Single-Ion Conducting Polymer Electrolytes for Solid-State Lithium–Metal Batteries: Design, Performance, and Challenges

Jiadeng Zhu, Zhen Zhang, Sheng Zhao, Andrew S. Westover, Ilias Belharouak, Peng Fei Cao

Research output: Contribution to journalReview articlepeer-review

245 Scopus citations

Abstract

Realizing solid-state lithium batteries with higher energy density and enhanced safety compared to the conventional liquid lithium-ion batteries is one of the primary research and development goals set for next-generation batteries in this decade. In this regard, polymer electrolytes have been widely researched as solid electrolytes due to their excellent processability, flexibility, and low weight. With high cationic transference numbers (tLi+ close to 1), single-ion conducting polymer electrolytes (SICPEs) have tremendous advantages compared to polymer electrolyte systems (tLi+ < 0.4) because of their potential to reduce the buildup of ion concentration gradients and suppress growth of lithium dendrites. The current review covers the fundamentals of SICPEs, including anionic unit synthesis, polymer structure design, and film fabrication, along with simulation and experimental results in solid-state lithium–metal battery applications. A perspective on current challenges, possible solutions, and potential research directions of SICPEs is also discussed to provide the research community with the critical technical aspects that may advance SICPEs as solid electrolytes in next-generation energy storage systems.

Original languageEnglish
Article number2003836
JournalAdvanced Energy Materials
Volume11
Issue number14
DOIs
StatePublished - Apr 15 2021

Funding

This research at the Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE‐AC05‐00OR22725, was sponsored by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory. P.‐F.C. also acknowledges partial financial support by the US Department of Energy, Office of Science, Basic Energy Science, Material Science, and Engineering Division. This paper was authored by UT‐Battelle, LLC under Contract No. DE‐AC05‐00OR22725 with the U.S. Department of Energy. This article has been contributed to by US Government contractors and their work is in the public domain in the USA. The Department of Energy provided 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 ). This research at the Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC05-00OR22725, was sponsored by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory. P.-F.C. also acknowledges partial financial support by the US Department of Energy, Office of Science, Basic Energy Science, Material Science, and Engineering Division. This paper was authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. This article has been contributed to by US Government contractors and their work is in the public domain in the USA. The Department of Energy provided 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).

FundersFunder number
Basic Energy Science, Material Science
DOE Public Access Plan
U.S. Department of EnergyDE‐AC05‐00OR22725
Office of Science
Oak Ridge National Laboratory
UT-Battelle

    Keywords

    • high energy density
    • lithium–metal batteries
    • polymer electrolytes
    • single-ion conducting

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