Shape-controlled carbon nanotube

architectures for thermal management

in aerospace applications
Pooja Puneet, Apparao M. Rao, and Ramakrishna Podila
Efficient structural design and thermal management for aerospace structures demand next-
generation lightweight thermally conductive and mechanically robust materials to withstand
high-velocity impacts and distribute localized heat fluxes from spacecraft components.
Notwithstanding the excellent mechanical, electrical, and thermal properties of individual
carbon nanotubes (CNTs), bulk CNT-based composites suffer from CNT anisotropy and
high interjunction resistance. We provide a brief overview of scalable methods that can tune
electrical and thermal connectivity in bulk CNT composites by tuning CNT shape, intertubular
bonding, and packing density. These scalable production methods are posited to open new
avenues for incorporating CNTs into thermal interface materials, structural reinforcement, and
auxiliary power units in the form of energy-storage devices, especially for use in aerospace
applications.

Introduction aerospace structures a reality: (1) notwithstanding the excel-

The air transportation industry continues to grow rapidly, adding
consumer space travel as a new facet on the horizon.1 Despite
this growth, the aerospace industry faces several challenges,
such as high fuel and maintenance costs, that seriously impede
its growth.1,2 Furthermore, there is a critical need for develop-
ing new lightweight materials and sensors that can provide early
warning for radiation and shield the air/spacecraft from pos-
sible hazards from exposure to ionizing radiation, and reduce the
amount of rocket fuel. Emerging lightweight, energy-efficient,
and multifunctional nanomaterial-based composites offer solu-
tions to overcome these challenges.1,2
Carbon-based nanomaterials, in particular, exhibit proper-
ties that are best suited for the highly demanding requirements
of aerospace applications (Figure 1). For instance, single-
and multiwalled carbon nanotubes (SWCNTs and MWCNTs,
respectively) exhibit high thermal conductivities3–12 (κ >
1000 W/[m K]), necessary for efficiently distributing other-
wise localized heat fluxes from spacecraft components such
as propulsion structures, electronic boxes, radiators, and their
accompanying thermal interfaces.
Although carbon nanotube- (CNT-) based composites hold
promise for aerospace applications, two main challenges must
be addressed to make the incorporation of nanomaterials into
lent electrical, thermal, and mechanical properties of indi-
vidual CNTs,6,7,10,12 bulk CNT-based composites suffer from
anisotropy due to inhomogeneous CNT distributions and
intertube interactions (which cause higher electrical and ther-
mal resistance),8,13 and (2) there is still a great need for scal-
able nanomanufacturing methods that increase the production
throughput and reduce the cost of nanomaterial-based com-
posites.14 In this article, we provide a succinct overview of
recent advances aimed at addressing these challenges, primar-
ily through defect engineering and the development of bulk
low-cost manufacturing methodologies.
Efficient CNT-based thermal management
Modern air- and spacecraft thermal design and management
is very challenging because of the continually increasing
heat loads from expanded avionic functionality, microproces-
sors in electronic systems, and complex electrical architec-
tures.2,15 In addition, military aircraft designers also need to
consider heat loads from advanced weapon systems. CNTs
offer excellent promise for efficient thermal management
in aerospace applications because their thermal conductivity
along the long axis of individual CNTs at room temperature
is κ > 3000 W/(m K).

Pooja Puneet, Department of Physics and Astronomy, Clemson University, USA; ppuneet@g.clemson.edu
Apparao M. Rao, Department of Physics and Astronomy, Clemson Nanomaterials Center, Clemson University, USA; arao@g.clemson.edu
Ramakrishna Podila, Department of Physics and Astronomy, Clemson University, USA; rpodila@g.clemson.edu
DOI: 10.1557/mrs.2015.229

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 SHAPE-CONTROLLED CARBON NANOTUBE ARCHITECTURES FOR THERMAL MANAGEMENT IN AEROSPACE APPLICATIONS

