
http://hdl.handle.net/20.500.11937/90996
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author Zhou, G.
Zhao, Shiyong
Wang, T.
Yang, S.Z.
Johannessen, B.
Chen, H.
Liu, C.
Ye, Y.
Wu, Y.
Peng, Y.
Liu, C.
Jiang, San Ping
Zhang, Q.
Cui, Y.
author_facet Zhou, G.
Zhao, Shiyong
Wang, T.
Yang, S.Z.
Johannessen, B.
Chen, H.
Liu, C.
Ye, Y.
Wu, Y.
Peng, Y.
Liu, C.
Jiang, San Ping
Zhang, Q.
Cui, Y.
author_sort Zhou, G.
building Curtin Institutional Repository
collection Online Access
description Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, 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 provides solutions for the development of high energy/power density Li-S batteries.
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institution Curtin University Malaysia
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publishDate 2020
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spelling curtin-20.500.11937-909962023-05-15T00:00:35Z Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries Zhou, G. Zhao, Shiyong Wang, T. Yang, S.Z. Johannessen, B. Chen, H. Liu, C. Ye, Y. Wu, Y. Peng, Y. Liu, C. Jiang, San Ping Zhang, Q. Cui, Y. Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Science & Technology - Other Topics Materials Science Physics Single-atom catalysts lithium-sulfur batteries catalytic conversion graphene density functional theory simulation LITHIUM POLYSULFIDES OXIDATION HOSTS Single-atom catalysts catalytic conversion density functional theory simulation graphene lithium−sulfur batteries Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, 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 provides solutions for the development of high energy/power density Li-S batteries. 2020 Journal Article http://hdl.handle.net/20.500.11937/90996 10.1021/acs.nanolett.9b04719 English http://purl.org/au-research/grants/arc/DP150102044 http://purl.org/au-research/grants/arc/DP180100568 http://purl.org/au-research/grants/arc/DP180100731 AMER CHEMICAL SOC fulltext
spellingShingle Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Applied
Physics, Condensed Matter
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
Single-atom catalysts
lithium-sulfur batteries
catalytic conversion
graphene
density functional theory simulation
LITHIUM
POLYSULFIDES
OXIDATION
HOSTS
Single-atom catalysts
catalytic conversion
density functional theory simulation
graphene
lithium−sulfur batteries
Zhou, G.
Zhao, Shiyong
Wang, T.
Yang, S.Z.
Johannessen, B.
Chen, H.
Liu, C.
Ye, Y.
Wu, Y.
Peng, Y.
Liu, C.
Jiang, San Ping
Zhang, Q.
Cui, Y.
Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title_full Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title_fullStr Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title_full_unstemmed Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title_short Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries
title_sort theoretical calculation guided design of single-atom catalysts toward fast kinetic and long-life li-s batteries
topic Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Applied
Physics, Condensed Matter
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
Single-atom catalysts
lithium-sulfur batteries
catalytic conversion
graphene
density functional theory simulation
LITHIUM
POLYSULFIDES
OXIDATION
HOSTS
Single-atom catalysts
catalytic conversion
density functional theory simulation
graphene
lithium−sulfur batteries
url http://purl.org/au-research/grants/arc/DP150102044
http://purl.org/au-research/grants/arc/DP150102044
http://purl.org/au-research/grants/arc/DP150102044
http://hdl.handle.net/20.500.11937/90996