Abstract

The challenge of optimizing the pore size distribution of porous electrodes for different electrolytes is encountered in supercapacitors, lithium-ion capacitors and hybridized battery-supercapacitor devices. A volume-averaged continuum model of ion transport, taking into account the pore size distribution, is employed for the design of porous electrodes for electrochemical double-layer capacitors (EDLCs) in this study. After validation against experimental data, computer simulations investigate two types of porous electrodes, an activated carbon coating and an activated carbon fabric, and three electrolytes: 1.5 M TEABF4 in acetonitrile (AN), 1.5 M TEABF4 in propylene carbonate (PC), and 1 M LiPF6 in ethylene carbonate:ethyl methyl carbonate (EC:EMC) 1:1 v/v. The design exercise concluded that it is important that the porous electrode has a large specific area in terms of micropores larger than the largest desolvated ion, to achieve high specific capacity, and a good proportion of mesopores larger than the largest solvated ion to ensure fast ion transport and accessibility of the micropores.

Highlights

  • Porous carbon is the main electrode material in the majority of symmetric electrochemical double-layer capacitors (EDLCs) [1], due to its good conductivity and ability to be activated into a large specific surface area

  • It is applied in different formats, including activated carbon fibers and activated carbon fabrics (ACFs) [2,3], activated carbon (AC) powder coatings [4,5,6], graphene [7,8,9,10,11], graphene oxide [11,12] and carbon nanotubes [13,14,15], where multiwall carbon nanotubes (MWCNT) enhance electrode conductivity [5,16,17]

  • M width:μm these largethese macropores are considered as the reservoirs the bulk of electrolyte electrolyte in the electrode, in the model of ion transport

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Summary

Introduction

Porous carbon is the main electrode material in the majority of symmetric electrochemical double-layer capacitors (EDLCs) [1], due to its good conductivity and ability to be activated into a large specific surface area It is applied in different formats, including activated carbon fibers and activated carbon fabrics (ACFs) [2,3], activated carbon (AC) powder coatings [4,5,6], graphene [7,8,9,10,11], graphene oxide [11,12] and carbon nanotubes [13,14,15], where multiwall carbon nanotubes (MWCNT) enhance electrode conductivity [5,16,17]. Such materials are easy to be recycled [19], where the supercapacitor is disassembled, and a dissolution process is applied to dissolve any electrode binder material [20,21], followed by dielectrophoresis to separate different carbon particulates such as AC, MWCNT and carbon black material [19,22]

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