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Physics Letters A ()

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4 Physics Letters A 70
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Dependence of the viscosity of nanouids on nanoparticle size and 78
13 material 79
14 80
15 81
V.Ya. Rudyak, S.L. Krasnolutskii
16 82
17 Novosibirsk State University of Architecture and Civil Engineering, Str. Leningradskaya 113, 630008 Novosibirsk, Russia 83
18 84
19 85
20 a r t i c l e i n f o a b s t r a c t 86
21 87
22 Article history: The viscosity of nanouids as a function of nanoparticle size and material is modeled and analyzed. 88
Received 23 January 2014 Dependences of the viscosity of nanouids based on liquid argon with aluminum and lithium
23 89
Received in revised form 28 April 2014 nanoparticles are obtained. The nanoparticle size ranges from 1 to 4 nm. The volume concentration
24 Accepted 30 April 2014 90
of nanoparticles is varied from 1% to 12%. It is shown that the viscosity of the nanouid increases with
25 Available online xxxx 91
Communicated by R. Wu
decreasing nanoparticle size and, in addition, depends on the nanoparticle material.
26 92
2014 Published by Elsevier B.V.
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Keywords:
28 94
Nanouid
29 Viscosity 95
30 Molecular dynamics 96
31 Nanoparticle 97
32 98
33 99
34 100
35
1. Introduction ity of these uids (Einstein, Batchelor, Mooney Akrivos and Chang, 101
36
Krieger, etc.). It has further been found that the effective viscosity 102
37 A nanouid is a two-phase system consisting of a carrier uid of nanouids depends not only on the concentration of nanopar- 103
38 and nanoparticles. Even today it can be argued that nanouids are ticles, but also on their size. Evidence for this has been provided 104
39 a very promising material. They have been used or are planned to by molecular dynamics simulations for the hard-sphere potential 105
40 be used in a variety of chemical reactors and plants, including cat- [4,5] as well as by experiments [3,68]. Recent studies have shown 106
41 alytic ones, for cooling various devices, in the development of new that at a given nanoparticle concentration, the viscosity of nanou- 107
42 systems of heat production and transportation, in biotechnology, ids increases with decreasing nanoparticle size. However, opposite 108
43 nanotechnology, and microelectromechanical systems (MEMS) for data have also been reported [9,10]. Thus, the question of how the 109
44 various purposes, in the design of new drugs and cosmetic prod- viscosity of nanouids depends on the nanoparticle size is still rel- 110
45 ucts, for the delivery of drugs, in the development of systems for evant. Answering this question is the rst objective of this work. 111
46 detecting various contaminants and cleaning air and water, in the Obtaining experimental data on the viscosity of nanouids is 112
47 development of new lubricants, paints, varnishes, construction ma- complicated by several factors: diculties in producing monodis- 113
48 terials, etc. perse suspensions, various methodical problems of accurate mea- 114
49 The specic small sizes of nanoparticles are responsible for surement of particle size, concentration, uniformity of size dis- 115
50 their very special properties. Due to this, nanouids also have spe- tribution, the formation of agglomerated particles, etc. An ideal 116
51 cial properties which cannot be described by classical theories. experiment with a monodisperse nanouid can be performed us- 117
52 Since nearly all applications of nanouids are related to channel ing molecular dynamics (MD) simulation of its viscosity. It is this 118
53 ows, viscosity is a determining factor in their use. The consid- method which is used in the present work to simulate the shear 119
54 erable practical importance of this problem has led several dozen viscosity of nanouids. However, unlike in [4,5], here we use real 120
55 research groups in different countries to undertake experimental interaction potentials, and not the hard-sphere potential. 121
56 studies of the viscosity of nanouids over the last ten to fteen In [3], it is noted that the viscosity of nanouids may also de- 122
57 years (see reviews [13]). It has been well established that the pend on the nanoparticle material. This correlates with the data 123
58 viscosity of nanouids is much higher than the viscosity of con- of the kinetic theory of gas nanosuspensions where this depen- 124
59 ventional dispersions at equal volume concentrations of dispersed dence has been well established [11,12]. The rst MD calculations 125
60 particles and is not described by any classical theory of the viscos- have conrmed the existence of this dependence [13]. Obtaining 126
61 systematic data that would give an unambiguous answer to the 127
62 question of the dependence of the viscosity of nanouids on the 128
63 E-mail address: valery.rudyak@mail.ru (V.Ya. Rudyak). nanoparticle material is the second objective of this paper. We 129
64 130
http://dx.doi.org/10.1016/j.physleta.2014.04.060
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0375-9601/ 2014 Published by Elsevier B.V.
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2 V.Ya. Rudyak, S.L. Krasnolutskii / Physics Letters A ()

