Structure and dynamics of small polyimide oligomers with silicon as a function of aging

Mary K. Burdette-Trofimov; Beth L. Armstrong; Luke Heroux; Mathieu Doucet; Robert L. Sacci; Gabriel M. Veith

doi:10.1039/d1sm00961c

Structure and dynamics of small polyimide oligomers with silicon as a function of aging

Mary K. Burdette-Trofimov, Beth L. Armstrong, Luke Heroux, Mathieu Doucet, Robert L. Sacci, Gabriel M. Veith

Research output: Contribution to journal › Article › peer-review

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Abstract

The effect of UV curing and shearing on the structure and behavior of a polyimide (PI) binder as it disperses silicon particles in a battery electrode slurry was investigated. PI dispersant effectiveness increases with UV curing time, which controls the overall binder molecular weight. The shear force during electrode casting causes higher molecular weight PI to agglomerate, resulting in battery anodes with poorly dispersed Si particles that do not cycle well. It is hypothesized that when PI binder is added above a critical amount, it conformally coats the silicon particles and greatly impedes Li ion transport. There is an "interzonal region"for binder loading where it disperses silicon well and provides a coverage that facilitates Li transport through the anode material and into the silicon particles. These results have implications in ensuring reproducible electrode manufacturing and increasing cell performance by optimizing the PI structure and coordination with the silicon precursor.

Original language	English
Pages (from-to)	7729-7742
Number of pages	14
Journal	Soft Matter
Volume	17
Issue number	33
DOIs	https://doi.org/10.1039/d1sm00961c
State	Published - Sep 7 2021

Funding

This research (MKBT, BLA, RLS, GMV) was supported by the U.S. Department of Energy’s Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. The authors thank Bill Aronoff and Paul Dodson for their invaluable help in obtaining the GPC results. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory (MD and LH). The ultra-small angle scattering measurements were done using the USANS instrument at the Spallation Neutron Source. This work benefited from the use of the SasView application, originally developed under NSF award DMR-0520547. SasView contains code developed with funding from the European Union’s Horizon 2020 research and innovation programme under the SINE2020 project, grant agreement no. 654000. This manuscript has been authored by UT-Battelle, LLC, under Contract 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 other 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).

Funders	Funder number
National Science Foundation	DMR-0520547
U.S. Department of Energy
Horizon 2020 Framework Programme	DE-AC05-00OR22725, 654000

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Cite this

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abstract = "The effect of UV curing and shearing on the structure and behavior of a polyimide (PI) binder as it disperses silicon particles in a battery electrode slurry was investigated. PI dispersant effectiveness increases with UV curing time, which controls the overall binder molecular weight. The shear force during electrode casting causes higher molecular weight PI to agglomerate, resulting in battery anodes with poorly dispersed Si particles that do not cycle well. It is hypothesized that when PI binder is added above a critical amount, it conformally coats the silicon particles and greatly impedes Li ion transport. There is an {"}interzonal region{"}for binder loading where it disperses silicon well and provides a coverage that facilitates Li transport through the anode material and into the silicon particles. These results have implications in ensuring reproducible electrode manufacturing and increasing cell performance by optimizing the PI structure and coordination with the silicon precursor.",

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AU - Veith, Gabriel M.

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Structure and dynamics of small polyimide oligomers with silicon as a function of aging

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