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

Title: Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries

Abstract

Although significant progress has been made in improving cycling performance of silicon-based electrodes, few studies have been performed on the architecture effect on polymer binder performance for lithium-ion batteries. A systematic study on the relationship between polymer architectures and binder performance is especially useful in designing synthetic polymer binders. Herein, a graft block copolymer with readily tunable architecture parameters is synthesized and tested as the polymer binder for the high-mass loading silicon (15 wt %)/graphite (73 wt %) composite electrode (active materials >2.5 mg/cm2). With the same chemical composition and functional group ratio, the graft block copolymer reveals improved cycling performance in both capacity retention (495 mAh/g vs 356 mAh/g at 100th cycle) and Coulombic efficiency (90.3% vs 88.1% at first cycle) than the physical mixing of glycol chitosan (GC) and lithium polyacrylate (LiPAA). Galvanostatic results also demonstrate the significant impacts of different architecture parameters of graft copolymers, including grafting density and side chain length, on their ultimate binder performance. By simply changing the side chain length of GC-g-LiPAA, the retaining delithiation capacity after 100 cycles varies from 347 mAh/g to 495 mAh/g.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [1];  [5];  [5];  [5]; ORCiD logo [3];  [3];  [6]; ORCiD logo [7]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Tulane Univ., New Orleans, LA (United States). Dept. of Physics and Engineering Physics; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy & Transportation Science Division
  4. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
  5. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
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), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1435230
Alternate Identifier(s):
OSTI ID: 1436937; OSTI ID: 1468273
Grant/Contract Number:  
AC05-00OR22725; DMR-1408811
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 4; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; graft copolymer; grafting density; polymer binder; side chain length; silicon/graphite anode

Citation Formats

Cao, Peng-Fei, Naguib, Michael, Du, Zhijia, Stacy, Eric, Li, Bingrui, Hong, Tao, Xing, Kunyue, Voylov, Dmitry N., Li, Jianlin, Wood, David L., Sokolov, Alexei P., Nanda, Jagjit, and Saito, Tomonori. Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries. United States: N. p., 2018. Web. doi:10.1021/acsami.7b13205.
Cao, Peng-Fei, Naguib, Michael, Du, Zhijia, Stacy, Eric, Li, Bingrui, Hong, Tao, Xing, Kunyue, Voylov, Dmitry N., Li, Jianlin, Wood, David L., Sokolov, Alexei P., Nanda, Jagjit, & Saito, Tomonori. Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries. United States. https://doi.org/10.1021/acsami.7b13205
Cao, Peng-Fei, Naguib, Michael, Du, Zhijia, Stacy, Eric, Li, Bingrui, Hong, Tao, Xing, Kunyue, Voylov, Dmitry N., Li, Jianlin, Wood, David L., Sokolov, Alexei P., Nanda, Jagjit, and Saito, Tomonori. 2018. "Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries". United States. https://doi.org/10.1021/acsami.7b13205. https://www.osti.gov/servlets/purl/1435230.
@article{osti_1435230,
title = {Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries},
author = {Cao, Peng-Fei and Naguib, Michael and Du, Zhijia and Stacy, Eric and Li, Bingrui and Hong, Tao and Xing, Kunyue and Voylov, Dmitry N. and Li, Jianlin and Wood, David L. and Sokolov, Alexei P. and Nanda, Jagjit and Saito, Tomonori},
abstractNote = {Although significant progress has been made in improving cycling performance of silicon-based electrodes, few studies have been performed on the architecture effect on polymer binder performance for lithium-ion batteries. A systematic study on the relationship between polymer architectures and binder performance is especially useful in designing synthetic polymer binders. Herein, a graft block copolymer with readily tunable architecture parameters is synthesized and tested as the polymer binder for the high-mass loading silicon (15 wt %)/graphite (73 wt %) composite electrode (active materials >2.5 mg/cm2). With the same chemical composition and functional group ratio, the graft block copolymer reveals improved cycling performance in both capacity retention (495 mAh/g vs 356 mAh/g at 100th cycle) and Coulombic efficiency (90.3% vs 88.1% at first cycle) than the physical mixing of glycol chitosan (GC) and lithium polyacrylate (LiPAA). Galvanostatic results also demonstrate the significant impacts of different architecture parameters of graft copolymers, including grafting density and side chain length, on their ultimate binder performance. By simply changing the side chain length of GC-g-LiPAA, the retaining delithiation capacity after 100 cycles varies from 347 mAh/g to 495 mAh/g.},
doi = {10.1021/acsami.7b13205},
url = {https://www.osti.gov/biblio/1435230}, journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 4,
volume = 10,
place = {United States},
year = {Thu Jan 04 00:00:00 EST 2018},
month = {Thu Jan 04 00:00:00 EST 2018}
}

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

Citation Metrics:
Cited by: 66 works
Citation information provided by
Web of Science

Figures / Tables:

Scheme 1. Scheme 1.: Synthesis of graft copolymer GC-g-LiPAA via RAFT polymerization

Save / Share:

Works referenced in this record:

Combs and Bottlebrushes in a Melt
journal, April 2017


An In Situ X-Ray Diffraction Study of the Reaction of Li with Crystalline Si
journal, January 2007


Sodium Carboxymethyl Cellulose
journal, January 2007


Solvent-free, supersoft and superelastic bottlebrush melts and networks
journal, November 2015


