J Nanopart Res (2008) 10:10891097 DOI 10.

1007/s11051-007-9352-1

FOCUS ON NANOFLUIDS

Thermal conductance of nanouids: is the controversy over?

Pawel Keblinski Ravi Prasher Jacob Eapen

Received: 16 December 2007 / Accepted: 22 December 2007 / Published online: 18 January 2008 Springer Science+Business Media B.V. 2008

Abstract Over the last decade nanouids (colloidal suspensions of solid nanoparticles) sparked excitement as well as controversy. In particular, a number of researches reported dramatic increases of thermal conductivity with small nanoparticle loading, while others showed moderate increases consistent with the effective medium theories on well-dispersed conductive spheres. Accordingly, the mechanism of thermal conductivity enhancement is a hotly debated topic. We present a critical analysis of the experimental data in terms of the potential mechanisms and show that, by accounting for linear particle aggregation, the well established effective medium theories for composite materials are capable of explaining the vast majority of the reported data without resorting to novel mechanisms such as Brownian motion induced nanoconvection, liquid layering at the interface, or near-eld radiation. However, particle aggregation required to signicantly enhance thermal conductivity, also increases uid viscosity rendering the benet
P. Keblinski (&) Materials Science and Engineering Department, Rensselaer Polytechnic Institute, Troy, NY 12180, USA e-mail: keblip@rpi.edu R. Prasher Intel Corporation, 5000 W. Chandler Blvd, Chandler, AZ 85226, USA J. Eapen Theoretical Division (T-12), Los Alamos National Laboratory, Los Alamos, NM 87545, USA

of nanouids to ow based cooling applications questionable. Keywords Nanouids Aggregation Thermal conductivity Theory Nanoparticles Heat transfer

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 uid 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 nanouidsheat transfer uids containing suspensions of nanoparticleshas been proposed as a means of meeting these challenges (Choi 1995). Nanouids are solid-liquid composite materials consisting of solid nanoparticles or nanobers, with

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sizes typically on the order of 1100 nm, suspended in a liquid. Nanouids 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 in ethylene glycol and oil, respectively, was reported to increase the inherently poor thermal conductivity of the liquid by 40 and 150%, respectively (Choi et al. 2001; Eastman et al. 2001). Conventional suspensions of well-dispersed particles require high concentrations ([10%) of particles to achieve such enhancement; problems of rheology and stability, which are amplied at high concentrations, preclude the widespread use of conventional slurries as heat transfer uids. In several cases, the observed enhancement in thermal conductivity of nanouids is orders-of-magnitude larger than predicted by wellestablished theories of dispersed particles (Chopkar et al. 2006; Chopkar et al. 2007; Hong et al. 2006; Kang et al. 2006; Murshed et al. 2005, 2006; Zhu et al. 2006; Zhu et al. 2007).

 3/KNP Kfluid Kfluid 1 3Kfluid 1 /KNP Kfluid   31 /KNP Kfluid  KNF  1 KNP 3KNP /KNP Kfluid

The purported inadequacy of the effective medium theories The experimental observations described above led to numerous statements about inability of well-established effective medium theories for explaining the thermal conductivity enhancements of nanouids. In particular, in the limit of low particle volume fraction, /, and the particle conductivity, KNP, being much higher than the uid conductivity, Kuid, the effective medium (Maxwell) theory for vanishing interfacial thermal resistance predicts (Maxwell 1881; Nan et al. 1997) KNF 1 3/ Kfluid 1

Maxwells expression (the limiting case of which is given by Eq. 1) also corresponds to the lower bound of the well known Hashin and Shtrikman (H S) bounds for thermal conductivity obtained under the effective medium theory analysis (Hashin and Shtrikman 1962) without any restriction on the volume fraction. The HS bounds for a nanouid are given by:

