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chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx

liquid–liquid extraction column

Hossein Bahmanyar a,∗

a School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran

b Research Institute of Petroleum Industry, Tehran, Iran

a b s t r a c t

Mass transfer in gas–liquid systems has been signiﬁcantly enhanced by recent developments in nanotechnology.

However, the inﬂuence of nanoparticles in liquid–liquid systems has received much less attention. In the present

study, both experimental and theoretical works were performed to investigate the inﬂuence of nanoparticles on the

mass transfer behaviour of drops inside a pulsed liquid–liquid extraction column (PLLEC). The chemical system of

kerosene–acetic acid–water was used, and the drops were organic nanoﬂuids containing hydrophobic SiO2 nanopar-

ticles at concentrations of 0.01, 0.05, and 0.1 vol%. The experimental results indicate that the addition of 0.1 vol%

nanoparticles to the base ﬂuid improves the mass transfer performance by up to 60%. The increase in mass trans-

fer with increased nanoparticle content was more apparent for lower pulsation intensities (0.3–1.3 cm/s). At high

pulsation intensities, the Sauter mean diameter (d32 ) decreased to smaller sizes (1.1–2.2 mm), leading to decreased

Brownian motion in the nanoparticles. Using an analogy for heat and mass transfer, an approach for determining

the mass diffusion coefﬁcient was suggested. A new predictive correlation was proposed to calculate the effective

diffusivity and mass transfer coefﬁcient in terms of the nanoparticle volume fraction, Reynolds number, and Schmidt

number. Finally, model predictions were directly compared with the experimental results for different nanoﬂuids.

The absolute average relative error (%AARE) of the proposed correlation for the mass transfer coefﬁcient and effective

diffusivity were 5.3% and 5.4%, respectively.

© 2014 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keywords: Pulsed column; Nanoﬂuid drops; Mass transfer model; Effective mass diffusivity; Extraction efﬁciency

simple diffusion-based theories. The enhanced diffusion in

Nanoﬂuids are stable suspensions of nanometre-sized par- nanoﬂuids can therefore be utilised to improve mass transfer

ticles in conventional liquids. One advantage of nanoﬂuids in unit operations.

is their improved heat transfer: it has been experimentally To determine the degree of thermal conductivity enhance-

shown in many instances that nanoﬂuids have higher ther- ment in nanoﬂuids, Krishnamurthy et al. (2006) experimen-

mal conductivities and improved convective heat transfer in tally observed the diffusion of a dye droplet in a water-based

comparison to host liquids (Chen et al., 2008; Ding et al., 2010; nanoﬂuid and calculated the effective mass diffusivity of the

Garg et al., 2009; Li and Peterson, 2006; Wen et al., 2006). In dye in both the water and nanoﬂuid. The investigation showed

addition to enhancing heat transfer, suspended nanoparticles that the suspended nanoparticles remarkably increase the

have been found to improve mass transfer processes inside mass transfer of the dye. Olle et al. (2006) measured the oxy-

binary nanoﬂuids. Because convection and mass transfer are gen absorption rate in the presence of colloidal dispersions of

similar processes, several authors (Feng et al., 2005; Wen et al., magnetite (Fe3 O4 ) nanoparticles coated with oleic acid. Olle

2005; Olle et al., 2006) have proposed models that postulate et al. determined that this nanoﬂuid improves the gas–liquid

that nanoscale convection induced by the Brownian motion oxygen mass transfer coefﬁcient by more than 1.6-fold and

of the nanoparticles causes enhanced mixing. This increased the kL a value by up to 6-fold at nanoparticle concentrations

∗

Corresponding author. Tel.: +98 21 61112213; fax: +98 2166967788.

E-mail address: hbahmany@ut.ac.ir (H. Bahmanyar).

