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m-Phenylenediamine as a Building Block for Polyimide Battery Cathode Materials

  • Roman R. Kapaev*
    Roman R. Kapaev
    Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy boulevard 30 Building 1, Moscow 143026, Russia
    Institute of Problems of Chemical Physics of the Russian Academy of Sciences, Acad. Semenov Street 1, Chernogolovka 142432, Russia
    D.I. Mendeleev University of Chemical Technology of Russia, Miusskaya Square 9, Moscow 125047, Russia
    *Email: [email protected] (R.R.K.).
  • Alexey G. Scherbakov
    Alexey G. Scherbakov
    Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy boulevard 30 Building 1, Moscow 143026, Russia
    D.I. Mendeleev University of Chemical Technology of Russia, Miusskaya Square 9, Moscow 125047, Russia
  • Alexander F. Shestakov
    Alexander F. Shestakov
    Institute of Problems of Chemical Physics of the Russian Academy of Sciences, Acad. Semenov Street 1, Chernogolovka 142432, Russia
  • Keith J. Stevenson
    Keith J. Stevenson
    Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy boulevard 30 Building 1, Moscow 143026, Russia
  • , and 
  • Pavel A. Troshin
    Pavel A. Troshin
    Institute of Problems of Chemical Physics of the Russian Academy of Sciences, Acad. Semenov Street 1, Chernogolovka 142432, Russia
Cite this: ACS Appl. Energy Mater. 2021, 4, 5, 4465–4472
Publication Date (Web):March 3, 2021
https://doi.org/10.1021/acsaem.1c00092
Copyright © 2021 American Chemical Society
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Abstract

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Organic compounds have recently gained significant attention as materials for the next generation of sustainable energy storage devices. Polyimides are one of the most attractive types of organic battery cathode materials, especially if they are produced from easily accessible, inexpensive reagents. However, these polymers are still at the early stage of development for rechargeable metal-ion batteries. Particularly, the scope of amine building blocks that were used for the polyimide synthesis remains scarce. In this study, we propose m-phenylenediamine as a building block for polyimide-based cathode materials. We report the electrochemical properties of polyimides obtained from 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) and m- or p-phenylenediamines for lithium-, sodium-, and potassium-ion batteries; and show that the m-polyimide has several advantages over the p-isomer. It has larger capacities and superior high-rate capabilities, owing to a higher specific surface area and smaller particle size. In sodium- and potassium-based batteries, the redox potentials of the m-isomer are higher because of the spatial arrangement of adjacent imide units, which makes chelation of metal cations more energetically favorable. These results provide an impetus for designing new polyimide-based battery materials with higher energy density and fast charge–discharge kinetics.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.1c00092.

  • Comparison of experimental and theoretical FTIR spectra, powder XRD patterns, charge–discharge mechanisms, and additional data on DFT calculations (PDF)

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