1 studied the viscosity of model nanouids in which the carrier the parameters 12 , 12 and , . The simulation was performed as 67
2 uid was argon of density = 0.707 and temperature T = 300 K. follows. Carrieruid molecules and nanoparticles were uniformly 68
3 The dispersed component was lithium and aluminum nanoparti- placed in the simulation cell according to the specied values of 69
4 cles with a diameter from one to four nanometers. The number the density of the carrieruid and the volume concentration of 70
5 of argon molecules in the simulation cell was varied from 7000 to nanoparticles. The density of the pure uid was determined by the 71
6 14,800, and the number of nanoparticles from 1 to 64. The vol- parameters: = N 3 / V and = V / V 0 , where V is the volume of 72
7 ume concentration of nanoparticles was varied from 1% to 12%. the system (cell), V 0 = N 3 / 2 is the volume of close packing of 73
8 The obtained data were averaged over 2000 independent phase N molecules. The volume of the simulation cell for the nanouid 74
9 trajectories. The typical computation time for a single point on was given by the relation V = N 1 3 / 2 + 4 k V N 2 R 3 /3, where 75
10 a personal computer (single-core Intel Core 2) was about 500 h. N 1 and N 2 are the number of molecules and nanoparticles, respec- 76
11 The computational complexity and time naturally increases with tively. With the addition of nanoparticles, the coecient k V was 77
12 increasing number of molecules and nanoparticles in the simula- chosen so that the nanouid pressure was equal to the pressure of 78
13 tion cell and with increasing size and mass of nanoparticles. pure argon of the given density. 79
14 The initial velocities of molecules were specied according to 80
15 2. Simulation technique the Maxwell distribution at the given temperature, and those of 81
16 nanoparticles were set equal to zero. The calculation was started 82
17 In the simulation, we employed a standard molecular dynamics after an initial relaxation period, during which the whole system 83
18 method (see, e.g., [14,15]). A cubic cell and periodic boundary con- had come to equilibrium. The Newton equations were integrated 84
19 ditions were used. Interaction between the molecules of the carrier using Schoelds scheme [19]. 85
20 uid was described by the LennardJones potential Since the potentials used here have an innite range, they 86
21   should be truncated during the simulation. For potential (1), the 87
22 L J (r ) = 4 ( /r )12 ( /r )6 , (1) truncation radius was 2.5 , and for potential (2), it was (R + b12 ). 88
23 The value of b was chosen so that at the truncation radius for 89
where is the effective diameter of the uid molecules, is the
24 potential (2), the force exerted on a molecule by a nanoparticle 90
depth of the potential well, and r = |ri r j | is the distance between
25 was equal to the force of interaction between two molecules at 91
molecules i and j.
26 the truncation radius for potential (1). The quantity b depends on 92
Interaction between carrieruid molecules and a nanoparticle
27 the nanoparticle radius, material and the properties of the carrier 93
was described by the RudyakKrasnolutskii (RK) potential [16,17].
28 uid molecules. In particular, for Li nanoparticles (for the diameter 94
29 of the nanoparticles was 2 nm) in Ar, b was equal to 3.78, and for 95
(r ) = 9 (r ) 3 (r ),
30   Al nanoparticles, it was 4.02. The nanoparticle interaction potential 96
1 1 was truncated at a distance at which the interaction force between
31
i = C i 97
32 (r R )i (r + R )i nanoparticles was zero, i.e., the so-called soft-sphere potential was 98
33
  used. 99
ai 1 1
34 , (2) It should be noted that the simulation of the evolution of 100
r (r R )i 1 (r + R )i 1 nanouids imposes more severe restrictions on the size of the
35 101
36 where i = 9, 3, a9 = 9/8, a3 = 3/2, C 9 = (412 12 12
)/45V p , C 3 = simulation cell as compared with homogeneous uids. Since a 102
nanoparticle should not interact with itself, the side length of the
37 (212 12 )/3V p , V p = p /m p . Here p is the density of the
6 1 103
38 cubic cell L should be much greater than the range of the potential 104
nanoparticle material, m p is the mass of the molecule (atom) of
39 L  R. In practice, the distance should be, at least, several times 105
the nanoparticle, R is the radius of the nanoparticle, i j , i j are the
40 greater to avoid the corresponding correlations. 106
parameters of the interaction potential (1) between a carrieruid
41 The parameters of the interaction potential of argon molecules 107
molecule and a molecule of the nanoparticle.
42 were as follows: = 3.405 and /k B = 119.8 K [20]. The param- 108
As the nanoparticle interaction potential we use a specially con-
43 eters of potentials (2) and (3) were calculated using the following 109
structed potential [18], which for monodisperse nanoparticles has
44 parameters of potential (1): for lithium, = 3.95 and /k B = 110
the form
45 500 K [21], and for aluminum, = 2.551 and /k B = 857.6 K. 111
46 U (r , R ) = U 7 (r , R ) U 1 (r , R ), (3) The latter parameters were obtained from data on Youngs mod- 112
47 ulus and the structure of the crystal lattice (face-centered cubic) 113
48 where using a method similar to that described in [22]. The parameters 114
   12 and 12 were determined using the simple combinational re-
49 2 12 R 2 1 2 1 115
50 U 7 (r , R ) = + + lations: 12 = and 12 = . 116
315 V p2 r (r 2R )7 r7 (r + 2R )7 Shear viscosity was calculated from the GreenKubo formula
51
  [23]
117
52 R 1 1 118

