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

Peng Fei Cao, Michael Naguib, Zhijia Du, Eric Stacy, Bingrui Li, Tao Hong, Kunyue Xing, Dmitry N. Voylov, Jianlin Li, David L. Wood, Alexei P. Sokolov, Jagjit Nanda, Tomonori Saito

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87 Scopus citations

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.

Original languageEnglish
Pages (from-to)3470-3478
Number of pages9
JournalACS Applied Materials and Interfaces
Volume10
Issue number4
DOIs
StatePublished - Jan 31 2018

Funding

This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) (Acting Program Deputy Director: David Howell; Applied Battery Research Program Manager: Peter Faguy). A.P.S. acknowledges partial financial support for the polymer characterization by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.X. acknowledges financial support for the rheology measurement from NSF Polymer program (DMR-1408811). *P.-F. Cao. E-mail: [email protected]. *T. Saito. E-mail: [email protected]. ORCID Peng-Fei Cao: 0000-0003-2391-1838 Michael Naguib: 0000-0002-4952-9023 Jianlin Li: 0000-0002-8710-9847 Jagjit Nanda: 0000-0002-6875-0057 Tomonori Saito: 0000-0002-4536-7530 Notes This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). The authors declare no competing financial interest.

Keywords

  • graft copolymer
  • grafting density
  • polymer binder
  • side chain length
  • silicon/graphite anode

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