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Title: Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries

Abstract

Silicon is a high-energy density anode material for lithium-ion batteries, but it possesses shortcomings such as poor electronic conductivity, interfacial instability and mechanical fracturing that hinder its battery cycling. Carbon coating has been an important strategy for stabilizing silicon anodes, but the effects of the silicon surface properties on carbon coating morphology and the consequent silicon cycling stability have not been clearly elucidated. Herein, we find that thermal oxidation of the silicon anodes followed by chemical vapor deposition of carbonaceous precursors leads to a well-ordered graphene coating, whereas disordered graphite coating is formed on the native silicon surface. Graphene-coated silicon exhibits superior cycling performance, retaining a discharge capacity of ~1300 mAh g-1 after 300 cycles, whereas the disordered graphite-coated silicon suffers continuous degradation, retaining only~600 mAh g-1 after 300 cycles. Cryogenic electron microscopy reveals the mechanism behind the difference in cycling stabilities; graphene coated silicon is able to withstand the large mechanical strains induced during extended cycling, whereas disordered graphite coating is ruptured, exposing silicon surfaces to the electrolyte, leading to extensive buildup of SEI and poor cycling performance. Characterization of the silicon surface reveals that thermal treatment yields an oxygen-rich surface layer, which is hypothesized to play a decisivemore » role in dictating the carbon coating. This work highlights the effect of silicon surface properties on carbon coating microstructure, and presents thermal treatment as a facile avenue to attain graphene coating on silicon anodes.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [1];  [1];  [1];  [3]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); Samsung SDI (Korea, Republic of)
  3. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1867424
Grant/Contract Number:  
AC02-76SF00515; ECCS-2026822
Resource Type:
Accepted Manuscript
Journal Name:
MRS Bulletin
Additional Journal Information:
Journal Volume: 47; Journal Issue: 2; Journal ID: ISSN 0883-7694
Publisher:
Materials Research Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Kim, Sang Cheol, Huang, William, Zhang, Zewen, Wang, Jiangyan, Kim, Yongseok, Jeong, You Kyeong, Oyakhire, Solomon T., Yang, Yufei, and Cui, Yi. Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries. United States: N. p., 2022. Web. doi:10.1557/s43577-021-00191-4.
Kim, Sang Cheol, Huang, William, Zhang, Zewen, Wang, Jiangyan, Kim, Yongseok, Jeong, You Kyeong, Oyakhire, Solomon T., Yang, Yufei, & Cui, Yi. Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries. United States. https://doi.org/10.1557/s43577-021-00191-4
Kim, Sang Cheol, Huang, William, Zhang, Zewen, Wang, Jiangyan, Kim, Yongseok, Jeong, You Kyeong, Oyakhire, Solomon T., Yang, Yufei, and Cui, Yi. Fri . "Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries". United States. https://doi.org/10.1557/s43577-021-00191-4. https://www.osti.gov/servlets/purl/1867424.
@article{osti_1867424,
title = {Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries},
author = {Kim, Sang Cheol and Huang, William and Zhang, Zewen and Wang, Jiangyan and Kim, Yongseok and Jeong, You Kyeong and Oyakhire, Solomon T. and Yang, Yufei and Cui, Yi},
abstractNote = {Silicon is a high-energy density anode material for lithium-ion batteries, but it possesses shortcomings such as poor electronic conductivity, interfacial instability and mechanical fracturing that hinder its battery cycling. Carbon coating has been an important strategy for stabilizing silicon anodes, but the effects of the silicon surface properties on carbon coating morphology and the consequent silicon cycling stability have not been clearly elucidated. Herein, we find that thermal oxidation of the silicon anodes followed by chemical vapor deposition of carbonaceous precursors leads to a well-ordered graphene coating, whereas disordered graphite coating is formed on the native silicon surface. Graphene-coated silicon exhibits superior cycling performance, retaining a discharge capacity of ~1300 mAh g-1 after 300 cycles, whereas the disordered graphite-coated silicon suffers continuous degradation, retaining only~600 mAh g-1 after 300 cycles. Cryogenic electron microscopy reveals the mechanism behind the difference in cycling stabilities; graphene coated silicon is able to withstand the large mechanical strains induced during extended cycling, whereas disordered graphite coating is ruptured, exposing silicon surfaces to the electrolyte, leading to extensive buildup of SEI and poor cycling performance. Characterization of the silicon surface reveals that thermal treatment yields an oxygen-rich surface layer, which is hypothesized to play a decisive role in dictating the carbon coating. This work highlights the effect of silicon surface properties on carbon coating microstructure, and presents thermal treatment as a facile avenue to attain graphene coating on silicon anodes.},
doi = {10.1557/s43577-021-00191-4},
journal = {MRS Bulletin},
number = 2,
volume = 47,
place = {United States},
year = {Fri Feb 25 00:00:00 EST 2022},
month = {Fri Feb 25 00:00:00 EST 2022}
}

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