skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders

Abstract

Silicon is a promising anode material for lithium-ion batteries with its superior capacity. However, the drastic volume changes during lithiation/delithiation cycles hinder the cycling performance, resulting in particle pulverization, conductivity loss, and an unstable electrode-electrolyte interface. In this work, a series of synthetic polymeric binders, poly(acrylic acid-co-tetra(ethylene glycol) diacrylate)-featuring a poly(acrylic acid) (PAA) backbone branched via tetra(ethylene glycol) diacrylate (TEGDA)-are developed that edge toward evidencing well-balanced properties to confront capacity fading in Si-based electrodes. The incorporation of ether chain not only leads to the branching architecture of the PAA backbone, thus affecting its mechanical properties, but also promotes the conductivity of Li ions. As a result, a synergistic performance improvement is observed in both half and full cells. The best-performing cell using a branched PAA binder (bPAA) with a feeding molar ratio ([TEGDA]:[acrylic acid(AA)]) of 0.2 results in a 10% increase in initial capacity and a 31% increase in capacity retention over 100 cycles compared to the linear PAA cell. The cross-sectional microscopic images of the cycled electrodes reveal that bPAA binders can drastically reduce the electrode expansion. This improvement results from the well-balanced properties of the polymer design, which could guide further development for more advanced binder materials.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [2];  [3]; ORCiD logo [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1632851
Alternate Identifier(s):
OSTI ID: 1580540; OSTI ID: 1756183
Grant/Contract Number:  
AC02-06CH11357; AC02‐06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 10; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; branched PAA; lithium-ion batteries; polymer binder; silicon anode

Citation Formats

Jiang, Sisi, Hu, Bin, Shi, Zhangxing, Chen, Wei, Zhang, Zhengcheng, and Zhang, Lu. Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders. United States: N. p., 2019. Web. https://doi.org/10.1002/adfm.201908558.
Jiang, Sisi, Hu, Bin, Shi, Zhangxing, Chen, Wei, Zhang, Zhengcheng, & Zhang, Lu. Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders. United States. https://doi.org/10.1002/adfm.201908558
Jiang, Sisi, Hu, Bin, Shi, Zhangxing, Chen, Wei, Zhang, Zhengcheng, and Zhang, Lu. Fri . "Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders". United States. https://doi.org/10.1002/adfm.201908558. https://www.osti.gov/servlets/purl/1632851.
@article{osti_1632851,
title = {Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders},
author = {Jiang, Sisi and Hu, Bin and Shi, Zhangxing and Chen, Wei and Zhang, Zhengcheng and Zhang, Lu},
abstractNote = {Silicon is a promising anode material for lithium-ion batteries with its superior capacity. However, the drastic volume changes during lithiation/delithiation cycles hinder the cycling performance, resulting in particle pulverization, conductivity loss, and an unstable electrode-electrolyte interface. In this work, a series of synthetic polymeric binders, poly(acrylic acid-co-tetra(ethylene glycol) diacrylate)-featuring a poly(acrylic acid) (PAA) backbone branched via tetra(ethylene glycol) diacrylate (TEGDA)-are developed that edge toward evidencing well-balanced properties to confront capacity fading in Si-based electrodes. The incorporation of ether chain not only leads to the branching architecture of the PAA backbone, thus affecting its mechanical properties, but also promotes the conductivity of Li ions. As a result, a synergistic performance improvement is observed in both half and full cells. The best-performing cell using a branched PAA binder (bPAA) with a feeding molar ratio ([TEGDA]:[acrylic acid(AA)]) of 0.2 results in a 10% increase in initial capacity and a 31% increase in capacity retention over 100 cycles compared to the linear PAA cell. The cross-sectional microscopic images of the cycled electrodes reveal that bPAA binders can drastically reduce the electrode expansion. This improvement results from the well-balanced properties of the polymer design, which could guide further development for more advanced binder materials.},
doi = {10.1002/adfm.201908558},
journal = {Advanced Functional Materials},
number = 10,
volume = 30,
place = {United States},
year = {2019},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries
journal, July 2017