In the inequality given by Eq. 2, the lower (Maxwell) bound physically corresponds to a set of well-dispersed nanoparticles in a uid matrix while the upper limit corresponds to large pockets of uid separated by linked, chain-forming or clustered nanoparticles. From the point of view of circuit analysis, the lower HS limit lies closer to conductors connected in a series mode, while the upper limit lies closer to those in a parallel mode. The HS bounds do not give a precise mechanism of thermal conductance but sets the most restrictive limits based on the knowledge of volume fraction alone. It is relatively well known that a large number of experimental data on solid composites, and to a lesser extent the data on liquid mixtures, fall between the HS bounds (Eapen et al. 2007c). An unbiased estimation (neither favoring series nor parallel modes) predicts thermal conductivity values that lie between the upper and lower HS bounds (Landauer 1952). Several experimental data show that the enhancement in nanouids are well-described by Eq. 1 (Keblinski et al. 2005; Putnam et al. 2006; Venerus et al. 2006; Zhang et al. 2006a, b). For example at 1% particle volume fraction, the maximum relative enhancement is 3%. However, those experimental reports demonstrating much larger enhancements deem the classical effective medium theories to be inadequate, thereby giving credence to the so called anomalous or unusual thermal conductivity enhancements. This judgment is solely reached by comparing the experimental results with the theories that assume good dispersions of spherical nanoparticles. The evidences from Scanning Electron Microscopy (SEM) however, point to the existence of partial clustering and chain-like linear aggregation (Kim et al. 2007; Murshed et al. 2005; Zhu et al. 2006; Zhu et al. 2007). This demands a different effective medium model for nanouids wherein the effects of clustering is explicitly taken into account. The upper HS bound in Eq. 2 indicates that a linear aggregation will increase the thermal conductivity beyond the limit of well-dispersed nanouids. Viscosity data on nanouids has also shown anomalous increase as compared

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to the Einstein model for well-dispersed particles (Prasher et al. 2006c). Large increase in the viscosity is another indication of aggregation in the nanouids. It was also recognized that elongated nanoparticles would lead to larger predictions of the conductivity enhancements (Keblinski et al. 2002), however, in the most spectacular cases, the required nanoparticle aspect ratio was of the order of 100 or more, which is rather unrealistic for individual nanoparticles, unless there is linear particle agglomeration. Interestingly, in case of carbon nanotube suspension, the effective medium theory accounting for very high aspect ratio of nanotubes (Nan et al. 1997), predicts thermal conductivity enhancements which are in fact well above the reported values. This was attributed to a signicant interfacial resistance to heat ow between carbon nanotubes and the uid (Huxtable et al. 2003). On the basis of these observations, there is no sufcient reason to presume that there is a failure of effective medium theories in accounting for the thermal conductivity of nanouids. Other interesting observations in this rapidly evolving eld include a temperature dependence on the thermal conductivity (Das et al. 2003; Patel et al. 2003) and a strong size dependency (Hong et al. 2006; Kim et al. 2007). There appears to be a fundamental difference between the conductance behavior of solid composites and nanouids where smaller particle sizes favor an increased conductivity for the latter, and the reverse for the former. As with the nanotubes suspensions, the solid composite behavior is easily explained through the interfacial thermal resistance for nanometer sized ller particles (Every et al. 1992; Nan et al. 1997) while its role in nanouids is less than transparent. A few experiments (Hong et al. 2005; Zhu et al. 2006) also have also shown that the nanouid thermal conductivity is not correlated in a simple manner to that of the nanoparticle as predicted by the effective medium theories, and a saturation behavior at higher volume fractions which is qualitatively different from that in solid composites (Eapen et al. 2007c).