In-situ observation of volume expansion behavior of a silicon particle in various electrolytes
journal, January 2016


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


Mussel-inspired Polydopamine-treated Copper Foil as a Current Collector for High-performance Silicon Anodes
journal, August 2016


All-Aqueous Directed Assembly Strategy for Forming High-Capacity, Stable Silicon/Carbon Anodes for Lithium-Ion Batteries
journal, September 2015


Chitosan-Based Nanocarriers with pH and Light Dual Response for Anticancer Drug Delivery
journal, July 2013


Dendrimers and hyperbranched polymers
journal, January 2015


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


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


Electrochemically anodized porous silicon: Towards simple and affordable anode material for Li-ion batteries
journal, August 2017


Rechargeable Lithium–Sulfur Batteries
journal, July 2014


Cross-Linked Chitosan as an Efficient Binder for Si Anode of Li-ion Batteries
journal, January 2016


Optimization of multicomponent aqueous suspensions of lithium iron phosphate (LiFePO4) nanoparticles and carbon black for lithium-ion battery cathodes
journal, September 2013


High Areal Capacity Si/LiCoO 2 Batteries from Electrospun Composite Fiber Mats
journal, March 2017


High-Performance Lithium Metal Negative Electrode with a Soft and Flowable Polymer Coating
journal, November 2016


A Robust Ion-Conductive Biopolymer as a Binder for Si Anodes of Lithium-Ion Batteries
journal, May 2015


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


Interpenetrated Gel Polymer Binder for High-Performance Silicon Anodes in Lithium-ion Batteries
journal, July 2014


Comb Copolymer Brush with Chemically Different Side Chains
journal, June 2002


Design of Graft Block Polymer Thermoplastics
journal, November 2016


High Energy Density Calendered Si Alloy/Graphite Anodes
journal, January 2014


Poly(phenanthrenequinone) as a conductive binder for nano-sized silicon negative electrodes
journal, January 2015


Lithium polyacrylate as a binder for tin–cobalt–carbon negative electrodes in lithium-ion batteries
journal, March 2010


Side-Chain Conducting and Phase-Separated Polymeric Binders for High-Performance Silicon Anodes in Lithium-Ion Batteries
journal, February 2015


High-Capacity Retention of Si Anodes Using a Mixed Lithium/Phosphonium Bis(fluorosulfonyl)imide Ionic Liquid Electrolyte
journal, July 2017


A high-performance alginate hydrogel binder for the Si/C anode of a Li-ion battery
journal, January 2014


Towards Improving the Practical Energy Density of Li-Ion Batteries: Optimization and Evaluation of Silicon:Graphite Composites in Full Cells
journal, December 2016


Lithium Polyacrylate (LiPAA) as an Advanced Binder and a Passivating Agent for High-Voltage Li-Ion Batteries
journal, September 2015


Effect of Side Chain Rigidity on the Elasticity of Comb Copolymer Cylindrical Brushes:  A Monte Carlo Simulation Study
journal, June 1999


In Situ and Operando Investigations of Failure Mechanisms of the Solid Electrolyte Interphase on Silicon Electrodes
journal, September 2016


Catenated Poly(ε-caprolactone) and Poly( l -lactide) via Ring-Expansion Strategy
journal, June 2015


Frustrated crystallisation and hierarchical self-assembly behaviour of comb-like polymers
journal, January 2013


Building better batteries
journal, February 2008


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


Multifunctional Molecular Design as an Efficient Polymeric Binder for Silicon Anodes in Lithium-Ion Batteries
journal, October 2014


What is the Young's Modulus of Silicon?
journal, April 2010


Alloy Negative Electrodes for Li-Ion Batteries
journal, October 2014


50th Anniversary Perspective : Polymers with Complex Architectures
journal, February 2017


Mussel-Inspired Adhesive Binders for High-Performance Silicon Nanoparticle Anodes in Lithium-Ion Batteries
journal, December 2012


Soft Poly(dimethylsiloxane) Elastomers from Architecture-Driven Entanglement Free Design
journal, August 2015


Electrical energy storage for transportation—approaching the limits of, and going beyond, lithium-ion batteries
journal, January 2012


Strategies to succeed in improving the lithium-ion storage properties of silicon nanomaterials
journal, January 2016


ABA Triblock Brush Polymers: Synthesis, Self-Assembly, Conductivity, and Rheological Properties
journal, July 2015


Computer Simulations of Bottle Brushes: From Melts to Soft Networks
journal, July 2015


Elastic Modulus of Amorphous Polymer Thin Films: Relationship to the Glass Transition Temperature
journal, August 2009


A Trefoil Knotted Polymer Produced through Ring Expansion
journal, February 2015


Works referencing / citing this record:

Sustainable Battery Materials from Biomass
journal, April 2020


Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries
journal, January 2019


Facile Fabrication of Porous Si Microspheres from Low‐Cost Precursors for High‐Capacity Electrode
journal, December 2019


Compact Si/C anodes fabricated by simultaneously regulating the size and oxidation degree of Si for Li-ion batteries
journal, January 2019


Si nanoflake-assembled blocks towards high initial coulombic efficiency anodes for lithium-ion batteries
journal, January 2018


Continuous Flow Fabrication of Block Copolymer–Grafted Silica Micro‐Particles in Environmentally Friendly Water/Ethanol Media
journal, October 2018


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.