Smart polymeric cathode material with intrinsic overcharge protection based on a 2,5-di-tert-butyl- 1,4-dimethoxybenzene core structure

Wei Weng, Zhengcheng Zhang, Ali Abouimrane, Paul C. Redfern, Larry A. Curtiss, Khalil Amine

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Polymer-based electroactive materials have been studied and applied in energy storage systems as a valid replacement for transition metal oxides. As early as 1999, Hass et al. proposed an interesting concept on the possible incorporation of both charge storage and overcharge protection functionality into a single material. However, there are virtually no examples of polymeric materials that can not only store the charge, but also consume the overcharge current. Herein, a new material based on a cross-linked polymer (I) with 2,5-di-tert-butyl-1,4-dimethoxybenzene as the core structure is reported. The cyclic voltammogram of the synthesized polymer shows a single oxidation/reduction peak at 3.9-4.0 V. At 1C rate (56 mA/g), polymer I shows stable cycling up to 200 cycles with <10% capacity loss. The redox shuttle mechanism remarkably can be activated when cell voltage is elevated to 4.3 V and the overcharge plateau at 4.2 V (2 nd plateau) is persistent for more than 100 hours. The overcharge protection was due to the release of a chemical redox shuttle species in the electrolyte during the initial charging process. Both DFT calculations and NMR analysis of the aromatic signals in the 1H-NMR spectrum of electrolytes from "overcharged" cells provide evidence for this hypothesis.

Original languageEnglish
Pages (from-to)4485-4492
Number of pages8
JournalAdvanced Functional Materials
Volume22
Issue number21
DOIs
Publication statusPublished - 7 Nov 2012

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Keywords

  • DFT calculation
  • overcharge protection
  • polymer battery
  • polymer cathode
  • redox shuttle

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

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