Received 30 June 2013; Received in revised form 17 December 2013; Accepted 18 January 2014

0263-8762/$ – see front matter © 2014 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

http://dx.doi.org/10.1016/j.cherd.2014.01.024

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

ARTICLE IN PRESS

2 chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx

Nomenclature

Subscripts

a interfacial area, m2 /m3 c continuous phase

A pulsation amplitude, cm d dispersed phase

C solute concentration in the dispersed phase, p particle

kg/m3 s solid

C0 initial concentration of solute in the dispersed ad auxiliary diffusivity

phase, kg/m3 bf base ﬂuid

C* equilibrium concentration of solute in the dis- nf nanoﬂuid

persed phase, kg/m3

d droplet diameter, m

d32 Sauter mean diameter of droplets, m below 1 vol% in an agitated, sparged reactor. Interestingly, the

di the ith group droplet diameter, m enhancement in kL a levelled off at a nanoparticle volume frac-

Dd molecular diffusivity of transferred component tion of approximately 1% (v/v).

in the dispersed phase, m2 /s Although the mechanism of the enhanced mass transport

DE effective diffusivity in Handlos–Baron equa- from the suspended nanoparticles is still not well understood,

tion, Eddy diffusivity in the Temos equation, some existing work assumed that the irregular Brownian

m2 /s motion of the nanoparticles is one of the main factors con-

DOE overall effective diffusivity, m2 /s tributing to the enhancement of mass transport (Xuan et al.,

E mass transfer enhancement 2003; Prasher et al., 2005).

E0 Eotvus number, 1 s–1 In another study, Lee et al. (2010) found that the absorption

E0c Eotvus number when the droplet has critical rate of ammonia by nanoﬂuids is higher than that of conven-

diameter pulsation frequency, 1 s–1 tional ﬂuids. Lee et al. also showed that despite the higher

f pulsation frequency, s−1 thermal conductivity of a CNT-nanoﬂuid compared to a Al2 O3 -

fV fractional segmental volume of drop which is nanoﬂuid, the absorption performance of the CNT-nanoﬂuid

stagnant is not better than that of the Al2 O3 -nanoﬂuid. Lee et al. spec-

g gravity acceleration, m2 /s ulated that this behaviour was due to the higher aspect ratio

H effective height of the column, cm of CNTs, which leads to less Brownian motion in comparison

k the dimensionless number in Eq. (14), =E0c /6 to spherical Al2 O3 nanoparticles.

kd dispersed phase mass transfer coefﬁcient, m/s To date, the use of nanoﬂuids to enhance mass trans-

kH empirical constant of Eq. (12), which varies fer has dealt only with gas–liquid systems. However, little

between 0 and 1 is known regarding the effects of nanoparticles on the mass

KB Boltzmann constant, =1.3807 × 10−23 J/K transfer behaviour of droplets in liquid–liquid systems. Such

L column height, m phenomena are examined both experimentally and theo-

ni the number of the ith group droplets retically in this study using hydrophobic SiO2 nanoparticles

Nu Nusselt number, dimensionless with droplet ﬂows in a pulsed liquid–liquid extraction col-

PI pulsation intensity, cm/s umn (PLLEC). The decision to use a pulsed column in this

Pr Prandtl number, dimensionless study was based on the column’s ability to offer a more robust

Qc continuous phase ﬂow rate, m3 /s medium for the investigation of nanoparticle inﬂuence on

Qd dispersed phase ﬂow rate, m3 /s droplet behaviour. Experimental and computational investi-

the modifying coefﬁcient of the transferred gations were conducted to study the effect of nanoparticles on

component molecular diffusivity due to the the mass transfer characteristics of nanoﬂuid drops. Employ-

internal circulations ing the analogy between heat and mass transfer, an approach

Re Reynolds number, dimensionless for determining the effective mass diffusivity and mass trans-

Sc Schmidt number, dimensionless fer coefﬁcient was suggested and discussed. The ﬁnal aim of

Sh Sherwood number, dimensionless this study was to clarify how nanoparticles can be utilised

t resident time of the dispersed phase in column, to improve mass transfer in liquid–liquid unit operations.

contact time, s Numerical analysis supports the concept that the Brownian

T temperature, K motion of the nanoparticles increases the internal circulation

Vt terminal velocity of a droplet, m/s of droplets. In this study, the enhanced diffusion coefﬁcient

has been predicted, and its effect on mass transfer has been

Greek symbol calculated. These ﬁndings have direct implications for sep-

interfacial tension, N/m aration technology and are promising for the application of

nanoparticle volume fraction nanoﬂuids in other liquid–liquid contact devices, such as

density, kg/m3 rotary disc contractors and packed columns.