engineer thermal boundaries to mitigate phonon

scattering at intertube junctions. Previously, it
has been shown that exposure to ion/electron
irradiation at elevated temperatures can induce
coalescence of nanotubes and weld interjunc-
tions.21,22 Building on these studies, we showed
that spark-plasma sintering (SPS) at 1600°C
can induce covalent intertubular bonding in
aligned MWCNTs, resulting in an enhanced
value of κ ≈ 31 W/(m K) at 300 K in the longi-
tudinal direction (parallel to the axes of tubes),
which is one of the highest reported values for
three-dimensional CNT materials.17,18 SPS is a
high-energy, low-voltage, pulsed plasma dis-
charge method in a low-pressure atmosphere
that can generate highly localized Joule heat-
ing (up to a few thousand kelvin) in a few
minutes.23,24 In addition to inducing intertube
bonding, the SPS process is a high-throughput
Figure 1. Overview of carbon nanotube-based composites and their related applications method by which the packing density of CNTs
in aerospace: (a) Helically coiled multiwalled carbon nanotubes (HCNTs) offer unique can be controlled with the applied pressure and
mechanical properties that are useful in impact protection and electromagnetic interference sintering temperature (see Figure 2a–c).
(EMI) shielding. (b) Aligned arrays of multiwalled carbon nanotubes (MWCNTs) are excellent
lightweight thermal interface materials, and could also be used as supercapacitor electrodes As shown in Figure 2d–f, we observed that
because of their high surface area. (c) MWCNTs can also be assembled into hierarchical the SPS processing temperature (TSPS) provides
aerogels that constitute layers of the so-called buckypapers stitched together by carbon excellent control of density and intertube inter-
fibers for applications in lightweight composites and thermal management.
actions and, thereby, improves the electrical and
thermal conductivities.17,18 In addition to the SPS-
Despite the high κ values of individual CNTs, uncom- induced changes in MWCNT density, high-resolution transmis-
pressed vertically aligned CNTs exhibit a room-temperature sion electron microscopy studies indicated that the MWCNTs
thermal conductivity of κ ≈ 15 W/(m K)8 along the tube direc- were locally welded together during the SPS process (inset
tion, whereas for randomly oriented bulk CNTs, κ ≈ 3 W/(m K).16 in Figure 2c), which is expected to provide new percolating
Evidently, the heat transport in bulk CNT structures is strongly paths to electrons and phonons, thereby mitigating intertube
influenced by the interactions between CNTs, which increase junction resistance. Although such intertube welding may be per-
the interjunction resistance.17,18 Indeed, intertube interactions ceived as a structural defect from a lattice-symmetry standpoint, it
have been proposed to be the dominant factor governing the ultimately improves the electrical and thermal conductivities.
macroscopic electrical and thermal transport in CNT compos- SPS thus is a scalable industrial process for improving the
ites. Although these interactions can break electron–hole sym- thermal properties of MWCNT ensembles through defect engi-
metry and distort the electronic density of states to alter the neering, such as intertubular bonding between neighboring
electrical behavior, the intertube junctions efficiently scatter MWCNTs. The direct current (DC) energy in the SPS process,
phonons to reduce the thermal conductivity.7 which activates the MWCNT surfaces and welds them togeth-
Another factor that can profoundly affect thermal con- er, is often pulsed in a square waveform with a particular ON/
ductivity is the packing density of CNTs. Previously, Hone OFF ratio of p/q, where DC is ON for p pulses and OFF for q
et al. showed that denser SWCNT films exhibit a low resis- pulses in a total of p + q pulses constituting the total SPS pro-
tivity of ρ ≈ 0.125 mΩ cm and a high thermal conductivity cessing time. Previously, we observed that the ON/OFF ratio
of κ > 200 W/(m K) at room temperature parallel to the axes plays a critical role in welding nanojunctions. In this regard,
of the CNTs.19 Wang et al. reported a mechanical process by the SPS process can be further tuned in the future by varying
which high-quality buckypapers could be prepared by roll- the ON/OFF ratio to efficiently weld the tubes and extinguish
ing a cylindrical pin over arrays of MWCNTs. The aligned anisotropy in thermal conductivity through intertubular bond-
orientation of the MWCNTs in their samples improved the ing to achieve predicted κ > 100 W/(m K) in bulk CNTs.23
room-temperature electrical conductivity (σ) in the oriented
direction by a factor of 1.3 and κ by a factor of 2, but the latter Helically coiled carbon nanotubes in aerospace
was still limited to 15 W/(m K).20 applications
For realistic aerospace applications, we must go beyond Many intriguing natural structures gain their functional-
the existing thermal transport paradigm and develop economi- ity through nonlinear complex architectures. For example,
cally viable and scalable methodologies that can efficiently biomolecules, including DNA and proteins, adapt nonlinear

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 SHAPE-CONTROLLED CARBON NANOTUBE ARCHITECTURES FOR THERMAL MANAGEMENT IN AEROSPACE APPLICATIONS

Figure 2. (a) Scanning electron microscope (SEM) image of as-prepared multiwalled carbon nanotube (MWCNT) buckypaper, with
a digital photograph in the inset. (b) SEM image showing the densification of some MWCNTs in the buckypaper upon spark-plasma
sintering (SPS) processing at 1000°C. (c) Higher resolution SEM image of the densified MWCNTs, with a high-resolution transmission
electron microscope image in the inset showing that the MWCNTs are joined at the intertube junction. (d) An increase in the SPS
processing temperature (TSPS) increases the MWCNT packing density, thereby resulting in (e) improved thermal conductivity and
(f) reduced electrical resistivity (ρRT). Reproduced with permission from Reference 17. © 2010 IOP Publishing, and Reference 18.
© 2010 Elsevier.