the concept of Brownian motion induced micro or nanoconvection (Jang and Choi 2004; Koo and Kleinstreuer 2004; Prasher et al. 2005). They argued in different forms that each Brownian particle generates a long-ranged velocity eld in the surrounding uid, akin to that present around a particle moving with a constant velocity, which decays approximately as the inverse of the distance from the particle center. The ability of large volumes of uid dragged by the nanoparticles to carry substantial amount of heat was credited for the large thermal conductivity increases of nanouids. A key weakness of this argument is that the thermal diffusivity, DT, of base uid, that measures the rate of the heat ow via thermal conduction is several orders of magnitude larger than nanoparticle diffusivity, DNP, that measures the rate of mass motion due to nanoparticle diffusion, and thus the magnitude of possible nanoconvection effects is negligible (Evans et al. 2006). These estimates were supported by the results of molecular dynamics simulations (Evans et al. 2006; Vladkov and Barrat 2006), and by the results of experimental measurements on well-dispersed spherical nanoparticle uids (Putnam et al. 2006; Rusconi et al. 2006; Venerus et al. 2006; Zhang et al. 2006a, b) all showing thermal conductivity enhancements (positive and negative) that agree with the lower HS (Maxwell) limit. In a direct experimental investigation, the density effects associated with the postulated nanoconvection (Prasher et al. 2005) were experimentally tested with lighter silica and Teon particles, and were shown to be incorrect (Eapen et al. 2007d). The nanoconvection velocities were further shown to be of the order of thermophoretic velocities, which for most nanouids were insignicant [as low as (10-9 m/s)]. Even for sub-nanometer clusters, as evidenced from molecular dynamics simulations, the thermophoretic velocities are exceedingly small which effectively preclude a discernible contribution to the nanouid thermal conductivity from any conceivable nanoconvection mechanism (Eapen et al. 2007c).

New physics Brownian motion Motivated by the unusual thermal conductivity enhancements, a number of researchers promoted Interfacial liquid layer Considering that the molecular structure of liquid at the solid interface is more ordered, possibilities of

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larger thermal conductivity of this ordered liquid layer and tunneling of heat carrying phonons from one particle to another (Keblinski et al. 2002) were put forward. The subsequent molecular dynamics simulation work concluded that those mechanisms do not contribute signicantly to heat transfer (Xue et al. 2004). For strong solidliquid interactions, typical of those in nanouids with metallic nanoparticles, a percolating network of amorphous-like uid structures can emerge which can facilitate additional thermal conduction paths (Eapen et al. 2007a, b). However, a discernible increase in thermal conductivity is possible only for exceedingly small colloidal particles (limited to few tens of atoms). Experiments have shown that the structured interfacial uid layers are limited to a few molecular spacings from a solid surface (Yu et al. 2001) which makes them inadequate to inuence the thermal transport in common nanouids. Furthermore, interpretation of the cooling rates of Au nanoparticles suspended in water and organic solvents does not appear to require any unusual thermophysical properties of the surrounding liquid to explain the experimental results (Wilson et al. 2002).

Back to old physics: the effective medium theory revisited As discussed in Sect. The purported inadequacy of the effective medium theories, it is generally believed that the thermal conductivity in nanouids is in disagreement with the effective medium theories, however, this disagreement is with the theories that assume well-dispersed particles. Linear agglomeration of particles leads to extended paths of high thermal conductivity, which naturally has a positive impact on the thermal conductivity. Recently, using a multi-level effective medium theory, it was demonstrated that the thermal conductivity of nanouids can be signicantly enhanced by the aggregation of nanoparticles into chain-like clusters, and this enhancement can be quite dramatic from large, but sparse clusters (Prasher et al. 2006a). Predictions of this aggregation model were in excellent agreement with detailed numerical calculations on model nanouids involving fractal clusters (Prasher et al. 2006a). In the limit /DNP =Dfluid  1 this model predicts DNF/ Duid = (//3)DNP/Duid which can be compared to (2//3)DNP/Duid and /DNP/Duid, for the upper HS bound and parallel mode respectively, where DNP denotes the nanoparticle thermal conductivity. Notice that the effective thermal conductivity for aggregated nanouids is a function of DNP and a larger enhancement is theoretically predicted when DNP/ Duid is large. Thus, allowing for clustering effects dramatically broaden the thermal conductivity range that is consistent with the effective medium theory. To test our assertions, in Fig. 1, we have depicted a large number of representative experimental data (Eapen et al. 2007c) on nanouid thermal conductivity as a function of nanoparticle volume fraction along with the lower and upper HS bounds (dashed and solid lines respectively). Quite strikingly, almost all the data fall within these bounds supporting the classical nature of thermal conduction behavior in nanouids.

