DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites

Abstract

Composite thin films incorporating vertically aligned carbon nanotubes (VACNTs) offer promise for a variety of applications where the vertical alignment of the CNTs is critical to meet performance requirements, e.g., highly permeable membranes, thermal interfaces, dry adhesives, and films with anisotropic electrical conductivity. However, current VACNT fabrication techniques are complex and difficult to scale up. In this paper, we describe a solution-based, electric-field-assisted approach as a costeffective and scalable method to produce large-area VACNT composites. Multiwall-carbon nanotubes are dispersed in a polymeric matrix, aligned with an alternating-current (AC) electric field, and electrophoretically concentrated to one side of the thin film with a direct-current (DC) component to the electric field. This approach enables the fabrication of highly concentrated, individually aligned nanotube composites from suspensions of very dilute (Φ=4×10–4) volume fraction. We experimentally investigate the basic electrokinetics of nanotube alignment under AC electric fields, and show that simple models can adequately predict the rate and degree of nanotube alignment using classical expressions for the induced dipole moment, hydrodynamic drag, and the effects of Brownian motion. The composite AC þ DC field also introduces complex fluid motion associated with AC electro-osmosis and the electrochemistry of the fluid/electrode interface. We experimentally probe the electric-fieldmore » parameters behind these electrokinetic phenomena, and demonstrate, with suitable choices of processing parameters, the ability to scalably produce large-area composites containing VACNTs at number densities up to 1010 nanotubes/cm2. This VACNT number density exceeds that of previous electric-fieldfabricated composites by an order of magnitude, and the surface-area coverage of the 40nm VACNTs is comparable to that of chemical-vapor-deposition-grown arrays of smaller-diameter nanotubes.« less

Authors:
 [1];  [1];  [1];  [2]; ORCiD logo [2];  [1]
  1. Rutgers Univ., Piscataway, NJ (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); Defense Threat Reduction Agency (DTRA)
OSTI Identifier:
1763190
Report Number(s):
LLNL-JRNL-737629
Journal ID: ISSN 0021-8979; 889324; TRN: US2206065
Grant/Contract Number:  
AC52-07NA27344; BA12PHM123
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 117; Journal Issue: 21; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Electromagnetism; Electrokinetic phenomena; Electroosmosis; Brownian motion; Thin films; Nanotubes; Electrical conductivity; Materials; Electric fields; Complex fluids

Citation Formats

Castellano, Richard J., Akin, Cevat, Giraldo, Gabriel, Kim, Sangil, Fornasiero, Francesco, and Shan, Jerry W. Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites. United States: N. p., 2015. Web. doi:10.1063/1.4921948.
Castellano, Richard J., Akin, Cevat, Giraldo, Gabriel, Kim, Sangil, Fornasiero, Francesco, & Shan, Jerry W. Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites. United States. https://doi.org/10.1063/1.4921948
Castellano, Richard J., Akin, Cevat, Giraldo, Gabriel, Kim, Sangil, Fornasiero, Francesco, and Shan, Jerry W. Tue . "Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites". United States. https://doi.org/10.1063/1.4921948. https://www.osti.gov/servlets/purl/1763190.
@article{osti_1763190,
title = {Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites},
author = {Castellano, Richard J. and Akin, Cevat and Giraldo, Gabriel and Kim, Sangil and Fornasiero, Francesco and Shan, Jerry W.},
abstractNote = {Composite thin films incorporating vertically aligned carbon nanotubes (VACNTs) offer promise for a variety of applications where the vertical alignment of the CNTs is critical to meet performance requirements, e.g., highly permeable membranes, thermal interfaces, dry adhesives, and films with anisotropic electrical conductivity. However, current VACNT fabrication techniques are complex and difficult to scale up. In this paper, we describe a solution-based, electric-field-assisted approach as a costeffective and scalable method to produce large-area VACNT composites. Multiwall-carbon nanotubes are dispersed in a polymeric matrix, aligned with an alternating-current (AC) electric field, and electrophoretically concentrated to one side of the thin film with a direct-current (DC) component to the electric field. This approach enables the fabrication of highly concentrated, individually aligned nanotube composites from suspensions of very dilute (Φ=4×10–4) volume fraction. We experimentally investigate the basic electrokinetics of nanotube alignment under AC electric fields, and show that simple models can adequately predict the rate and degree of nanotube alignment using classical expressions for the induced dipole moment, hydrodynamic drag, and the effects of Brownian motion. The composite AC þ DC field also introduces complex fluid motion associated with AC electro-osmosis and the electrochemistry of the fluid/electrode interface. We experimentally probe the electric-field parameters behind these electrokinetic phenomena, and demonstrate, with suitable choices of processing parameters, the ability to scalably produce large-area composites containing VACNTs at number densities up to 1010 nanotubes/cm2. This VACNT number density exceeds that of previous electric-fieldfabricated composites by an order of magnitude, and the surface-area coverage of the 40nm VACNTs is comparable to that of chemical-vapor-deposition-grown arrays of smaller-diameter nanotubes.},
doi = {10.1063/1.4921948},
journal = {Journal of Applied Physics},
number = 21,
volume = 117,
place = {United States},
year = {Tue Jun 02 00:00:00 EDT 2015},
month = {Tue Jun 02 00:00:00 EDT 2015}
}