A Highly Cross-Linked Polymeric Binder for High-Performance Silicon Negative Electrodes in Lithium Ion Batteries
journal, July 2012

  • Koo, Bonjae; Kim, Hyunjung; Cho, Younghyun
  • Angewandte Chemie International Edition, Vol. 51, Issue 35
  • DOI: 10.1002/anie.201201568

A More Versatile Route to Block Copolymers and Other Polymers of Complex Architecture by Living Radical Polymerization:  The RAFT Process
journal, March 1999

  • Chong, ) Y. K.; Le, Tam P. T.; Moad, Graeme
  • Macromolecules, Vol. 32, Issue 6
  • DOI: 10.1021/ma981472p

Using Rheological Data To Determine the Branching Level in Metallocene Polyethylenes
journal, October 2000

  • Wood-Adams, Paula M.; Dealy, John M.
  • Macromolecules, Vol. 33, Issue 20
  • DOI: 10.1021/ma991534r

Ionically Conductive Self-Healing Binder for Low Cost Si Microparticles Anodes in Li-Ion Batteries
journal, February 2018

  • Munaoka, Takatoshi; Yan, Xuzhou; Lopez, Jeffrey
  • Advanced Energy Materials, Vol. 8, Issue 14
  • DOI: 10.1002/aenm.201703138

Characterization of the stereochemical structure of poly(acrylic acid) by one- and two-dimensional 13C-1H nuclear magnetic resonance spectra
journal, January 1995


Reactivity ratios for acrylic acid–methyl acrylate copolymerization in 1,4-dioxane
journal, November 1976

  • Eldridge, R. J.; Treloar, F. E.
  • Journal of Polymer Science: Polymer Chemistry Edition, Vol. 14, Issue 11
  • DOI: 10.1002/pol.1976.170141122

Effect of Molecular Shape on Rheological Properties in Molecular Dynamics Simulation of Star, H, Comb, and Linear Polymer Melts
journal, July 2003

  • Jabbarzadeh, A.; Atkinson, J. D.; Tanner, R. I.
  • Macromolecules, Vol. 36, Issue 13
  • DOI: 10.1021/ma025782q

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

  • Tarascon, J.-M.; Armand, M.
  • Nature, Vol. 414, Issue 6861, p. 359-367
  • DOI: 10.1038/35104644

Silicon-Based Anodes for Lithium-Ion Batteries: From Fundamentals to Practical Applications
journal, January 2018


Copolymerization reactivity ratios acrylic and methacrylic acids with butyl acrylate and butyl methacrylate
journal, February 1963


Enhanced Cycling Stability of Sulfur Electrodes through Effective Binding of Pyridine-Functionalized Polymer
journal, September 2017


Sodium Carboxymethyl Cellulose
journal, January 2007

  • Li, Jing; Lewis, R. B.; Dahn, J. R.
  • Electrochemical and Solid-State Letters, Vol. 10, Issue 2
  • DOI: 10.1149/1.2398725

Surface-Functionalized Silicon Nanoparticles as Anode Material for Lithium-Ion Battery
journal, November 2018

  • Jiang, Sisi; Hu, Bin; Sahore, Ritu
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 51
  • DOI: 10.1021/acsami.8b17729

Stable Li-ion battery anodes by in-situ polymerization of conducting hydrogel to conformally coat silicon nanoparticles
journal, June 2013

  • Wu, Hui; Yu, Guihua; Pan, Lijia
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2941

Rheological behavior of star-shaped polymers
journal, July 1993

  • Fetters, Lewis J.; Kiss, Andrea D.; Pearson, Dale S.
  • Macromolecules, Vol. 26, Issue 4
  • DOI: 10.1021/ma00056a015

Poly(ethylene oxide)-based electrolytes for lithium-ion batteries
journal, January 2015

  • Xue, Zhigang; He, Dan; Xie, Xiaolin
  • Journal of Materials Chemistry A, Vol. 3, Issue 38
  • DOI: 10.1039/C5TA03471J

Phase Behavior of Blends of Poly(ethylene glycol) and Partially Neutralized Poly(acrylic acid)
journal, April 1995