Near eld radiation Somewhat less popular, was the idea of anomalously high radiative energy transfers between nanoparticles (Domingues et al. 2005). Since the classical radiation theory does not predict radiative transfer of signicance for nanouids, molecular dynamics simulations of thermal energy exchange between two silica nanoparticles were carried on, resulting in prediction of enormous thermal conductance due to near-eld interactions, when particles were closely separated (Domingues et al. 2005). However, the thermal conductance obtained from molecular dynamics was signicantly larger than that obtained under the assumption that all the thermal energy is exchanged between two nanoparticles within a single atomic vibration period. Further analysis demonstrated that near-eld interactions do not affect the nanouid thermal conductivity (Ben-Abdallah 2006).

Discussion There are several interesting aspects with the nanouid data depicted in Fig. 1. First, the HS bounds obeyed by nanouids are remarkably similar to those

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J Nanopart Res (2008) 10:10891097 Fig. 1 Lower (dashed) and upper (solid) Hashin and Shtrikman (HS) bounds for nanouid thermal conductivity. The thermal conductivity data are taken from (Choi et al. 2001; Das et al. 2003; Eapen et al. 2007c; Eastman et al. 1997; Eastman et al. 2001; Hwang et al. 2007; Kang et al. 2006; Lee et al. 1999; Li and Peterson 2006; Masuda et al. 1993; Murshed et al. 2005, 2006; Patel et al. 2003; Shaikh et al. 2007; Wen and Ding 2004a; Wen and Ding 2004b, 2006; Zhang et al. 2006a, b; Zhu et al. 2006; Zhu et al. 2007) while the properties are given in (Eapen et al. 2007c)
Water-Al2O3
100 100 10 1 0.1 0.01 1E-3 0 1 2 3 4 5 0 1 2 3 4 5

1093
Water-CuO

Enhancement in (%)

1
0.1 0.01 1E-3

Eapen et al2007c Eastman et al1997 Masuda et al 1993 Das et al 2003 Wen et al 2004b

Enhancement in (%)

10

Eastman et al (1997) Zhu et al (2007) LiandPeterson(2006) Lee et al (1999) Das et al (2003)

6

(Al2O3) % Water-ZrO2
100

(CuO)% Water-TiO2

Enhancement in (%)

10

Enhancement in (%)

10

Eapenet al 2007c Zhanget al 2006b

0.1

Murshed et al 2005 Wen and Ding 2006 Zhang et al 2006b

0 1 2 3 4 5

10

(ZrO2)%
Water-SiO2

(TiO2) % Water-Fe3O4 (Zhu et al2006)

Enhancement (%)

10

Enhancement in (%)

10

Eapen et al 2007 c Kang et al 2006

1

10 12 14 16 18 20

(SiO2) %

(Fe3O4)%

observed in solid composites and even liquid mixtures (Eapen et al. 2007c). Second, as the ller particle size approaches the nanometer scales, the effective thermal conductivity of solid composites decreases due to increasing interfacial resistance (Eapen et al. 2007c; Every et al. 1992; Nan et al. 1997). A large body of experimental data in Fig. 1 however, suggests that the interfacial resistance does not play a signicant role in nanouids even when the particle sizes are in tens of nanometers. This is easily veried for well-dispersed nanoparticles where the thermal conductivity largely follows the classical

Maxwell relationship. The fact that solid composites are different from nanouids in this respect is likely associated with the possibility of having imperfect solidsolid interfaces, including effects of physical delamination and voids that can be present near or at the interface. This can substantially increase the interface resistance as compared with that originating solely from acoustic mismatch between the ller and the matrix. By contrast uids form void free contacts with solids. Another important point is that the Kapitza length which is given by Rbkm, where Rb is the interface resistance and km is the thermal

