Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries are considered as a highly promising energy storage system due to their ultrahigh theoretical energy density. However, the sluggish kinetics of the complex multi-electron sulfur redox reactions seriously hinders the actual battery performance especially under practica...

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Main Authors: Meng Zhao, Xi-Yao Li, Xiang Chen, Bo-Quan Li, Stefan Kaskel, Qiang Zhang, Jia-Qi Huang
Format: Article
Language:English
Published: KeAi Communications Co. Ltd. 2021-11-01
Series:eScience
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S266714172100001X
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author Meng Zhao
Xi-Yao Li
Xiang Chen
Bo-Quan Li
Stefan Kaskel
Qiang Zhang
Jia-Qi Huang
author_facet Meng Zhao
Xi-Yao Li
Xiang Chen
Bo-Quan Li
Stefan Kaskel
Qiang Zhang
Jia-Qi Huang
author_sort Meng Zhao
collection DOAJ
description Lithium–sulfur (Li–S) batteries are considered as a highly promising energy storage system due to their ultrahigh theoretical energy density. However, the sluggish kinetics of the complex multi-electron sulfur redox reactions seriously hinders the actual battery performance especially under practical working conditions. Homogeneous redox mediation, through elaborately designing the additive molecules, is an effective approach to promote the sulfur redox kinetics. Herein a promoter of mixed organodiselenides (mixed-Se) is proposed to comprehensively improve the sulfur redox kinetics following the redox comediation principles. Concretely, diphenyl diselenide promotes the liquid–liquid conversion between polysulfides and the solid–liquid conversion regarding lithium sulfide oxidation to polysulfides, while dimethyl diselenide enhances the liquid–solid conversion regarding lithium sulfide deposition. Consequently, the mixed-Se promoter endows a high discharge capacity of 1002 mAh g−1 with high sulfur loading of 4.0 mg cm−2, a high capacity retention of 81.6% after 200 cycles at 0.5 C, and a high actual energy density of 384 Wh kg−1 at 0.025 C in 1.5 Ah-level Li–S pouch cells. This work affords an effective kinetic promoter to construct high-energy-density Li–S batteries and inspires molecular design of kinetic promoters toward targeted energy-related redox reactions.
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spelling doaj.art-438dab5eb77c4e129a2c265e18275b6b2022-12-22T04:42:05ZengKeAi Communications Co. Ltd.eScience2667-14172021-11-01114452Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteriesMeng Zhao0Xi-Yao Li1Xiang Chen2Bo-Quan Li3Stefan Kaskel4Qiang Zhang5Jia-Qi Huang6School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaSchool of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaDepartment of Inorganic Chemistry, Technische Universität Dresden, Bergstr. 66, Dresden 01069, GermanyBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China; Corresponding authors.School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China; Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China; Corresponding authors.Lithium–sulfur (Li–S) batteries are considered as a highly promising energy storage system due to their ultrahigh theoretical energy density. However, the sluggish kinetics of the complex multi-electron sulfur redox reactions seriously hinders the actual battery performance especially under practical working conditions. Homogeneous redox mediation, through elaborately designing the additive molecules, is an effective approach to promote the sulfur redox kinetics. Herein a promoter of mixed organodiselenides (mixed-Se) is proposed to comprehensively improve the sulfur redox kinetics following the redox comediation principles. Concretely, diphenyl diselenide promotes the liquid–liquid conversion between polysulfides and the solid–liquid conversion regarding lithium sulfide oxidation to polysulfides, while dimethyl diselenide enhances the liquid–solid conversion regarding lithium sulfide deposition. Consequently, the mixed-Se promoter endows a high discharge capacity of 1002 mAh g−1 with high sulfur loading of 4.0 mg cm−2, a high capacity retention of 81.6% after 200 cycles at 0.5 C, and a high actual energy density of 384 Wh kg−1 at 0.025 C in 1.5 Ah-level Li–S pouch cells. This work affords an effective kinetic promoter to construct high-energy-density Li–S batteries and inspires molecular design of kinetic promoters toward targeted energy-related redox reactions.http://www.sciencedirect.com/science/article/pii/S266714172100001XLithium–sulfur batteriesSulfur redox kineticsOrganodiselenideLithium polysulfidesRedox comediation
spellingShingle Meng Zhao
Xi-Yao Li
Xiang Chen
Bo-Quan Li
Stefan Kaskel
Qiang Zhang
Jia-Qi Huang
Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
eScience
Lithium–sulfur batteries
Sulfur redox kinetics
Organodiselenide
Lithium polysulfides
Redox comediation
title Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
title_full Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
title_fullStr Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
title_full_unstemmed Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
title_short Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium–sulfur batteries
title_sort promoting the sulfur redox kinetics by mixed organodiselenides in high energy density lithium sulfur batteries
topic Lithium–sulfur batteries
Sulfur redox kinetics
Organodiselenide
Lithium polysulfides
Redox comediation
url http://www.sciencedirect.com/science/article/pii/S266714172100001X
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