Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium–Sulfur Batteries

Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li–S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to...

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Published in	Journal of the American Chemical Society Vol. 141; no. 9; pp. 3977 - 3985
Main Authors	Du, Zhenzhen, Chen, Xingjia, Hu, Wei, Chuang, Chenghao, Xie, Shuai, Hu, Ajuan, Yan, Wensheng, Kong, Xianghua, Wu, Xiaojun, Ji, Hengxing, Wan, Li-Jun
Format	Journal Article
Language	English
Published	United States American Chemical Society 06.03.2019
Subjects	batteries catalysts cobalt electrochemistry electrodes energy energy density graphene X-ray absorption spectroscopy
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Abstract	Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li–S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co–N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co–N–C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co–N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g–1, and it exhibits an areal capacity of 5.1 mAh cm–2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm–2 on the electrode disk.
AbstractList	Because of their high theoretical energy density and low cost, lithium-sulfur (Li-S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li-S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co-N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co-N-C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co-N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g-1, and it exhibits an areal capacity of 5.1 mAh cm-2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm-2 on the electrode disk.Because of their high theoretical energy density and low cost, lithium-sulfur (Li-S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li-S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co-N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co-N-C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co-N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g-1, and it exhibits an areal capacity of 5.1 mAh cm-2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm-2 on the electrode disk. Because of their high theoretical energy density and low cost, lithium-sulfur (Li-S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li-S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co-N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co-N-C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li S in discharge and charge processes, respectively. The S@Co-N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g , and it exhibits an areal capacity of 5.1 mAh cm with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm on the electrode disk. Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li–S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li₂S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co–N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co–N–C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li₂S in discharge and charge processes, respectively. The S@Co–N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g–¹, and it exhibits an areal capacity of 5.1 mAh cm–² with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm–² on the electrode disk. Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li–S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co–N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co–N–C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co–N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g–1, and it exhibits an areal capacity of 5.1 mAh cm–2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm–2 on the electrode disk.
Author	Chen, Xingjia Hu, Ajuan Ji, Hengxing Du, Zhenzhen Yan, Wensheng Kong, Xianghua Xie, Shuai Wan, Li-Jun Hu, Wei Chuang, Chenghao Wu, Xiaojun
AuthorAffiliation	Chinese Academy of Sciences Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, iChEM, Department of Applied Chemistry Tamkang University National Synchrotron Radiation Laboratory CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry Hefei National Laboratory for Physical Sciences at the Microscales, Synergetic Innovation of Quantum Information & Quantum Technology, CAS Key Laboratory of Materials for Energy Conversion, and CAS Center for Excellence in Nanoscience, Department of Materials Sciences and Engineering School of Chemistry and Chemical Engineering Department of Physics
AuthorAffiliation_xml	– name: CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry – name: School of Chemistry and Chemical Engineering – name: Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, iChEM, Department of Applied Chemistry – name: Chinese Academy of Sciences – name: National Synchrotron Radiation Laboratory – name: Department of Physics – name: Hefei National Laboratory for Physical Sciences at the Microscales, Synergetic Innovation of Quantum Information & Quantum Technology, CAS Key Laboratory of Materials for Energy Conversion, and CAS Center for Excellence in Nanoscience, Department of Materials Sciences and Engineering – name: Tamkang University
Author_xml	– sequence: 1 givenname: Zhenzhen surname: Du fullname: Du, Zhenzhen organization: School of Chemistry and Chemical Engineering – sequence: 2 givenname: Xingjia surname: Chen fullname: Chen, Xingjia – sequence: 3 givenname: Wei surname: Hu fullname: Hu, Wei – sequence: 4 givenname: Chenghao surname: Chuang fullname: Chuang, Chenghao organization: Tamkang University – sequence: 5 givenname: Shuai surname: Xie fullname: Xie, Shuai – sequence: 6 givenname: Ajuan surname: Hu fullname: Hu, Ajuan – sequence: 7 givenname: Wensheng orcidid: 0000-0001-6297-4589 surname: Yan fullname: Yan, Wensheng – sequence: 8 givenname: Xianghua surname: Kong fullname: Kong, Xianghua email: kongxh@hfut.edu.cn organization: School of Chemistry and Chemical Engineering – sequence: 9 givenname: Xiaojun orcidid: 0000-0003-3606-1211 surname: Wu fullname: Wu, Xiaojun email: xjwu@ustc.edu.cn – sequence: 10 givenname: Hengxing orcidid: 0000-0003-2851-9878 surname: Ji fullname: Ji, Hengxing email: jihengx@ustc.edu.cn – sequence: 11 givenname: Li-Jun orcidid: 0000-0002-0656-0936 surname: Wan fullname: Wan, Li-Jun organization: Chinese Academy of Sciences
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/30764605$$D View this record in MEDLINE/PubMed
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Snippet	Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The... Because of their high theoretical energy density and low cost, lithium-sulfur (Li-S) batteries are promising next-generation energy storage devices. The...
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Title	Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium–Sulfur Batteries
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