Toward Efficient Binders for Li-Ion Battery Si-Based Anodes: Polyacrylic Acid
journal, October 2010

  • Magasinski, Alexandre; Zdyrko, Bogdan; Kovalenko, Igor
  • ACS Applied Materials & Interfaces, Vol. 2, Issue 11
  • DOI: 10.1021/am100871y

Physically Cross-linked Polymer Binder Induced by Reversible Acid–Base Interaction for High-Performance Silicon Composite Anodes
journal, October 2015

  • Lim, Sanghyun; Chu, Hodong; Lee, Kukjoo
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 42
  • DOI: 10.1021/acsami.5b06682

The Effects of Cross-Linking in a Supramolecular Binder on Cycle Life in Silicon Microparticle Anodes
journal, January 2016

  • Lopez, Jeffrey; Chen, Zheng; Wang, Chao
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 3
  • DOI: 10.1021/acsami.5b11363

Designing nanostructured Si anodes for high energy lithium ion batteries
journal, October 2012


Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Promises and challenges of nanomaterials for lithium-based rechargeable batteries
journal, June 2016


A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries
journal, September 2011


Hollow Carbon Nanospheres with Superior Rate Capability for Sodium-Based Batteries
journal, May 2012

  • Tang, Kun; Fu, Lijun; White, Robin J.
  • Advanced Energy Materials, Vol. 2, Issue 7
  • DOI: 10.1002/aenm.201100691

Enhancement of the Cyclability of a Si/Graphite@Graphene composite as anode for Lithium-ion batteries
journal, January 2014


Small things make a big difference: binder effects on the performance of Li and Na batteries
journal, January 2014

  • Chou, Shu-Lei; Pan, Yuede; Wang, Jia-Zhao
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 38
  • DOI: 10.1039/C4CP02475C

Living Free-Radical Polymerization by Reversible Addition−Fragmentation Chain Transfer:  The RAFT Process
journal, August 1998

  • Chiefari, John; Chong, Y. K. (Bill); Ercole, Frances
  • Macromolecules, Vol. 31, Issue 16
  • DOI: 10.1021/ma9804951

Li-alloy based anode materials for Li secondary batteries
journal, January 2010

  • Park, Cheol-Min; Kim, Jae-Hun; Kim, Hansu
  • Chemical Society Reviews, Vol. 39, Issue 8, p. 3115-3141
  • DOI: 10.1039/b919877f

Correlation between glass transition temperature and chain structure for randomly crosslinked high polymers
journal, September 1996


High performance polymer binders inspired by chemical finishing of textiles for silicon anodes in lithium ion batteries
journal, January 2017

  • Wei, Liangming; Hou, Zhongyu
  • J. Mater. Chem. A, Vol. 5, Issue 42
  • DOI: 10.1039/C7TA05195F

Confronting Issues of the Practical Implementation of Si Anode in High-Energy Lithium-Ion Batteries
journal, September 2017


Size-exclusion chromatography (SEC) of branched polymers and polysaccharides
journal, October 2010

  • Gaborieau, Marianne; Castignolles, Patrice
  • Analytical and Bioanalytical Chemistry, Vol. 399, Issue 4
  • DOI: 10.1007/s00216-010-4221-7

Influence of cross-link density on rheological properties of temperature-sensitive microgel suspensions
journal, September 2000


Living Radical Polymerization by the RAFT Process
journal, January 2005

  • Moad, Graeme; Rizzardo, Ezio; Thang, San H.
  • Australian Journal of Chemistry, Vol. 58, Issue 6
  • DOI: 10.1071/CH05072

Electrochemical performance and interfacial investigation on Si composite anode for lithium ion batteries in full cell
journal, August 2017


Water Soluble Binder, an Electrochemical Performance Booster for Electrode Materials with High Energy Density
journal, July 2017

  • Li, Jun-Tao; Wu, Zhan-Yu; Lu, Yan-Qiu
  • Advanced Energy Materials, Vol. 7, Issue 24
  • DOI: 10.1002/aenm.201701185

Electron/Ion Transport Enhancer in High Capacity Li-Ion Battery Anodes
journal, September 2016