4.8 Article

High-performance organic pseudocapacitors via molecular contortion

Journal

NATURE MATERIALS
Volume 20, Issue 8, Pages 1136-+

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41563-021-00954-z

Keywords

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Funding

  1. US National Science Foundation Division of Materials Research [DMR-2002634]
  2. Office of Naval Research (ONR) [N00014-16-1-2921]
  3. US Air Force Office of Scientific Research (AFOSR) [FA9550-18-1-0020]
  4. US Department of Defense through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program
  5. National Science Foundation Graduate Research Fellowship Program (NSF GRFP) [2019279091]
  6. Columbia Nano Initiative
  7. Columbia University
  8. Air Force Office of Scientific Research [FA9550-20-1-0233]

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Pseudocapacitors utilize unique charge-storage mechanisms to achieve high-capacity and rapidly cycling devices. An organic system designed through molecular contortion is now shown to exhibit unprecedented electrochemical performance and stability.
Pseudocapacitors harness unique charge-storage mechanisms to enable high-capacity, rapidly cycling devices. Here we describe an organic system composed of perylene diimide and hexaazatrinaphthylene exhibiting a specific capacitance of 689 F g(-1) at a rate of 0.5 A g(-1), stability over 50,000 cycles, and unprecedented performance at rates as high as 75 A g(-1). We incorporate the material into two-electrode devices for a practical demonstration of its potential in next-generation energy-storage systems. We identify the source of this exceptionally high rate charge storage as surface-mediated pseudocapacitance, through a combination of spectroscopic, computational and electrochemical measurements. By underscoring the importance of molecular contortion and complementary electronic attributes in the selection of molecular components, these results provide a general strategy for the creation of organic high-performance energy-storage materials. Pseudocapacitors exhibit charge-storage mechanisms leading to high-capacity and rapidly cycling devices. An organic system designed via molecular contortion is now shown to exhibit unprecedented electrochemical performance and stability.

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