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8.1 Introduction
Cooling is one of the most important technical challenges facing numerous diverse
industries, including microelectronics, transportation, solid-state lighting, and manufacturing. Developments driving the increased thermal loads that require advances
in cooling include faster speeds (in the multi-GHz range) and smaller features (to
< 100 nm) for microelectronic devices, higher power engines, and brighter optical devices. The conventional method for increasing heat dissipation is to increase
the area available for exchanging heat with a heat transfer fluid, but this approach
requires an undesirable increase in the size of thermal management system. There
is therefore an urgent need for new and innovative coolants with improved performance. About a decade ago a novel concept of nanofluids, i.e., heat transfer fluids
containing suspensions of nanoparticles, was proposed as a means of meeting these
challenges [1].
Nanofluids are solidliquid composite materials consisting of solid nanoparticles
or nanofibers, with sizes typically on the order of 1100 nm, suspended in a liquid.
Nanofluids have attracted great interest recently due to reports of greatly enhanced
thermal properties at low volume fractions. For example, a small amount (less
than 1% volume fraction) of copper nanoparticles and carbon nanotubes dispersed
S. Volz (ed.), Thermal Nanosystems and Nanomaterials, Topics in Applied Physics, 118
c Springer-Verlag Berlin Heidelberg 2009
DOI 10.1007/978-3-642-04258-4 8,
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in ethylene glycol and oil, respectively, was reported to increase the inherently poor
thermal conductivity of the liquid by 40% and 150%, respectively [25]. Conventional suspensions of well-dispersed particles require high concentrations (> 10%)
of particles to achieve such enhancement; problems of rheology and stability, which
are amplified at high concentrations, preclude the widespread use of conventional
slurries as heat transfer fluids. In several cases, the observed enhancement in thermal conductivity of nanofluids is orders-of-magnitude larger than predicted by wellestablished theories of dispersed particles [612].
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ticle moving with a constant velocity, which decays approximately as the inverse of
the distance from the particle center. The ability of large volumes of fluid dragged
by the nanoparticles to carry substantial amounts of heat was credited for the large
thermal conductivity increases in nanofluids.
A key weakness of this argument is that the thermal diffusivity DT of the base
fluid, which measures the rate of the heat flow via thermal conduction, is several orders of magnitude larger than nanoparticle diffusivity DNP , which measures the rate
of mass motion due to nanoparticle diffusion, whence the magnitude of possible
nanoconvection effects is negligible [24]. Furthermore, the velocity field around a
Brownian particle is much shorter-ranged than that around a particle moving with a
constant velocity [25]. The low estimates for the contribution to thermal transport of
Brownian motion were supported by the results of molecular dynamics simulations
[24, 26], and by the results of experimental measurements on well-dispersed spherical nanoparticle fluids [1619, 27], all showing thermal conductivity enhancements
(positive and negative) that agree with (8.1). In a direct experimental investigation,
the density effects associated with the postulated nanoconvection [23] were experimentally tested with lighter silica and Teflon particles, and were shown to be
incorrect [28]. The nanoconvection velocities were further shown to be of the order of thermophoretic velocities, which for most nanofluids were insignificant (as
low as 109 m/s). Even for sub-nanometer clusters, as evidenced from molecular
dynamics simulations, the thermophoretic velocities are exceedingly small, and this
effectively precludes a discernible contribution to the nanofluid thermal conductivity from any conceivable nanoconvection mechanism [29].
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(8.2)
A simple measure of the relative importance of the interfacial resistance in the overall heat flow in a composite can be obtained from the equivalent thickness h, defined
as the distance over which the temperature drop is the same as at the interface. This
thickness is given by the ratio of the fluid thermal conductivity fluid to the interfacial conductance, i.e., h = fluid /G.
The interfacial thermal resistance effect on well-dispersed spherical particle composites can be estimated by effective medium theory to be [15]
1
NF
,
1 = 3
fluid
+2
(8.3)
where is the ratio of the particle radius to the equivalent matrix thickness h. According to (8.3), when the particle radius becomes equal to the equivalent matrix
thickness ( = 1), there is no enhancement at all, while for larger interfacial resistance ( < 1), the addition of particles decreases the thermal conductivity of the
composite. This effect can explain the decrease of thermal conductivity of nanofluids below the base fluid value [18, 19] and much lower than expected thermal conductivity increases of carbon nanotube nanofluids and carbon nanotube polymer
composites [35, 36].
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8.3 Discussion
Clear experimental evidence for extensive clustering observed in nanofluids indicates that the expected thermal conductivity can fall within a wide range bounded
by (8.4) and strongly depends on the actual aggregation. Recently, using a multilevel effective medium theory, it was demonstrated that the thermal conductivity of
nanofluids can be significantly enhanced by the aggregation of nanoparticles into
chain-like clusters, and this enhancement can be quite dramatic for large, but sparse
clusters [43]. Predictions of this aggregation model were in excellent agreement
with detailed numerical calculations on model nanofluids involving fractal clusters [43]. Thus, allowing for clustering effects dramatically broadens the thermal
conductivity range that is consistent with the effective medium theory [29]. Quite
strikingly, it was demonstrated that the vast majority of experimental results fall
within these bounds, supporting the classical nature of thermal conduction behavior
in nanofluids [44].
The increase in the relative thermal conductivity of nanofluids with temperature [4] is another example of anomalous behavior that cannot be explained on the
assumption of well-dispersed particles. Similarly, the increase in the thermal conductivity with decreasing particle size cannot be explained if the particles are well
dispersed. The probability of aggregation increases with increasing temperature and
decreasing particle size [45]. Therefore the apparent contradictions between experiment and theory, such as particle size effects, can be resolved by weighing in the
ability of nanoparticles to form linear clusters. Furthermore, the temperature dependence is not as strong as it was previously believed to be, with recent experiments
showing a similar variation for both nanofluids and the base fluid [19, 29]. This
implies that the mechanism for increase in the thermal conductivity of water (presumably from the hydrogen bonded structures) is partly responsible for the thermal
conductivity increase in nanofluids as well. Conversely, it is reasonable to expect a
decrease in the nanofluid thermal conductivity for a base fluid that has a negative
change in conductivity with increasing temperature.
It remains a challenge to accurately identify and manipulate the cluster configuration to modify the thermal transport properties of a nanofluid. The two characterization techniques, DLS and SEM, have limitations in assessing the structure of
nanoparticles. DLS measurements are limited to dilute suspensions ( < 1%) for
most nanofluids, while SEM imaging can be performed only after drying the base
fluid. While the science of making well-dispersed colloids has reached a fair level
of maturity, attempts to generate targeted nanoparticle configurations are still in an
evolving phase.
The fact that significant aggregation is required to obtain substantial increases in
thermal transport has an important consequence for the potential application of such
fluids in flow-based cooling, which is the most important benefit from the technological point of view. It is well known that aggregation into sparse but large clusters
increases fluid viscosity. Such increases become very dramatic when the aggregates
start to touch each other, which can occur at very low volume fractions, as low as
0.2% [46]. Therefore, the same aggregate structures that are most beneficial to the
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thermal transport are also the most detrimental to the fluid flow characteristics. Future research should therefore address the issue of optimizing nanofluid structure
with the best combination of thermal conductivity and viscosity.
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