Works referenced in this record:

Aligned single-wall carbon nanotube polymer composites using an electric field
journal, January 2006

  • Park, Cheol; Wilkinson, John; Banda, Sumanth
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 44, Issue 12
  • DOI: 10.1002/polb.20823

AC Electric-Field-Induced Fluid Flow in Microelectrodes
journal, September 1999

  • Ramos, Antonio; Morgan, Hywel; Green, Nicolas G.
  • Journal of Colloid and Interface Science, Vol. 217, Issue 2
  • DOI: 10.1006/jcis.1999.6346

Scalable Fabrication of Carbon Nanotube/Polymer Nanocomposite Membranes for High Flux Gas Transport
journal, September 2007

  • Kim, Sangil; Jinschek, Joerg R.; Chen, Haibin
  • Nano Letters, Vol. 7, Issue 9
  • DOI: 10.1021/nl071414u

Programmable transdermal drug delivery of nicotine using carbon nanotube membranes
journal, June 2010

  • Wu, J.; Paudel, K. S.; Strasinger, C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 26
  • DOI: 10.1073/pnas.1004714107

Rotational electrophoresis of striped metallic microrods
journal, January 2007


Effect of purification of the electrical conductivity and complex permittivity of multiwall carbon nanotubes
journal, October 2001

  • Grimes, C. A.; Dickey, E. C.; Mungle, C.
  • Journal of Applied Physics, Vol. 90, Issue 8
  • DOI: 10.1063/1.1400100

Enhanced flow in carbon nanotubes
journal, November 2005

  • Majumder, Mainak; Chopra, Nitin; Andrews, Rodney
  • Nature, Vol. 438, Issue 7064
  • DOI: 10.1038/438044a

Fast Mass Transport Through Sub-2-Nanometer Carbon Nanotubes
journal, May 2006


Effect of Mild Nitric Acid Oxidation on Dispersability, Size, and Structure of Single-Walled Carbon Nanotubes
journal, November 2007

  • Tchoul, Maxim N.; Ford, Warren T.; Lolli, Giulio
  • Chemistry of Materials, Vol. 19, Issue 23
  • DOI: 10.1021/cm071758l

Electron Conductive and Proton Permeable Vertically Aligned Carbon Nanotube Membranes
journal, March 2014

  • Pilgrim, Gregory A.; Leadbetter, Joanne W.; Qiu, Fen
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl403696y

Fabrication of flexible, aligned carbon nanotube/polymer composite membranes by in-situ polymerization
journal, June 2014


Electrophoretically induced aqueous flow through single-walled carbon nanotube membranes
journal, January 2012


Transient electric birefringence in suspensions of single-walled carbon nanotubes
journal, November 2005


Organizing Single-Walled Carbon Nanotubes on Gold Using a Wet Chemical Self-Assembling Technique
journal, April 2000

  • Liu, Zhongfan; Shen, Ziyong; Zhu, Tao
  • Langmuir, Vol. 16, Issue 8
  • DOI: 10.1021/la9914110

In-plane-aligned membranes of carbon nanotubes
journal, April 2001


Induced-Charge Electro-Osmosis
text, January 2003


Induced-charge electro-osmosis
journal, January 1999


Carbon nanotube-reinforced epoxy-composites: enhanced stiffness and fracture toughness at low nanotube content
journal, November 2004


Maxwell-Wagner relaxation in piezoactive media
journal, May 2002


Enhancement of hydrogen gas permeability in electrically aligned MWCNT-PMMA composite membranes
journal, October 2010


Chemical Detection with a Single-Walled Carbon Nanotube Capacitor
journal, March 2005

  • Snow, E. S.; Perkins, F. K.; Houser, E. J.
  • Science, Vol. 307, Issue 5717, p. 1942-1945
  • DOI: 10.1126/science.1109128

Water conduction through the hydrophobic channel of a carbon nanotube
journal, November 2001

  • Hummer, G.; Rasaiah, J. C.; Noworyta, J. P.
  • Nature, Vol. 414, Issue 6860
  • DOI: 10.1038/35102535

