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Title: Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling

Abstract

Mechanical degradation caused by lithiation/delithiation-induced stress and large volume change is the primary cause of fast capacity fading of silicon (Si)-based electrodes. Although intensive efforts have been devoted to understanding electromechanically induced fractures of electrodes made of Si alone (e.g., Si particles, Si thin films, and Si wafers), the cracking behavior of Si/polymeric binders/carbon black composite electrodes is unclear and poorly understood. Here, we investigate, by in situ and ex situ techniques, the cracking behavior of Si composite electrodes made with different binders, including polyvinylidene fluoride (PVDF), sodium-alginate (SA), sodium-carboxymethyl cellulose (Na-CMC), and Nafion. We found that extensive cracks form during the 1st delithiation process, which periodically open and close during subsequent lithiation/delithiation cycles at the same locations in the Si composite electrodes made with SA, Na-CMC, and Nafion. In contrast, a significantly fewer number of cracks form in the Si/PVDF electrodes after electrochemical cycling. A possible mechanism is proposed to help understand the effects of binders on the cracking behavior (e.g., crack spacing and island size) of Si composite electrodes. We also suggest possible approaches, including reducing the electrode thickness, patterning electrodes, and using highly recoverable binders, to inhibit cracks and improve the mechanical integrity of Si composite electrodes.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [1]; ORCiD logo [1];  [1]
  1. Univ. of Kentucky, Lexington, KY (United States)
  2. Univ. of Kentucky, Lexington, KY (United States); Shanghai University (China)
Publication Date:
Research Org.:
General Motors LLC, Detroit, MI (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1799373
Alternate Identifier(s):
OSTI ID: 2325527
Grant/Contract Number:  
EE0007787
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 438; Journal Issue: C; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Chemistry; Electrochemistry; Energy & Fuels; Materials Science; Silicon electrode; Cracking; Polymeric binder; In situ observation; Adhesion; Lithium ion battery

Citation Formats

Wang, Yikai, Dang, Dingying, Li, Dawei, Hu, Jiazhi, Zhan, Xiaowen, and Cheng, Yang-Tse. Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling. United States: N. p., 2019. Web. doi:10.1016/j.jpowsour.2019.226938.
Wang, Yikai, Dang, Dingying, Li, Dawei, Hu, Jiazhi, Zhan, Xiaowen, & Cheng, Yang-Tse. Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling. United States. https://doi.org/10.1016/j.jpowsour.2019.226938
Wang, Yikai, Dang, Dingying, Li, Dawei, Hu, Jiazhi, Zhan, Xiaowen, and Cheng, Yang-Tse. Wed . "Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling". United States. https://doi.org/10.1016/j.jpowsour.2019.226938. https://www.osti.gov/servlets/purl/1799373.
@article{osti_1799373,
title = {Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling},
author = {Wang, Yikai and Dang, Dingying and Li, Dawei and Hu, Jiazhi and Zhan, Xiaowen and Cheng, Yang-Tse},
abstractNote = {Mechanical degradation caused by lithiation/delithiation-induced stress and large volume change is the primary cause of fast capacity fading of silicon (Si)-based electrodes. Although intensive efforts have been devoted to understanding electromechanically induced fractures of electrodes made of Si alone (e.g., Si particles, Si thin films, and Si wafers), the cracking behavior of Si/polymeric binders/carbon black composite electrodes is unclear and poorly understood. Here, we investigate, by in situ and ex situ techniques, the cracking behavior of Si composite electrodes made with different binders, including polyvinylidene fluoride (PVDF), sodium-alginate (SA), sodium-carboxymethyl cellulose (Na-CMC), and Nafion. We found that extensive cracks form during the 1st delithiation process, which periodically open and close during subsequent lithiation/delithiation cycles at the same locations in the Si composite electrodes made with SA, Na-CMC, and Nafion. In contrast, a significantly fewer number of cracks form in the Si/PVDF electrodes after electrochemical cycling. A possible mechanism is proposed to help understand the effects of binders on the cracking behavior (e.g., crack spacing and island size) of Si composite electrodes. We also suggest possible approaches, including reducing the electrode thickness, patterning electrodes, and using highly recoverable binders, to inhibit cracks and improve the mechanical integrity of Si composite electrodes.},
doi = {10.1016/j.jpowsour.2019.226938},
journal = {Journal of Power Sources},
number = C,
volume = 438,
place = {United States},
year = {Wed Jul 31 00:00:00 EDT 2019},
month = {Wed Jul 31 00:00:00 EDT 2019}
}

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