Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles
Abstract
Abstract We report a new approach for nanosilicon–graphene hybrids with uniquely stable solid electrolyte interphase. Expanded graphite is gently exfoliated creating “defect‐free” graphene that is non‐catalytic towards electrolyte decomposition, simultaneously introducing high mass loading (48 wt. %) Si nanoparticles. Silane surface treatment creates epoxy chemical tethers, mechanically binding nano‐Si to CMC binder through epoxy ring‐opening reaction while stabilizing the Si surface chemistry. Epoxy‐tethered silicon pristine–graphene hybrid “E‐Si‐pG” exhibits state‐of‐the‐art performance in full battery opposing commercial mass loading (12 mg cm −2 ) LiCoO 2 (LCO) cathode. At 0.4 C, with areal capacity of 1.62 mAh cm −2 and energy of 437 Wh kg −1 , achieving 1.32 mAh cm −2 , 340.4 Wh kg −1 at 1 C. After 150 cycles, it retains 1.25 mAh cm −2 , 306.5 Wh kg −1 . Sputter‐down XPS demonstrates survival of surface C‐Si‐O‐Si groups in E‐Si‐pG after repeated cycling. The discovered synergy between support defects, chemical‐mechanical stabilization of Si surfaces, and SEI‐related failure may become key LIB anode design rule.
- Authors:
-
[1];
[4]
- Institute of New-Energy and Low-Carbon Technology (INELT) Sichuan University Chengdu Sichuan 610065 China, Engineering Research Center of Alternative Energy Materials &, Devices Ministry of Education Sichuan University Chengdu Sichuan 610065 China
- Institute of New-Energy and Low-Carbon Technology (INELT) Sichuan University Chengdu Sichuan 610065 China
- Chemical &, Biomolecular Engineering Clarkson University Potsdam NY 13699 USA
- Walker Department of Mechanical Engineering The University of Texas at Austin Austin Texas 78712-1591 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1603182
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition) Journal Volume: 58 Journal Issue: 46; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Liu, Wei, Li, Hongju, Jin, Jialun, Wang, Yizhe, Zhang, Zheng, Chen, Zidong, Wang, Qin, Chen, Yungui, Paek, Eunsu, and Mitlin, David. Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles. Germany: N. p., 2019.
Web. doi:10.1002/anie.201906612.
Liu, Wei, Li, Hongju, Jin, Jialun, Wang, Yizhe, Zhang, Zheng, Chen, Zidong, Wang, Qin, Chen, Yungui, Paek, Eunsu, & Mitlin, David. Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles. Germany. https://doi.org/10.1002/anie.201906612
Liu, Wei, Li, Hongju, Jin, Jialun, Wang, Yizhe, Zhang, Zheng, Chen, Zidong, Wang, Qin, Chen, Yungui, Paek, Eunsu, and Mitlin, David. Thu .
"Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles". Germany. https://doi.org/10.1002/anie.201906612.
@article{osti_1603182,
title = {Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles},
author = {Liu, Wei and Li, Hongju and Jin, Jialun and Wang, Yizhe and Zhang, Zheng and Chen, Zidong and Wang, Qin and Chen, Yungui and Paek, Eunsu and Mitlin, David},
abstractNote = {Abstract We report a new approach for nanosilicon–graphene hybrids with uniquely stable solid electrolyte interphase. Expanded graphite is gently exfoliated creating “defect‐free” graphene that is non‐catalytic towards electrolyte decomposition, simultaneously introducing high mass loading (48 wt. %) Si nanoparticles. Silane surface treatment creates epoxy chemical tethers, mechanically binding nano‐Si to CMC binder through epoxy ring‐opening reaction while stabilizing the Si surface chemistry. Epoxy‐tethered silicon pristine–graphene hybrid “E‐Si‐pG” exhibits state‐of‐the‐art performance in full battery opposing commercial mass loading (12 mg cm −2 ) LiCoO 2 (LCO) cathode. At 0.4 C, with areal capacity of 1.62 mAh cm −2 and energy of 437 Wh kg −1 , achieving 1.32 mAh cm −2 , 340.4 Wh kg −1 at 1 C. After 150 cycles, it retains 1.25 mAh cm −2 , 306.5 Wh kg −1 . Sputter‐down XPS demonstrates survival of surface C‐Si‐O‐Si groups in E‐Si‐pG after repeated cycling. The discovered synergy between support defects, chemical‐mechanical stabilization of Si surfaces, and SEI‐related failure may become key LIB anode design rule.},
doi = {10.1002/anie.201906612},
journal = {Angewandte Chemie (International Edition)},
number = 46,
volume = 58,
place = {Germany},
year = {Thu Sep 26 00:00:00 EDT 2019},
month = {Thu Sep 26 00:00:00 EDT 2019}
}
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