Metal-Assisted Organization of Shortened Carbon Nanotubes in Monolayer and Multilayer Forest Assemblies
journal, September 2001

  • Chattopadhyay, Debjit; Galeska, Izabela; Papadimitrakopoulos, Fotios
  • Journal of the American Chemical Society, Vol. 123, Issue 38
  • DOI: 10.1021/ja0160243

Preferential Forest Assembly of Single-Wall Carbon Nanotubes on Low-Energy Electron-Beam Patterned Nafion Films
journal, March 2006

  • Wei, Haoyan; Kim, Sang Nyon; Marcus, Harris L.
  • Chemistry of Materials, Vol. 18, Issue 5
  • DOI: 10.1021/cm051074i

Aligning single-wall carbon nanotubes with an alternating-current electric field
journal, June 2001

  • Chen, X. Q.; Saito, T.; Yamada, H.
  • Applied Physics Letters, Vol. 78, Issue 23
  • DOI: 10.1063/1.1377627

Dielectric Measurement of Individual Microtubules Using the Electroorientation Method
journal, May 2006


Dielectric enhancement and Maxwell–Wagner effects in ferroelectric superlattice structures
journal, September 2000

  • O’Neill, D.; Bowman, R. M.; Gregg, J. M.
  • Applied Physics Letters, Vol. 77, Issue 10
  • DOI: 10.1063/1.1290691

Ion exclusion by sub-2-nm carbon nanotube pores
journal, June 2008

  • Fornasiero, F.; Park, H. G.; Holt, J. K.
  • Proceedings of the National Academy of Sciences, Vol. 105, Issue 45
  • DOI: 10.1073/pnas.0710437105

Density control of self-aligned shortened single-wall carbon nanotubes on polyelectrolyte-coated substrates
journal, September 2005

  • Kim, Bumsu; Sigmund, Wolfgang M.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 266, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2005.05.070

DC electric field assisted alignment of carbon nanotubes on metal electrodes
journal, November 2003


Carbon Nanotubes: Present and Future Commercial Applications
journal, January 2013

  • De Volder, Michael F. L.; Tawfick, Sameh H.; Baughman, Ray H.
  • Science, Vol. 339, Issue 6119
  • DOI: 10.1126/science.1222453

Enhancement of thermal interface materials with carbon nanotube arrays
journal, May 2006


Induced electro-optic effects in single-walled carbon nanotubes. II. Hydrodynamics of nanotubes in viscous media
journal, April 2011


Alternating Current Electrokinetic Properties of Gold-Coated Microspheres
journal, September 2012

  • García-Sánchez, Pablo; Ren, Yukun; Arcenegui, Juan J.
  • Langmuir, Vol. 28, Issue 39
  • DOI: 10.1021/la302402v

Hydrodynamic interactions in metal rodlike-particle suspensions due to induced charge electroosmosis
journal, January 2009


Rotational friction of single-wall carbon nanotubes in liquid suspension
journal, February 2009

  • Zimmermann, Frank M.; Shan, Jerry W.
  • Applied Physics Letters, Vol. 94, Issue 5
  • DOI: 10.1063/1.3033365

Predictions of selectivity and flux for CH4/H2 separations using single walled carbon nanotubes as membranes
journal, February 2006


Aligned Multiwalled Carbon Nanotube Membranes
journal, January 2004


Separation Techniques for Carbon Nanotubes
reference-book, November 2007


Simultaneous positioning and orientation of single nano-wires using flow control
journal, January 2013

  • Mathai, Pramod P.; Carmichael, Peter T.; Shapiro, Benjamin A.
  • RSC Advances, Vol. 3, Issue 8
  • DOI: 10.1039/c2ra23190e

Rotational friction on globular proteins combining dielectric and hydrodynamic effects
journal, March 2005


Carbon Nanotube Arrays with Strong Shear Binding-On and Easy Normal Lifting-Off
journal, October 2008


Fast Mass Transport Through Carbon Nanotube Membranes
journal, December 2007


Electromechanics of particles
journal, November 1996


Growth of Ultrahigh Density Single-Walled Carbon Nanotube Forests by Improved Catalyst Design
journal, March 2012

  • Zhong, Guofang; Warner, Jamie H.; Fouquet, Martin
  • ACS Nano, Vol. 6, Issue 4
  • DOI: 10.1021/nn203035x

Electrical polarizability of carbon nanotubes in liquid suspension
journal, May 2007

  • Brown, Matthew S.; Shan, Jerry W.; Lin, Chen
  • Applied Physics Letters, Vol. 90, Issue 20
  • DOI: 10.1063/1.2740186