geometries, particularly spring-like or helically coiled mor-
phologies (such as double-helix, α-coils, or helices) that
provide excellent flexibility and yet impart or retain high
mechanical strength.25 Building on these blueprints provid-
ed by nature, we and others have developed helically coiled
carbon nanotubes (HCNTs) to enable elastic memory devic-
es, flexible electronics, impact protection, nanoinductors,
and efficient electromagnetic shielding for applications in
many fields including aerospace.25–29
The mechanical properties of bulk HCNT foams, (made up
of vertically aligned HCNTs) which originate from their hier-
archically organized microstructure characterized by aligned
and entangled helical coils of MWCNTs, are of particular
interest as structural composites for aerospace applications
(Figure 3a–b).30 HCNTs act like elastic springs, with their
deformation behavior governed by geometric nonlinearity in
their spring constants, which is directly (/inversely) propor-
tional to the HCNT diameter (/coil radius). Such geometric
nonlinearity in the deformation of the individual HCNTs col-
lectively leads to highly nonlinear and non-Hertzian contact
interactions (i.e., mechanical contact interactions where fric-
tion cannot be ignored and surfaces are nanostructured and
not continuous) with projectiles in HCNT foams, which can
efficiently mitigate both low- and high-velocity (0.1–5 m s−1)
impact forces (Figure 3c) and fully recover deformation on the
order 5 μm (5% strain).25,30
In addition to their excellent mechanical properties, HCNTs
exhibit a larger relative dielectric permittivity (ε′), at least
twice that of SWCNTs.29 This increase in ε′ can be explained
on the basis of enhanced capacitive coupling between alter-
nate windings/segments of the coils in HCNTs. Because of
this increase, the electromagnetic interference (EMI) shielding
efficiency of HCNT–reactive ethylene terpolymer composites
could be increased by at least 50% over that of SWCNTs
(Figure 3d). Like HCNTs, bucky aerogels consisting of BP
laminates stitched together by carbon fibers31 also exhibit
improved impact-protection properties and enhanced EMI
shielding because of the capacitive coupling between alter-
nate BP layers.
The National Aeronautics and Space Administration (NASA)
has specified risks of exposure to space radiation as one of
the most significant factors limiting our ability for long dura-
tion space missions. The high chemical and thermal stabil-
ity of HCNTs, combined with their excellent EMI shielding
efficiency, opens new avenues for the use of nanocarbons in
space applications. Furthermore, others, as well as our group,
previously demonstrated the use of CNT arrays in gas-filled
proportional counters 32–34 to overcome the problems of low
absolute detection efficiency and operational issues in radia-
tion detectors. Such detectors can reach detection efficiencies
as low as 10–6%, making it possible for early detection of ion-
izing and other radiations in space.

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engines in aircrafts can be addressed by plac-