˛ thermal diffusivity, m2 /s

dynamic viscosity, Ns/m2 2. Experiments

v kinematic viscosity, m2 /s

ratio of the dispersed phase viscosity to contin- A schematic diagram of the experimental setup used in this

uous phase viscosity study is presented in Fig. 1. The column consisted of a 70 cm

ϕ dispersed phase hold-up long vertical Pyrex tube with an inner diameter of 90 mm.

The column contained 10 perforated stainless steel plates

regularly spaced 5 cm apart and was supported on an 8 mm

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

ARTICLE IN PRESS

chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx 3

Fig. 1 – A schematic diagram of the pulsed liquid–liquid extraction column used in this study.

diameter central rod. Two separating chambers were present Evaluation of the nanoﬂuids’ stability was carried out by

on either side of the column. Holes 3 mm in diameter were the sedimentation method using UV–vis spectrometry, which

arranged in a 6 mm triangular pitch at each plate, providing a proved that the nanoﬂuids remained stable for several days

nominal free fraction area of 0.20 (Khoobi et al., 2013). Pulsa- (Khoobi et al., 2013). Despite this observation, nanoﬂuids were

tion was obtained via a newly designed pulsator, consisting of applied to the pulsed column shortly after their preparation.

an air compressor; a 3-way, 2-position direct-acting solenoid At the end of each test run, the absence of the nanoparticles

valve; and a microcontroller (AVR-8051) as a programmable in the continuous phase was ensured using UV–vis spectrom-

controller unit (PCU). The PCU was capable of periodically etry. The amorphous fumed hydrophobic silica powders are

energising the solenoid valve to allow ﬂow of the compressed highly pure, with nanoparticles in the range of 5–30 nm and a

air for an adjustable period of time, pulsating the ﬂow along density of 2200 kg/m3 . Their surfaces have been modiﬁed by

the column with an intensity of 0.3–2.3 cm/s. The PCU pro- OSi(CH3 )2 groups. The densities of water and kerosene are

vided an adjustable time-off in the range of 0.020–65.535 s. 996 and 800 kg/m3 , respectively. In addition, the viscosities of

This pulsator, which was speciﬁcally designed and built for the mentioned liquids are 1.0 and 1.67 mPa s, respectively.

this type of research, offers the advantage of 1 ms accuracy

in pulsation time, does not require maintenance typical of

3. Analysis

mechanical pump pulsators, and does not suffer from the lim-

itations of airlift pulsators. Two ﬂowmeters were employed

to supply and monitor the ﬂow rates of the continuous and

3.1. Nanoﬂuid properties in modelling

dispersed phases.

The availability of correlations for various nanoﬂuid prop-

Both the continuous and dispersed phases were mutu-

erties is critical when solving the governing conservation

ally saturated before being used in the experiments. At the

equations. However, generating a speciﬁc correlation for each

beginning of each test run, the continuous phase was ini-

type of nanoﬂuid is cumbersome. To address this issue, Vajjha

tially allowed into the column from the top, which was ﬁlled

and Das (2010) carefully analysed all of the data from Namburu

to the speciﬁed height (valve 4, H = 44.5 cm). The dispersed

et al. (2007a,b) and Sahoo et al. (2009) to develop a gen-

phase was then fed into the column via a glassy nozzle (inner

eral correlation for the nanoﬂuid viscosity. A correlation was

diameter 2 mm) from the bottom. The ﬂowmeters were then

derived which expressed the viscosity in a non-dimensional

ﬁxed to the speciﬁed ratio (Qc /Qd = 1.2). The pulsation ampli-

form, valid for nanoﬂuids containing CuO, Al2 O3 , and/or SiO2

tude and frequency were adjusted to the desired values by

nanoparticles.

setting the time-on and time-off periods in the PCU. Acetic

acid (5 vol%) was added to the saturated kerosene to pro-

duce the base ﬂuid for all of the systems under investigation, nf

= A1 e(A2 ) (1)

as listed in Table 1. The nanoﬂuids were prepared by dis- bf

persing SiO2 nanoparticles supplied by the Wacker–Chemie

Company (HDK H18 with hydrophobicity of 18) into the base In the generalised correlation above, A1 and A2 are constants

ﬂuid. All of the nanoﬂuid samples were subjected to ultra- and are not functions of nanoparticle volume fraction (),

sonication (Heilscher ultrasound generator) for 1 h to ensure unlike previous correlations (Sahoo et al., 2009). The values of

proper nanoparticle dispersion. constants A1 and A2 are given for SiO2 nanoparticles in Table 2.

