Helical Covalent Polymers with Unidirectional Ion Channels as Single Lithium-Ion Conducting Electrolytes

Yiming Hu, Nathan Dunlap, Hai Long, Hongxuan Chen, Lacey Wayment, Michael Ortiz, Yinghua Jin, Abdulrahiman Nijamudheen, Jose Mendoza-Cortes, Se-hee Lee, Wei Zhang

Research output: Contribution to journalArticlepeer-review

20 Scopus Citations

Abstract

Single-ion conducting polymer electrolytes have attracted great attention as safe alternatives to liquid electrolytes in high energy density lithium-ion batteries. Herein, we report the first example of a crystalline anionic helical polymer as a single lithium-ion conducting solid polymer electrolyte (SPE). Single-crystal X-ray analysis shows that the polymer folds into densely packed double helices, with bundles of unidirectional negatively charged channels formed that can facilitate lithium-ion transportation. Such a helical covalent polymer (HCP) exhibits excellent room temperature lithium-ion conductivity (1.2 × 10−3 S·cm−1) in the absence of external lithium salts, a high transference number (0.84), low activation energy (0.14 eV), and a wide electrochemical stability window (0.2–5 V). We found that nonflammable, nonvolatile ionic liquid can serve as a solvating medium and excellent conductivity enhancer (>1000 times increase). These ion-conducting properties are comparable to the best polyethylene oxide-based polymer electrolytes mixed with lithium salts. Finally, we show that the solvated HCP SPE enables the reversible cycling of an all-solid-state cell prepared with a high-voltage NMC 811 cathode. Our study opens up new possibilities for developing next-generation high-performance solid-state electrolytes.

Original languageAmerican English
Pages (from-to)2762-2770
Number of pages9
JournalCCS Chemistry
Volume3
Issue number12
DOIs
StatePublished - 1 Dec 2021

Bibliographical note

Publisher Copyright:
© 2021 Chinese Chemical Society. All right reserved.

NREL Publication Number

  • NREL/JA-2C00-81916

Keywords

  • Helical covalent polymer
  • Single-ion conducting electrolyte
  • Spiroborate

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