ing supercapacitors in parallel with batteries.
The excellent electrochemical stability and
high electrical conductivity of CNTs makes
them ideal electrodes for supercapacitors.
In particular, arrays of vertically aligned mul-
tiwalled CNTs (VACNTs) are attractive for
supercapacitors because of the ability to control
the ion-accessible surface by varying the CNT
areal density on growth substrates. VACNT
electrodes have been used to achieve high-
power-density electrochemical double-layer
capacitors (EDLCs).36–38
However, aerospace applications of VACNTs
have been limited by the lack of continuous
synthesis methods for preparing VACNTs
directly on current collectors (e.g., aluminum
foil) at relatively low cost. Although CNTs can
be synthesized in large quantities, present pro-
cesses are not amenable for VACNT growth
directly on current collectors for scalable man-
ufacturing of EDLC electrodes.
To resolve this challenge, others, and our
group, have developed a commercially viable
Figure 3. (a) Microscopic structure of helically coiled carbon nanotube (HCNT) foams, and relatively low-temperature roll-to-roll (R2R)
characterized by vertically aligned bundles of entangled HCNTs. (b) Representative
transmission electron microscopy image of an HCNT bundle. Reproduced with permission process14,35,39,40 for growing VACNTs on inex-
from Reference 28. © 2008 Wiley. (c) Dynamic stress–strain responses of HCNT foams pensive aluminum-foil current collectors to
subjected to repeated impacts at increasing velocities, showing that HCNT foams can act achieve continuous production of CNT-based
as excellent impact protection materials with recoveries up to 5% strain. Reproduced with
permission from Reference 28. © 2008 Wiley. (d) Electromagnetic interference shielding supercapacitors (Figure 4a). Our electrochem-
efficiency (SE) was observed to be higher for helically coiled CNT foams (labeled CCNT), ical studies on VACNTs produced using this
than for single-walled carbon nanotubes (SWCNTs), a mixture of SWCNTs and multiwalled R2R method displayed significantly lower
carbon nanotubes (labeled as Mix), and pure reactive ethylene terpolymer (RET) because
27
of the capacitive coupling between the alternate coils in HCNTs. Reproduced with contact resistance than traditional activated-
permission from Reference 27. © 1993 American Physical Society. carbon supercapacitors.14 More importantly,
supercapacitors comprising R2R-produced
VACNT electrodes exhibit high power den-
Scalable nanomanufacturing of energy-storage sities (1270 W/kg) and energy densities (11.5 Wh/kg) with
devices for aircraft no loss in performance over more than 1000 cycles and should
In commercial and military aircraft, as well as rocket launches, be highly suitable for integration with batteries for APUs in
particularly those operating in cold regions, large transient elec- aircraft. As an alternative to the R2R process, CNTs can be
trical loading requirements are often placed on their batteries dispersed into ink form and spray-coated directly onto alu-
to provide so-called cold-cranking power to a starter motor. minum foils to achieve supercapacitors with excellent energy
In many current aircraft, the battery system is often oversized and power densities (Figure 4b–c).
to provide the peak powers demanded by the starter motor.
Although batteries have high energy densities, they suffer from Conclusions
poor power delivery rates. The inherently low power densities In this article, we have provided an overview of the possible
of batteries result in an induced stress during operation under mechanical, electrical, and thermal uses of carbon nanomate-
extreme conditions that worsens as the batteries are cycled mul- rials in aerospace applications. Major challenges in integrating
tiple times. This induced stress in batteries increases the servic- CNTs in aircraft design have been the lack of (1) an ability to
ing time and maintenance costs and, more importantly, could control the properties of CNT ensembles and (2) scalable pro-
lead to undesired electrical problems that can harm aircraft. duction methods. However, the SPS method and helical forms
Electrochemical supercapacitors use high-surface-area elec- of CNTs present solutions to control the thermal and electri-
trodes that inherently have high energy and power densities cal properties of bulk CNT composites, and R2R synthesis of
and can function as “fast batteries.”14,35 The increasing power MWCNTS can address the existing manufacturing challeng-
demands of modern electric aircraft and cold-crank auxil- es. With the advent of scalable manufacturing methodologies
iary power units (APUs) necessary to power start the main and improvement of bulk CNT composite properties, one can

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 SHAPE-CONTROLLED CARBON NANOTUBE ARCHITECTURES FOR THERMAL MANAGEMENT IN AEROSPACE APPLICATIONS

Figure 4. (a) Schematic showing the chemical vapor deposition system for roll-to-roll (R2R) production of vertically aligned multiwalled
carbon nanotube (MWCNT) supercapacitor electrodes. The insets at right show a spool of kitchen aluminum foil before and after the growth
of MWCNTs using the R2R process. Reproduced with permission from Reference 14. © 2014 Elsevier. (b) Schematic of a high-throughput
spray-coating R2R process that can also be used to scalably manufacture supercapacitor electrodes. Reproduced with permission from
Reference 30. © 2015 Royal Society of Chemistry. (c) R2R electrodes (magenta stars and red hexagons) exhibit higher energy and power
densities than traditional electrolytic capacitors (olive-green triangles) and state-of-the-art activated carbon electrodes (pink triangles),
but still require further improvements to match the energy density of commercial lithium-ion batteries (black squares). Reproduced with
permission from Reference 30. © 2015 Royal Society of Chemistry.

envision the economically viable incorporation of CNT-based
composites in structural, thermal, and electrical applications
of interest to the aircraft industry. The development of scal-
able intertube bonding methods such as SPS, and high ther-
mal conductivity bulk CNT composites is expected to result in
lightweight materials that can efficiently dissipate heat as well
as shield air and spacecraft from radiation.
Acknowledgments
The authors are thankful to their collaborators Profs. Prabhakar
Bandaru (University of California at San Diego), Chiara
Daraio (ETH Zurich), Jian He (Clemson University), and
Terry M. Tritt (Clemson University) for their support in the
mechanical and thermal characterization of CNT materials. Our
work on the scalable manufacturing of CNTs was supported
by National Science Foundation CMMI Award 1246800.
We dedicate this article to the late Dr. A.P.J. Abdul Kalam,
who played a pivotal role in the development of ballistic and
launch vehicle technologies.
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