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

Journal Article · · ACS Energy Letters
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

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.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1511916
Journal Information:
ACS Energy Letters, Vol. 4, Issue 5; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 88 works
Citation information provided by
Web of Science

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Cited By (4)

Room‐Temperature Crosslinkable Natural Polymer Binder for High‐Rate and Stable Silicon Anodes journal December 2019
Biomaterials for High‐Energy Lithium‐Based Batteries: Strategies, Challenges, and Perspectives journal September 2019
Facile Fabrication of Porous Si Microspheres from Low‐Cost Precursors for High‐Capacity Electrode journal December 2019
Polymer Binders Constructed through Dynamic Noncovalent Bonds for High‐Capacity Silicon‐Based Anodes journal September 2009

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