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Title: Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes

Abstract

Although several principles have been recognized to fabricate a nominal “better” binder, there continues to be a lack of a rational design and synthesis approach that would meet the robust criteria required for silicon (Si) anodes. Herein, we report a synthetic polymer binder, i.e., catechol-functionalized chitosan cross-linked by glutaraldehyde (CS-CG+GA), that serves dual functionalities: (a) wetness-resistant adhesion capability via catechol grafting and (b) mechanical robustness via in situ formation of a three-dimensional (3D) network. A SiNP-based anode with a designed functional polymer network (CS-CG10%+6%GA) exhibits a capacity retention of 91.5% after 100 cycles (2144 ± 14 mAh/g). Properties that are traditionally considered to be advantageous, including stronger adhesion strength and higher mechanical robustness, do not always improve the binder performance. A clear relationship between these properties and ultimate electrochemical performance is established by assessing the rheological behavior, mechanical property, adhesion force, peel stress, morphology evolution, and semiquantitative evaluation. This study provides a clear path for the rational design of high-performance functional polymer binders for not only Si-based electrodes but also other types of alloy and conversion-based electrodes.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [3]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Georgia Inst. of Technology, Atlanta, GA (United States). School of Material Science and Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1511916
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Cao, Pengfei, Yang, Guang, Li, Bingrui, Zhang, Yiman, Zhao, Sheng, Zhang, Shuo, Erwin, Andrew J., Zhang, Zhengcheng, Sokolov, Alexei P., Nanda, Jagjit, and Saito, Tomonori. Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.9b00815.
Cao, Pengfei, Yang, Guang, Li, Bingrui, Zhang, Yiman, Zhao, Sheng, Zhang, Shuo, Erwin, Andrew J., Zhang, Zhengcheng, Sokolov, Alexei P., Nanda, Jagjit, & Saito, Tomonori. Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes. United States. doi:10.1021/acsenergylett.9b00815.
Cao, Pengfei, Yang, Guang, Li, Bingrui, Zhang, Yiman, Zhao, Sheng, Zhang, Shuo, Erwin, Andrew J., Zhang, Zhengcheng, Sokolov, Alexei P., Nanda, Jagjit, and Saito, Tomonori. Mon . "Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes". United States. doi:10.1021/acsenergylett.9b00815.
@article{osti_1511916,
title = {Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes},
author = {Cao, Pengfei and Yang, Guang and Li, Bingrui and Zhang, Yiman and Zhao, Sheng and Zhang, Shuo and Erwin, Andrew J. and Zhang, Zhengcheng and Sokolov, Alexei P. and Nanda, Jagjit and Saito, Tomonori},
abstractNote = {Although several principles have been recognized to fabricate a nominal “better” binder, there continues to be a lack of a rational design and synthesis approach that would meet the robust criteria required for silicon (Si) anodes. Herein, we report a synthetic polymer binder, i.e., catechol-functionalized chitosan cross-linked by glutaraldehyde (CS-CG+GA), that serves dual functionalities: (a) wetness-resistant adhesion capability via catechol grafting and (b) mechanical robustness via in situ formation of a three-dimensional (3D) network. A SiNP-based anode with a designed functional polymer network (CS-CG10%+6%GA) exhibits a capacity retention of 91.5% after 100 cycles (2144 ± 14 mAh/g). Properties that are traditionally considered to be advantageous, including stronger adhesion strength and higher mechanical robustness, do not always improve the binder performance. A clear relationship between these properties and ultimate electrochemical performance is established by assessing the rheological behavior, mechanical property, adhesion force, peel stress, morphology evolution, and semiquantitative evaluation. This study provides a clear path for the rational design of high-performance functional polymer binders for not only Si-based electrodes but also other types of alloy and conversion-based electrodes.},
doi = {10.1021/acsenergylett.9b00815},
journal = {ACS Energy Letters},
number = 5,
volume = 4,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
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This content will become publicly available on April 22, 2020
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