In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries

Yan Xu; Yifan Ye; Shuyang Zhao; Jun Feng; Jia Li; Hao Chen; Ankun Yang; Feifei Shi; Lujie Jia; Yang Wu; Xiaoyun Yu; Per Anders Glans-Suzuki; Yi Cui; Jinghua Guo; Yuegang Zhang

doi:10.1021/acs.nanolett.8b05208

In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries

Yan Xu, Yifan Ye, Shuyang Zhao, Jun Feng, Jia Li, Hao Chen, Ankun Yang, Feifei Shi, Lujie Jia, Yang Wu, Xiaoyun Yu, Per Anders Glans-Suzuki, Yi Cui, Jinghua Guo, Yuegang Zhang

Research output: Contribution to journal › Article › peer-review

30 Scopus citations

Abstract

The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)₂-AlCl₃ electrolyte. We find that the capacity degradation is mainly due to the formation of irreversible discharge products, such as MgS and Mg₃S₈, through a direct electrochemical deposition or a chemical disproportionation of intermediate polysulfide. In light of the fundamental understanding, we propose to use TiS₂ as a catalyst to activate the irreversible reaction of low-order MgS_x and MgS, which results in an increased discharging capacity up to 900 mAh·g^-1 and a longer cycling life.

Original language	English (US)
Pages (from-to)	2928-2934
Number of pages	7
Journal	Nano letters
Volume	19
Issue number	5
DOIs	https://doi.org/10.1021/acs.nanolett.8b05208
State	Published - May 8 2019

All Science Journal Classification (ASJC) codes

Bioengineering
Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.8b05208

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Xu, Yan ; Ye, Yifan ; Zhao, Shuyang ; Feng, Jun ; Li, Jia ; Chen, Hao ; Yang, Ankun ; Shi, Feifei ; Jia, Lujie ; Wu, Yang ; Yu, Xiaoyun ; Glans-Suzuki, Per Anders ; Cui, Yi ; Guo, Jinghua ; Zhang, Yuegang. / In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries. In: Nano letters. 2019 ; Vol. 19, No. 5. pp. 2928-2934.

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title = "In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries",

abstract = "The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)2-AlCl3 electrolyte. We find that the capacity degradation is mainly due to the formation of irreversible discharge products, such as MgS and Mg3S8, through a direct electrochemical deposition or a chemical disproportionation of intermediate polysulfide. In light of the fundamental understanding, we propose to use TiS2 as a catalyst to activate the irreversible reaction of low-order MgSx and MgS, which results in an increased discharging capacity up to 900 mAh·g-1 and a longer cycling life.",

author = "Yan Xu and Yifan Ye and Shuyang Zhao and Jun Feng and Jia Li and Hao Chen and Ankun Yang and Feifei Shi and Lujie Jia and Yang Wu and Xiaoyun Yu and Glans-Suzuki, {Per Anders} and Yi Cui and Jinghua Guo and Yuegang Zhang",

note = "Funding Information: This work was supported by the National Key Research and Development Program of China (2016YFB0100100, 2017YFB0701600), the National Natural Science Foundation of China (No. 21433013, U11874036, U1832218), the CAS-DOE Joint Research Program (121E32KYSB20150004), CAS-Queensland Collaborative Science Fund (121E32KYSB20160032), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (Grant No. 2017BT01N111), and the Basic Research Project of Shenzhen (JCYJ20170412171430026). The S K-edge XAS experiment was performed on BL 5.3.1 at Advanced Light Source and BL 4-3 at Stanford Linear Accelerator Center. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. J.H.G. was also supported by the Joint Center for Energy Storage Research (JCESR). Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

year = "2019",

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doi = "10.1021/acs.nanolett.8b05208",

language = "English (US)",

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In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries. / Xu, Yan; Ye, Yifan; Zhao, Shuyang; Feng, Jun; Li, Jia; Chen, Hao; Yang, Ankun; Shi, Feifei; Jia, Lujie; Wu, Yang; Yu, Xiaoyun; Glans-Suzuki, Per Anders; Cui, Yi; Guo, Jinghua; Zhang, Yuegang.

In: Nano letters, Vol. 19, No. 5, 08.05.2019, p. 2928-2934.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries

AU - Xu, Yan

AU - Ye, Yifan

AU - Zhao, Shuyang

AU - Feng, Jun

AU - Li, Jia

AU - Chen, Hao

AU - Yang, Ankun

AU - Shi, Feifei

AU - Jia, Lujie

AU - Wu, Yang

AU - Yu, Xiaoyun

AU - Glans-Suzuki, Per Anders

AU - Cui, Yi

AU - Guo, Jinghua

AU - Zhang, Yuegang

N1 - Funding Information: This work was supported by the National Key Research and Development Program of China (2016YFB0100100, 2017YFB0701600), the National Natural Science Foundation of China (No. 21433013, U11874036, U1832218), the CAS-DOE Joint Research Program (121E32KYSB20150004), CAS-Queensland Collaborative Science Fund (121E32KYSB20160032), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (Grant No. 2017BT01N111), and the Basic Research Project of Shenzhen (JCYJ20170412171430026). The S K-edge XAS experiment was performed on BL 5.3.1 at Advanced Light Source and BL 4-3 at Stanford Linear Accelerator Center. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. J.H.G. was also supported by the Joint Center for Energy Storage Research (JCESR). Publisher Copyright: © 2019 American Chemical Society.

PY - 2019/5/8

Y1 - 2019/5/8

N2 - The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)2-AlCl3 electrolyte. We find that the capacity degradation is mainly due to the formation of irreversible discharge products, such as MgS and Mg3S8, through a direct electrochemical deposition or a chemical disproportionation of intermediate polysulfide. In light of the fundamental understanding, we propose to use TiS2 as a catalyst to activate the irreversible reaction of low-order MgSx and MgS, which results in an increased discharging capacity up to 900 mAh·g-1 and a longer cycling life.

AB - The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)2-AlCl3 electrolyte. We find that the capacity degradation is mainly due to the formation of irreversible discharge products, such as MgS and Mg3S8, through a direct electrochemical deposition or a chemical disproportionation of intermediate polysulfide. In light of the fundamental understanding, we propose to use TiS2 as a catalyst to activate the irreversible reaction of low-order MgSx and MgS, which results in an increased discharging capacity up to 900 mAh·g-1 and a longer cycling life.

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JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

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ER -

In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries

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