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1094 Fig. 1 Continued

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Toulene-Au (Patel et al, 2003)
1000

EG-Cu (Eastman et al, 2001)

Enhancement in (%)

Enhancement in (%)

100 10 1 0.1 0.01 0.0

0.1

0.01

With Acid Old

0.1 0.2 0.3 0.4 0.5 0.6

1E-3 0.004

0.006

0.008

0.010

0.012

(Au) %

(Cu) %

EG-Al (Mursheed et al 2006)

10000
1000

Engine Oil-Al (Mursheed et al 2006)

Enhancement (%)

100

Enhancement (%)
1 2

1000

100

10

10

1 3 4 5

1
1 2

(Al) %

(Al) %

Oil/Water-Carbon Nanotubes
10000 1000
Enhancement in (%)
1000

EG-Diamond (Kang et al 2006)

100 1 0.1 0.01 Shaik et al (2007) Zhang et al (2006) Choi et al (2001) Hwang et al (2007) Wen and Ding(2007) 0.0 0.2

Enhancement (%)

10

100

10

1E-3 1E-4 1E-5 0.4

0.6

0.8

1.0

0.1 0.00

0.25

0.50

0.75

1.00

1.25

1.50

(Nanotubes)%

(Diamond)

conductivity of the matrix is higher in solids than liquid due to higher value of km. Higher value of Kapitza length means higher impact of the interface resistance. Increase in the relative thermal conductivity of the nanouids with temperature (Das et al. 2003) is another anomalous behavior that cannot be explained based on the assumptions of well-dispersed particles. Similarly 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 (Prasher et al. 2006b). Therefore the apparent contradictions between experiment and theory, such as particle size effects, can be resolved by weighing in the ability of nanoparticles into forming linear clusters. Furthermore, the temperature dependence is also not as strong as it was earlier believed with the recent experiments showing a similar variation for both nanouids and the base uid (Eapen et al. 2007c; Zhang et al. 2006b). This implies that the mechanism for increase in the thermal conductivity of water (presumably from the hydrogen bonded structures) is partly responsible for

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the thermal conductivity increase in nanouids as well. Conversely, it is reasonable to expect a decrease in the nanouid thermal conductivity for a base uid that has a negative change in conductivity with increasing temperature. It remains a challenge to accurately identify and manipulate the cluster conguration to modify the thermal transport properties of a nanouid. 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 nanouids while SEM imaging can be performed only after drying the base uid. While the science of making well-dispersed colloids have reached a fair amount of maturity, the attempts at generating targeted nanoparticle congurations is still in an evolving phase.

are most benecial to the thermal transport are also the most detrimental to the uid ow characteristics. The future research, therefore, should address the issue of optimization of nanouid structure with the best combination of thermal conductivity and viscosity.

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Conclusions Our considerations strongly suggest that the apparent disagreement between the experiment and the effective medium theory is simply an artifact of focusing on a particular effective medium theory, namely, Maxwells theory of well-dispersed particles. Removing this constraint and allowing chain-forming morphologies for nanoparticles, we show that the effective medium theories are capable of predicting thermal conductivity enhancements well beyond the Maxwell prediction. Indeed, all the published data on nanouids, except for a couple of sets, lies between the well-known Hashin and Shtrikman (HS) effective medium bounds. Thus, we provide a strong evidence to show that the thermal conductance behavior of nanouids, to a large extent, is no different from that in binary solid composites or liquid mixtures (Eapen et al. 2007c). The fact that signicant aggregation is required to obtain substantial increases in thermal transport has an important consequence on the potential application of such uids in ow based cooling, which is the most important benet from the technological point of view. It is well know that aggregation into sparse but large clusters increase uid viscosity. Such increases become very dramatic when the aggregates start to touch each other, which can occur at very low volume fraction, as low as 0.2% (Kwak and Kim 2005). Therefore, the same aggregate structures that

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