Electro-orientation of a metal nanowire counterbalanced by thermal torques
journal, June 2014


Colloidal electroconvection in a thin horizontal cell. I. Microscopic cooperative patterns at low voltage
journal, April 2005

  • Han, Yilong; Grier, David G.
  • The Journal of Chemical Physics, Vol. 122, Issue 16
  • DOI: 10.1063/1.1884599

Direct Measurement of Resistance of Multiwalled Carbon Nanotubes Using Micro Four-Point Probes
journal, December 2005

  • Dohn, Søren; Mølhave, Kristian; Bøggild, Peter
  • Sensor Letters, Vol. 3, Issue 4
  • DOI: 10.1166/sl.2005.041

Room-temperature transistor based on a single carbon nanotube
journal, May 1998

  • Tans, Sander J.; Verschueren, Alwin R. M.; Dekker, Cees
  • Nature, Vol. 393, Issue 6680
  • DOI: 10.1038/29954

Large-Scale Preparation of Solubilized Carbon Nanotubes
journal, August 2003

  • Qin, Yujun; Liu, Luqi; Shi, Jiahua
  • Chemistry of Materials, Vol. 15, Issue 17
  • DOI: 10.1021/cm030219n

Self-Alignment of Shortened Multiwall Carbon Nanotubes on Polyelectrolyte Layers
journal, May 2003

  • Kim, Bumsu; Sigmund, Wolfgang M.
  • Langmuir, Vol. 19, Issue 11
  • DOI: 10.1021/la026679x

A facile method to align carbon nanotubes on polymeric membrane substrate
journal, December 2013

  • Zhao, Haiyang; Zhou, Zhijun; Dong, Hang
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep03480

Electric field-induced aligned multi-wall carbon nanotube networks in epoxy composites
journal, January 2005


Dissolution of Full-Length Single-Walled Carbon Nanotubes
journal, April 2001

  • Chen, Jian; Rao, Apparao M.; Lyuksyutov, Sergei
  • The Journal of Physical Chemistry B, Vol. 105, Issue 13
  • DOI: 10.1021/jp002596i

Immobilizing Shortened Single-Walled Carbon Nanotubes (SWNTs) on Gold Using a Surface Condensation Method
journal, January 2002

  • Nan, Xiaolin; Gu, Zhennan; Liu, Zhongfan
  • Journal of Colloid and Interface Science, Vol. 245, Issue 2
  • DOI: 10.1006/jcis.2001.8039

Electro-orientation and electrorotation of metal nanowires
journal, December 2013


Carbon Nanomaterials for Advanced Energy Conversion and Storage
journal, March 2012


Osmotic water transport through carbon nanotube membranes
journal, July 2003

  • Kalra, A.; Garde, S.; Hummer, G.
  • Proceedings of the National Academy of Sciences, Vol. 100, Issue 18, p. 10175-10180
  • DOI: 10.1073/pnas.1633354100

Ultralow Liquid/Solid Friction in Carbon Nanotubes: Comprehensive Theory for Alcohols, Alkanes, OMCTS, and Water
journal, September 2012

  • Falk, Kerstin; Sedlmeier, Felix; Joly, Laurent
  • Langmuir, Vol. 28, Issue 40
  • DOI: 10.1021/la3029403

Electro-casting aligned MWCNTs/polystyrene composite membranes for enhanced gas separation performance
journal, July 2014


Highly efficient electroosmotic flow through functionalized carbon nanotube membranes
journal, January 2011

  • Wu, Ji; Gerstandt, Karen; Majumder, Mainak
  • Nanoscale, Vol. 3, Issue 8
  • DOI: 10.1039/c1nr10303b

Separation Techniques for Carbon Nanotubes
journal, March 2005


Electro-orientation of ellipsoidal erythrocytes. Theory and experiment
journal, May 1993


Works referencing / citing this record:

Graphene−Perfluoroalkoxy Nanocomposite with High Through-Plane Thermal Conductivity Fabricated by Hot-Pressing
journal, September 2019

  • Zhang, Xinru; Xie, Xiaoyu; Cai, Xinzhi
  • Nanomaterials, Vol. 9, Issue 9
  • DOI: 10.3390/nano9091320

Influence of concentration, length and orientation of multiwall carbon nanotubes on the electromechanical response of polymer nanocomposites
journal, September 2019


High-performance Supercapacitors Based on Electrochemical-induced Vertical-aligned Carbon Nanotubes and Polyaniline Nanocomposite Electrodes
journal, March 2017

  • Wu, Guan; Tan, Pengfeng; Wang, Dongxing
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep43676

Aligned-graphene composites: a review
journal, October 2018