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

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4 chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx

System’s name Continuous phase Dispersed phase c (kg/m3 ) d (kg/m3 ) c (mPa s) d (mPa s) Interfacial tension

(mN/m)

W-NF1 SW SK + AA + 0.01 vol% HDK H18 996 826 0.87 1.97 47.2

W-NF2 SW SK + AA + 0.05 vol% HDK H18 996 881 0.87 2.50 48.1

W-NF3 SW SK + AA + 0.1 vol% HDK H18 996 951 0.87 3.37 49.0

SW, saturated water; SK, saturated kerosene; AA, 0.05 vol% acetic acid; and NF, nanoﬂuid.

The effective mass density of the nanoﬂuid eff is calcu- when the experimental data (ϕ, d32 , and Qd ) throughout the

lated according to mixing theory (Vajjha and Das, 2010) using height of column are available, as is the case in this work, the

the following equation: contact time between two phases can be obtained using Eq.

(5). The mass transfer coefﬁcient (Kd ) along the column height

eff = (1 − )bf + s (2) can then be obtained using Eqs. (3) and (4).

where bf and s are the mass densities of the base ﬂuid and 3.3. Determination of the hydrodynamic

the solid nanoparticles, respectively. characteristics

3.2. Determination of the mass transfer characteristics To determine the drop size and hold-up, the pulsation inten-

sity in the column was varied while the mass ﬂux ratio was

The overall mass transfer of the dispersed or continuous phase kept constant. When performing these hydrodynamic exper-

is a fundamental parameter in liquid–liquid extractor design. iments, the system must be operated in a steady state. To

In this study, the mass transfer coefﬁcients were calculated ensure a steady state condition, the column was operated in

using a semi-empirical method. The mass balance for a drop recycle mode until no further changes in the phase interface

may be described by: could be detected. The drop sizes in the column were then

determined by taking digital photos of the column contents.

d The drop size was evaluated as the Sauter mean diameter as:

Kd = − ln(1 − E) (3)

6t 3

nd

where d32 = i i2 (6)

ni di

C0 − C

E= (4) where ni is the number of corresponding droplet diameters

C0 − C∗

and di is the measured droplet diameter.

C0 is the solute concentration in the primary drop (before con- Hold-up was determined by the displacement method. At

tact), C is the solute concentration at a speciﬁed height from the end of each test run, the inlet and outlet ﬂows were

the column bottom (44.5 cm for the setup in this work taken stopped simultaneously, and the dispersion was allowed to

from valve 4), and C* is the solute concentration of in equi- coalesce at the interface. The hold-up was then determined by

librium with the continuous phase. The solute (acetic acid) measuring the total volume and the dispersed phase volume

concentrations in the collected droplets (C) and the continuous as:

phase were determined by titration with a 0.1 M NaOH solution

Vd

and phenolphthalein as the indicator. At least three titrations ϕ= (7)

Vd + Vc

with a sampling volume of 10 mL were performed, and the

average value of the titrations was recorded. The uncertain- where Vd and Vc are the volumes of the dispersed and contin-

ties of the tests, including instrument and personal errors, uous phases, respectively.

were omitted. The solute concentration in equilibrium with

the continuous phase (C*) was determined using liquid–liquid 4. Theoretical predictions of mass transfer

equilibrium data for the ternary acetic acid–water–kerosene coefﬁcients

system. The relationship between contact time (t), dispersed

phase volumetric ﬂow rate (Qd ), and hold-up (ϕ) can be The overall mass transfer coefﬁcient of the dispersed or con-

described as follows (Treybal, 1990): tinuous phase is a fundamental parameter in pulsed column

design. Several equations have been presented in the liter-

Qd t

L= (5) ature for calculating the overall mass transfer coefﬁcient of

Sϕ

dispersed phase. These equations are generally based on three

theoretical models as presented in Table 3.