53 3r (r 2R )6 (r + 2R )6
119
  V
54
1 1 2 1 = J xy (t ) J xy (t + t 1 ) + J yz (t ) J yz (t + t 1 )
120
55 5+ , 3k B T 121
30r (r 2R )5 r (r + 2R )5 0
56
    122
57 2 2 6 r 2 4R 2 2 1 1 + J zx (t ) J zx (t + t 1 ) dt 1 , (4) 123
58 U 1 (r , R ) = ln + 2R + 2 . 124
3 V p2 r2 r 2 4R 2 r where the xy component of the stress tensor for a binary mixture
59 125
has the form
60 Here R is the radius of the nanoparticles, and are the parame- 126
61 ters of the LennardJones (1) interaction potential of the nanopar- 1 
2 
N
1 
N1
127
62 ticle molecules. J xy = m xi y i + F x,i j y i j 128
V 2
63 Potentials (2) and (3) were constructed under the assump- =1 i =1 =1,i = j 129
64 tion that the interaction between the carrieruid molecules and
 130
1  N2

N1 N2
65 nanoparticle molecules and the interaction of the nanoparticle + F x,i j y i j + F x,i j y i j . (5) 131
66 molecules form are described by potential (1), respectively, with 2 132
=2,i = j i =1 j =1
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V.Ya. Rudyak, S.L. Krasnolutskii / Physics Letters A () 3

