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Title: Optimizing supercapacitor electrode density: achieving the energy of organic electrolytes with the power of aqueous electrolytes

Abstract

The value of electrode density is often overlooked in the pursuit of impressive supercapacitor metrics. Low-density electrodes deliver the best performance in terms of gravimetric energy and power densities when only the mass of the electrodes is considered. However, energy and power values with respect to the total system mass (electrode + electrolyte) or volume are more meaningful for practical application. Low-density electrodes are impractical due to both large mass contributions by the electrolyte and large system volumes. In this work, we use highly compressible graphene aerogel electrodes (up to 87.5% volumetric compression) to systematically characterize the effects of electrode density on energy and power metrics. The results reveal that electrode density is similar to electrode thickness in that both parameters have a squared effect on power. Accounting for the aqueous electrolyte's mass lowered the gravimetric energy and power by almost an order of magnitude for 0.144 g cm–3 dense carbon electrodes but only by a factor of 1.5 when the electrode density was increased to 1.15 g cm–3 through compression. The high-density electrodes achieve 8 W h kg–1, 70 000 W kg–1, and 144 F cm–3 in a symmetric electrode setup after factoring in the aqueous electrolyte's mass. Therefore,more » in the pursuit of high energy per mass, it can be just as effective to lower the system's mass with smaller electrolyte fractions as it is to use electrolytes with larger voltage ranges. High electrode densities allow aqueous electrolyte supercapacitors to attain energy densities per the system mass comparable to those of commercially-available organic electrolyte supercapacitors while maintaining 10–100× greater power.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1883022
Report Number(s):
LLNL-JRNL-638656
Journal ID: ISSN 2046-2069; 757538
Grant/Contract Number:  
AC52-07NA27344; 12-ERD-035; 13-LW-099
Resource Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 81; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Merrill, M. D., Montalvo, E., Campbell, P. G., Wang, Y. M., Stadermann, M., Baumann, T. F., Biener, J., and Worsley, M. A. Optimizing supercapacitor electrode density: achieving the energy of organic electrolytes with the power of aqueous electrolytes. United States: N. p., 2014. Web. doi:10.1039/c4ra08114e.
Merrill, M. D., Montalvo, E., Campbell, P. G., Wang, Y. M., Stadermann, M., Baumann, T. F., Biener, J., & Worsley, M. A. Optimizing supercapacitor electrode density: achieving the energy of organic electrolytes with the power of aqueous electrolytes. United States. https://doi.org/10.1039/c4ra08114e
Merrill, M. D., Montalvo, E., Campbell, P. G., Wang, Y. M., Stadermann, M., Baumann, T. F., Biener, J., and Worsley, M. A. Mon . "Optimizing supercapacitor electrode density: achieving the energy of organic electrolytes with the power of aqueous electrolytes". United States. https://doi.org/10.1039/c4ra08114e. https://www.osti.gov/servlets/purl/1883022.
@article{osti_1883022,
title = {Optimizing supercapacitor electrode density: achieving the energy of organic electrolytes with the power of aqueous electrolytes},
author = {Merrill, M. D. and Montalvo, E. and Campbell, P. G. and Wang, Y. M. and Stadermann, M. and Baumann, T. F. and Biener, J. and Worsley, M. A.},
abstractNote = {The value of electrode density is often overlooked in the pursuit of impressive supercapacitor metrics. Low-density electrodes deliver the best performance in terms of gravimetric energy and power densities when only the mass of the electrodes is considered. However, energy and power values with respect to the total system mass (electrode + electrolyte) or volume are more meaningful for practical application. Low-density electrodes are impractical due to both large mass contributions by the electrolyte and large system volumes. In this work, we use highly compressible graphene aerogel electrodes (up to 87.5% volumetric compression) to systematically characterize the effects of electrode density on energy and power metrics. The results reveal that electrode density is similar to electrode thickness in that both parameters have a squared effect on power. Accounting for the aqueous electrolyte's mass lowered the gravimetric energy and power by almost an order of magnitude for 0.144 g cm–3 dense carbon electrodes but only by a factor of 1.5 when the electrode density was increased to 1.15 g cm–3 through compression. The high-density electrodes achieve 8 W h kg–1, 70 000 W kg–1, and 144 F cm–3 in a symmetric electrode setup after factoring in the aqueous electrolyte's mass. Therefore, in the pursuit of high energy per mass, it can be just as effective to lower the system's mass with smaller electrolyte fractions as it is to use electrolytes with larger voltage ranges. High electrode densities allow aqueous electrolyte supercapacitors to attain energy densities per the system mass comparable to those of commercially-available organic electrolyte supercapacitors while maintaining 10–100× greater power.},
doi = {10.1039/c4ra08114e},
journal = {RSC Advances},
number = 81,
volume = 4,
place = {United States},
year = {Mon Sep 01 00:00:00 EDT 2014},
month = {Mon Sep 01 00:00:00 EDT 2014}
}

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