Conjugated Nitroxide Radical Polymers: Synthesis and Application in Flexible Energy Storage Devices

Yuan Xie, Kai Zhang, Michael J. Monteiro, Zhongfan Jia

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

The synthesis and electrochemical behavior of nitroxide radical conjugated polymers (NCPs) have long been an intriguing topic in redox polymer-based energy storage. However, common (electro)chemical oxidation polymerization methods have proved difficult in the synthesis of well-defined NCPs, and many of these polymers have been difficult to process into thin films. In addition to these drawbacks and coupled with the complex charge-transfer and storage mechanisms, the use of NCPs as electrodes has been significantly limited. The aim of this work is to provide mechanistic insights into this complex charge-transfer and storage process using a new and well-defined NCP synthesized using an ultrafast cyclopolymerization with the Grubbs 3rd generation catalyst. The monomer, consisting of a 1,6-heptadiyne group and a TEMPO (i.e. 2,2,6,6-tetramethylpiperidine-1-oxy) radical, through the cyclopolymerization produced a well-defined NCP with a five-membered ring-containing polyene backbone. This polymer demonstrated excellent film formation properties, allowing the study of their thin-film electrochemical behavior. We found that the electrochemical oxidation of the conjugated backbone and its internal charge transfer to the nitroxide radicals were strongly affected by the applied potential window, current densities, and cycle numbers. Using these new insights, we successfully utilized our NCPs in a flexible energy storage device by fabricating high-performance NCP-coated carbon cloth-based flexible electrodes.

Original languageEnglish
Pages (from-to)7096-7103
Number of pages8
JournalACS Applied Materials and Interfaces
Volume11
Issue number7
DOIs
Publication statusPublished - 28 Jan 2019
Externally publishedYes

Keywords

  • conjugated polymer
  • cyclopolymerization
  • electron transfer
  • energy storage
  • nitroxide radical

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