1 The second important point is that the viscosities of the 67


2 nanouids with aluminum and lithium nanoparticles are signi- 68
3 cantly different. Thus, the viscosity of nanouids indeed depends 69
4 on the nanoparticle material. 70
5 To answer the question of how nanouid viscosity depends on 71
6 the nanoparticle size, we performed calculations for nanouids 72
7 with lithium nanoparticles of diameter 1, 2, and 4 nm at vol- 73
8 ume concentrations of nanoparticles = 2% and 4%. The obtained 74
9 data are summarized in Fig. 2 for the two different concentrations, 75
10 = 2% (left) and = 4% (right). In these gures, as before, cir- 76
11 cles represent data for the nanouid with lithium particles, and 77
12 the dotted line shows the obtained dependence (6). 78
13 The results can be approximated, e.g., by the following ex- 79
14 ponential dependence on the nanoparticle diameter in the limit 80
15 D /d  1 which coincides with formula (7) 81
16  2
 82
17 r = B + 5.25 + 40.94 exp(0.208D /d), (8) 83
18 84
Fig. 1. Dependence of the dimensionless viscosity of a nanouid on a volume con- where D is the diameter of the nanoparticles and d is the diameter
19 centration of nanoparticles which are made of different materials. 85
of the molecules. In Fig. 2, this approximation is shown by the
20 86
dotdash line.
21
Here subscript = 1 refers to molecules, subscript 2 to 87
22 88
nanoparticles, mi is the mass of a particle (molecule or nanopar- 4. Discussion of results
23 89
ticle), V is the volume of the system, T is the temperature of the
24 90
medium, is the time to reach a plateau value, F is the force act- The data presented in the previous section suggest that the
25 91
ing on a molecule or nanoparticle, x and y are the coordinates of effective viscosity of nanouids increases with increasing concen-
26 92
the molecule or nanoparticle, and N 1 and N 2 are the numbers of tration of nanoparticles. At moderate volume concentrations of
27 93
molecules and nanoparticles, respectively. The angular brackets in particles, the dependence of the viscosity on the concentration of
28 94
(4) demote an ensemble average. nanoparticles can be described by the quadratic function (6), as
29 95
Eq. (4) were obtained in [23] for molecular systems, but in a for conventional dispersed uids. At the same time, the viscos-
30 96
book of one of the authors [24], it is shown that they have the ity of nanouids at a given particle concentration is substantially
31 97
same form for disperse systems, in particular, for nanouids. higher than that for conventional dispersed uids. This is con-
32 98
sistent with virtually all existing experimental data (see [13]).
33 99
3. Simulation results In addition, the viscosity of a nanouid cannot be described by
34 100
existing classical theories because it depends not only on the con-
35 101
Since all the nanouids studied had a relatively low concen- centration of nanoparticles, but also on their size. For the model
36 102
tration of nanoparticles, it might be expected that the resulting nanouids considered in this paper, this dependence is given by
37 103
viscosity would be described by a quadratic dependence on the relation (8), which is in qualitative agreement with the data of [3,
38 104
volume concentration of nanoparticles 68]. The viscosity of nanouids decreases with increasing parti-
39 105
cle size. Physically, this is a reasonable result since as the particle
40 106
size tends to the size of conventional macroscopic particles, rela-
41 = r = 1 + a1 + a2 2 , (6)
tion (6) should reduce to the classical formulas for the viscosity of 107
42
0 108
nanouids, e.g., in formula (7).
43 where 0 is the viscosity of pure argon. Our calculations have Another important feature that distinguishes the viscosity of 109
44 shown that it is indeed so. The dependence of the dimensionless nanouids from that of conventional dispersions is its dependence 110
45 viscosity r on the volume concentration of nanoparticles is shown on the nanoparticle material. This dependence should disappear 111
46 in Fig. 1. Here the density of the carrier uid was = 0.707, and with increasing nanoparticle size. However, if the particles are suf- 112
47 the temperature T = 300 K; circles represent data for the nanouid ciently small, accounting for this dependence is important and 113
48 with Li particles, and triangles represent data for the nanouid 114
one cannot hope to obtain a universal formula for the viscosity.
49 with Al particles. In all cases, the diameter of the nanoparticles 115
It can be expected that this dependence can be neglected even
50 was 2 nm. As a result, for the nanouid with lithium nanoparticles, 116
for nanouids with a characteristic particle size of more than ten
51 in formula (6) we obtained a1 = 3.20 and a2 = 25.38 (dashdot nanometers. Indirect evidence for this is provided by kinetic the- 117
52 line in Fig. 1), and for the nanouid with aluminum nanoparti- 118
ory [11,12] and molecular dynamics simulations of the diffusion
53 cles, a1 = 3.25 and a2 = 13.06 (dotted line in Fig. 1). In all cases, of nanoparticles [26]. It should also be noted that the appear- 119
54 the viscosity is substantially higher than that for conventional dis- 120
ance of the dependence on the nanoparticle material is not due
55 persions. Thus, even at low particle concentrations, the effective 121
to the choice of a particular interaction potential; it has also been
56 viscosity of nanouids is not described by Einsteins theory, which 122
recorded for the hard-sphere potential [4,5]. The appearance of this
57 gives a1 = 2.5. The dotted line in Fig. 1 shows the dependence dependence is due to taking into account the individual charac- 123
58 obtained by Batchelor [25] taking into account the hydrodynamic 124
teristics of nanoparticles (in particular, their weights and interac-
59 interaction of dispersed particles and their Brownian motion 125
tion potential parameters) in their interaction with carrieruid
60 126
molecules and with each other, as is the case in conventional
61 2 127
B = 1 + 2.5 + 6.2 , (7) molecular uids. To see this, it is necessary to analyze the simula-
62 128
tion process of nanouids from a molecular-kinetic point of view.
63 The Batchelor formula (7) provides a good t to various exper- According to (4), (5), the viscosity of nanouids contains several 129
64 imental data for conventional disperse systems, but the values different contributions: 130
65 given by this formula are signicantly smaller than those for 131
66 nanouids (see Fig. 1). = k + p + kp , (9) 132
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4 V.Ya. Rudyak, S.L. Krasnolutskii / Physics Letters A ()

1 67
2 68
3 69
4 70
5 71
6 72
7 73
8 74
9 75
10 76
11 77
12 78
13 79
14 80
15 81
16 82
17 83
18 84
19 85
Fig. 2. Dependence of the dimensionless coecient of effective viscosity on diameter (nanometer) of nanoparticles which are made of lithium in argon. = 0.707, T = 300 K,
20 86
= 2% (left), = 4% (right).
21 87
22 88
where the rst term describes the kinetic contribution Table 1
23 89
 N  Contributions of different components to the viscosity of nanouids (Pa s).
24
1 
  N
Ar AlAr LiAr
90
25 k = m xi y i (t ) m x j y j (t + t 1 ) dt 1 , 91
kB T V 117.4 169.8 182.9
26 ,=1,2 0 i =1 j =1 k 13.4 11.6 11.0
92
27 93
(10) p 88.0 138.5 153.0
28 kp 16.1 19.7 18.9 94
29 the second term describes the potential contribution p1,1 88.0 81.7 83.0 95
30 p12 34.7 44.0 96
 N 

