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Title: Evidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries

Silicon has the potential to revolutionize the energy storage capacities of lithium-ion batteries to meet the ever increasing power demands of next generation technologies. To avoid the operational stability problems of silicon-based anodes, we propose synergistic physicochemical alteration of electrode structures during their design. This capitalizes on covalent interaction of Si nanoparticles with sulfur-doped graphene and with cyclized polyacrylonitrile to provide a robust nanoarchitecture. This hierarchical structure stabilized the solid electrolyte interphase leading to superior reversible capacity of over 1,000 mAh g -1 for 2,275 cycles at 2 A g -1. Furthermore, the nanoarchitectured design lowered the contact of the electrolyte to the electrode leading to not only high coulombic efficiency of 99.9% but also maintaining high stability even with high electrode loading associated with 3.4 mAh cm -2. As a result, the excellent performance combined with the simplistic, scalable and non-hazardous approach render the process as a very promising candidate for Li-ion battery technology.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [2] ;  [1] ;  [1]
  1. Univ. of Waterloo, Waterloo, ON (Canada)
  2. General Motors Global Research and Development Center, Warren, MI (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
General Motors Global Research and Development Center, Warren, MI (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; chemical sciences; materials science; nanotechnology
OSTI Identifier:
1239317

Hassan, Fathy M., Batmaz, Rasim, Li, Jingde, Wang, Xiaolei, Xiao, Xingcheng, Yu, Aiping, and Chen, Zhongwei. Evidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries. United States: N. p., Web. doi:10.1038/ncomms9597.
Hassan, Fathy M., Batmaz, Rasim, Li, Jingde, Wang, Xiaolei, Xiao, Xingcheng, Yu, Aiping, & Chen, Zhongwei. Evidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries. United States. doi:10.1038/ncomms9597.
Hassan, Fathy M., Batmaz, Rasim, Li, Jingde, Wang, Xiaolei, Xiao, Xingcheng, Yu, Aiping, and Chen, Zhongwei. 2015. "Evidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries". United States. doi:10.1038/ncomms9597. https://www.osti.gov/servlets/purl/1239317.
@article{osti_1239317,
title = {Evidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries},
author = {Hassan, Fathy M. and Batmaz, Rasim and Li, Jingde and Wang, Xiaolei and Xiao, Xingcheng and Yu, Aiping and Chen, Zhongwei},
abstractNote = {Silicon has the potential to revolutionize the energy storage capacities of lithium-ion batteries to meet the ever increasing power demands of next generation technologies. To avoid the operational stability problems of silicon-based anodes, we propose synergistic physicochemical alteration of electrode structures during their design. This capitalizes on covalent interaction of Si nanoparticles with sulfur-doped graphene and with cyclized polyacrylonitrile to provide a robust nanoarchitecture. This hierarchical structure stabilized the solid electrolyte interphase leading to superior reversible capacity of over 1,000 mAh g-1 for 2,275 cycles at 2 A g-1. Furthermore, the nanoarchitectured design lowered the contact of the electrolyte to the electrode leading to not only high coulombic efficiency of 99.9% but also maintaining high stability even with high electrode loading associated with 3.4 mAh cm-2. As a result, the excellent performance combined with the simplistic, scalable and non-hazardous approach render the process as a very promising candidate for Li-ion battery technology.},
doi = {10.1038/ncomms9597},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {2015},
month = {10}
}