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Title: Molecular Simulation Results on Charged Carbon Nanotube Forest-Based Supercapacitors

Abstract

In this paper, electrochemical double-layer capacitances of charged carbon nanotube (CNT) forests with tetraethyl ammonium tetrafluoro borate electrolyte in propylene carbonate are studied on the basis of molecular dynamics simulation. Direct molecular simulation of the filling of pore spaces of the forest is feasible even with realistic, small CNT spacings. The numerical solution of the Poisson equation based on the extracted average charge densities then yields a regular experimental dependence on the width of the pore spaces, in contrast to the anomalous pattern observed in experiments on other carbon materials and also in simulations on planar slot-like pores. The capacitances obtained have realistic magnitudes but are insensitive to electric potential differences between the electrodes in this model. This agrees with previous calculations on CNT forest supercapacitors, but not with experiments which have suggested electrochemical doping for these systems. Finally, those phenomena remain for further theory/modeling work.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]
  1. Tulane Univ., New Orleans, LA (United States). Dept. of Chemical and Biomolecular Engineering
  2. Elizabethtown College, PA (United States). Dept. of Chemistry and Biochemistry
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Biological and Engineering Sciences
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Tulane Univ., New Orleans, LA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC); SNL Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1474079
Report Number(s):
SAND-2018-10191J
Journal ID: ISSN 1864-5631; 667946
Grant/Contract Number:  
NA0003525; AC02-05CH11231; AC52-06NA25296
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 11; Journal Issue: 12; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon; molecular dynamics; nanotubes; pores; supercapacitors

Citation Formats

Muralidharan, Ajay, Pratt, Lawrence R., Hoffman, Gary G., Chaudhari, Mangesh I., and Rempe, Susan B. Molecular Simulation Results on Charged Carbon Nanotube Forest-Based Supercapacitors. United States: N. p., 2018. Web. doi:10.1002/cssc.201800323.
Muralidharan, Ajay, Pratt, Lawrence R., Hoffman, Gary G., Chaudhari, Mangesh I., & Rempe, Susan B. Molecular Simulation Results on Charged Carbon Nanotube Forest-Based Supercapacitors. United States. doi:10.1002/cssc.201800323.
Muralidharan, Ajay, Pratt, Lawrence R., Hoffman, Gary G., Chaudhari, Mangesh I., and Rempe, Susan B. Thu . "Molecular Simulation Results on Charged Carbon Nanotube Forest-Based Supercapacitors". United States. doi:10.1002/cssc.201800323. https://www.osti.gov/servlets/purl/1474079.
@article{osti_1474079,
title = {Molecular Simulation Results on Charged Carbon Nanotube Forest-Based Supercapacitors},
author = {Muralidharan, Ajay and Pratt, Lawrence R. and Hoffman, Gary G. and Chaudhari, Mangesh I. and Rempe, Susan B.},
abstractNote = {In this paper, electrochemical double-layer capacitances of charged carbon nanotube (CNT) forests with tetraethyl ammonium tetrafluoro borate electrolyte in propylene carbonate are studied on the basis of molecular dynamics simulation. Direct molecular simulation of the filling of pore spaces of the forest is feasible even with realistic, small CNT spacings. The numerical solution of the Poisson equation based on the extracted average charge densities then yields a regular experimental dependence on the width of the pore spaces, in contrast to the anomalous pattern observed in experiments on other carbon materials and also in simulations on planar slot-like pores. The capacitances obtained have realistic magnitudes but are insensitive to electric potential differences between the electrodes in this model. This agrees with previous calculations on CNT forest supercapacitors, but not with experiments which have suggested electrochemical doping for these systems. Finally, those phenomena remain for further theory/modeling work.},
doi = {10.1002/cssc.201800323},
journal = {ChemSusChem},
number = 12,
volume = 11,
place = {United States},
year = {2018},
month = {5}
}

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