 N ( p1, p12 + p12, p1 ) 22.1 25.9
31
1  97
32 p = F x,i j y i j (t ) F x,kl ykl (t + t 1 ) dt 1 98
4k B T V
33 ,=1,2 0 i = j k=l contribution due to the last term in (11). From an analysis of the 99


  data, it appears that, rst, although the overall viscosity of nanou-
34 100
35 1 
N1 N2
 
N1 N2
ids is signicantly higher than the viscosity of the carrier uid, the 101
+ F x,i j y i j (t ) F x,kl ykl (t + t 1 ) dt 1
36
kB T V kinetic contributions k are lower. This decrease is due to a reduc- 102
i =1 j =1 k =1 l =1
37 0 tion in the number density of molecules in the nanouid compared 103
 N

 to the carrier uid. On the other hand, the kinetic contribution of
38 104
1 
N1 N2
39
+ F x,i j y i j (t ) F x,kl ykl (t + t 1 ) nanoparticles is small since the volume of a nanoparticle is much 105
40 2k B T V higher than the volume of the molecule, with the conservation of 106
0 i = j k =1 l =1
41
 the average kinetic energy of the molecules and nanoparticles. It 107
42 N1 N2

N should also be emphasized that since the uid is dense, the con- 108
43 + F x,kl ykl (t ) F x,i j y i j (t + t 1 ) dt 1 , (11) tribution of the kinetic processes to the transfer of the momentum 109
44 k =1 l =1 i = j (viscosity) is small: for argon, it is about 11%, and for the nanou- 110
45 ids, 67%. 111
and the third describes the cross effects
46 The potential contribution of the molecules p1,1 (sixth row of 112
 N 

 N in Table 1) in the nanouids is also slightly reduced. The role of
47 113
1 1
48
kp = m xi y i (t ) F x,kl ykl (t + t 1 ) dt 1 the cross terms kp (fth row in Table 1) is small and is about ten 114
49 kB T V 2 percent. In all our calculations, the potential contribution of the 115
,=1,2 0 i =1 k=l
50 particle interaction was almost equal to zero. Thus, the increase in 116
 N  
51 
  
N1 N2 the viscosity is due mainly to nanoparticlemolecule interactions 117
52 + m xi y i (t ) F x,kl ykl (t + t 1 ) dt 1 . and the correlations between moleculemolecule and molecule 118
53 =1,2 0 i =1 k =1 l =1 nanoparticle interactions. Dependence of value of these contribu- 119
54 tions on a size of the dispersed particles is easy for qualitative 120
(12)
55 estimating. Let there be particles with radiuses R 1 and R 2 , for 121
56 The table shows a comparison of each of the contributions for deniteness we will consider that R 2 > R 1 . At the given volume 122
57 argon and the two nanouids considered. In both cases, the con- concentration numbers of those and other particles in a unit vol- 123
58 centration of nanoparticles was equal to = 0.097, and the diam- ume are in inverse proportion to cubes of their radiuses: N 2 / N 1 = 124
59 eter of the nanoparticles was 2 nm. The pressure of all three uids R 31 / R 32 . On the other hand, total cross-sections of scattering of 125
60 was the same and equal to the pressure of pure Ar at a density molecules of a carrying uid with those and with other parti- 126
61 = 0.707 and a temperature T = 300 K. The sixth row of the ta- cles are accordingly equal S 1 = N 1 R 21 and S 2 = N 2 R 22 . Therefore 127
62 ble shows the potential contribution to the viscosity due to the the ratio of these cross-sections which determine value of consid- 128
63 interaction of argon molecules, the seventh row shows the poten- ered potential contributions, appears to be inversely proportional 129
64 tial contribution due to the correlation between the intermolecular to their radiuses: S 2 / S 1 = R 1 / R 2 . These simple estimations show 130
65 forces and the interaction forces of the molecules with the parti- that with growth of particle sizes the relative value of these con- 131
66 cle (the third term in formula (11)). Finally, the last row shows the tributions will decrease. In conclusion, two things must be pointed 132
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V.Ya. Rudyak, S.L. Krasnolutskii / Physics Letters A () 5

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14921506.
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70
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12 sity Press, 1995, 549 pp. 78
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