Conjugated Imine Polymer Synthesized via Step-Growth Metathesis for Highly Stable Silicon Nanoparticle Anodes in Lithium-Ion Batteries: Article No. 2203921

Trevor Martin, Leah Rynearson, Mackenzie Kuller, Joseph Quinn, Chongmin Wang, Brett Lucht, Nathan Neale

Research output: Contribution to journalArticlepeer-review

5 Scopus Citations

Abstract

This work reports a new method to synthesize polyphenylmethanimine (polyPMI) as a linear or a hyperbranched, conjugated polymer using an aldehyde-imine metathesis reaction. This work details the reaction mechanisms of this polymerization by characterizing a red-shift in its absorption spectrum as polymer conjugation length increases and verifies that this optical shift results from extended p-condensation using density functional theory. This new synthetic approach provides a polymer that can potentially be depolymerized for facile recyclability and is compatible with air- and water-sensitive chemistries. As an example of the utility of this new approach, this work demonstrates that this polymer can be directly grown on silicon nanoparticles to create silicon anodes for lithium-ion batteries with a high degree of electrochemical interfacial passivation. These silicon anodes exhibit Coulombic efficiencies above 99.9% and can accommodate silicon nanoparticle expansion and contraction during lithiation and delithiation as demonstrated by stable reversible capacities for 500 cycles. Finally, this work demonstrates that polyPMI facilitates the formation of a lithium fluoride rich solid electrolyte interphase that remains chemically and mechanically stable after long term cycling.
Original languageAmerican English
Number of pages12
JournalAdvanced Energy Materials
Volume13
Issue number13
DOIs
StatePublished - 2023

Bibliographical note

See NREL/JA-5900-84264 for ChemRxiv preprint

NREL Publication Number

  • NREL/JA-5900-85615

Keywords

  • conjugated polymers
  • lithium-ion batteries
  • nanoparticles
  • silicon anodes

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