Journal
ACS NANO
Volume 14, Issue 5, Pages 5314-5323Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b07116
Keywords
energy storage; computational modeling; diffuse double layer; supercapacitors; nanoarchitecture; porous media diffusion; COMSOL Multiyphysics
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Funding
- Air Force Office of Scientific Research (AFOSR) [FA9550-16-1-0230]
- TcSUH
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Structural electrodes made of reduced graphene oxide (rGO) and aramid nanofiber (ANF) are promising candidates for future structural supercapacitors. In this study, the influence of nanoarchitecture on the effective ionic diffusivity, porosity, and tortuosity in rGO/ANF structural electrodes is investigated through multiphysics computational modeling. Two specific nanoarchitectures, namely, house of cards and layered structures, are evaluated. The results obtained from nanoarchitecture computational modeling are compared to the porous media approach and show that the widely used porous electrode theories, such as Bruggeman or Millington-Quirk relations, overestimate the effective diffusion coefficient. Also, the results from nanoarchitecture modeling are validated with experimental measurements obtained from electro-chemical impedance spectroscopy and cyclic voltammetry. The effective diffusion coefficients obtained from nanoarchitectural modeling show better agreement with experimental measurements. Evaluation of microscopic properties such as porosity, tortuosity, and effective diffusivity through both experiment and simulation is essential to understand the material behavior and to improve its performance.
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