Table 2 – Constants of the viscosity correlation for The three mechanisms commonly used to determine the

nanoﬂuids containing SiO2 nanoparticles. mass transfer rates of solutes in drops are: molecular diffu-

A1 A2 Average particle Concentration sion in a stagnant spherical drop (Newman, Eq. (8)), laminar

size (nm) (%) diffusion with circulation induced by relative motion of a drop

and the continuous phase (Kronig and Brink, Eq. (9)), and eddy

1.092 5.954 20 0 < < 0.1

diffusion between internal toroidal streamlines (Handlos and

0.9693 7.074 50 0 < < 0.06

1.005 4.669 100 0 < < 0.06

Baron, Eq. (10)). The equations governing these mechanisms

are summarised in Table 3. Although small drops are often

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

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Table 3 – Previous equations for predicting the mass transfer correlation Kumar and Hartland (1999).

Models Expressions Remarks

−d

6 1 −4n2 2 Dd t

Newman Kod = ln exp (8) Molecular diffusion in stagnant

6t 2 n2 d2

−d

3 n=∞

n=1 64Dd t

drops

Kronig and Brink Kod = ln 2

An exp − n (9) Laminar diffusion with circulation

6t 8 n=1 d2

induced by relative motion of drop

and continuous phase

−d − n Dd tPe

Handlos and Baron Kod = ln 2 An exp (10) Eddy diffusion between internal

6t 128d2

n toroidal stream lines

subject to molecular diffusion rate control and large drops may where

exhibit Handlos–Baron behaviour, a transition between these V d

two mechanisms based on Reynolds, Weber, or other factors DE = 3.29 × 10−4 d i

d

does not appear to be reliable.

V d

Other investigators have presented various correlations

× 1 − exp −3.29 × 10−4 d i d

(17)

using the Newman equation with effective diffusivity instead d d

of molecular diffusivity (Dd instead of Dd ). These equations

are based on the Newman equation, but effective diffusivity Vi for Re 1 is given by:

is used to account for internal circulation of droplets. Effec-

tive diffusivity contains the effects of all known and unknown 2 + 3 1.45

Vi = 1− 0.5

Vt (18)

parameters that play an important role in calculating the exact 1 + (d d /c c ) Re0.5

value of mass transfer coefﬁcients. Some of the equations pre-

sented by these investigators for calculating are described while other models exist, most of them cannot be applied to

brieﬂy below: the present study because they have been determined for a

Steiner (1986) proposed calculating the modifying coef- speciﬁc column, solvent or other condition (Jie et al., 2005;

ﬁcient as a function of Reynolds and Schmidt number as Koncsag and Barbulescu, 2008).

follows:

5. Results and discussion

1
0.89

0.043 0.23

R = 1 + 0.177Re Sc (11)

1+ 5.1. Enhancement of mass transfer

This correlation is applicable when Re < 10. Hydrodynamic studies suggest that the column behaviour

Davies (1966) proposed a correlation in which the internal under near ﬂooding conditions is not stable: small changes

part of the droplet is divided into two sections: a section with to the operating conditions (e.g., feed ﬂow rates or pulsation

internal circulation and a stagnant section with molecular dif- intensity) lead to an over- or under-ﬂooded operation. In this

fusion: study, the experiments were designed for the PLLEC to operate

DOE

kH Vt d

under no ﬂooding conditions in accordance with prescribed

R= = fV + (1 − fV ) (12) operating conditions recommended in the literature (Godfrey

Dd 2048(1 + )Dd

and Slater, 1994). In analysing the data obtained from a PLLEC,

where fV is the fractional segment stagnant volume and kH is conventional pulsation intensity (PI), deﬁned as the product of

the impurity coefﬁcient and varies from 0 to 1. When kH = 0, pulsation frequency (f) and stroke length or pulsation ampli-

the system is completely pure. Conversely, when kH = 1, the tude (A), was used. The units of PI are cm/s.

system is completely impure.

PI = A · f (19)

Vt d

DE = (13)

2048(1 + ) Fig. 2 shows the enhancement of the mass transfer rate

with a nanoparticle addition for a mass ﬂux ratio of 1:2. The

0.098E0 −2.21 mass transfer rate signiﬁcantly increases with an increas-

fV = 1 − exp − , 6k = E0c (14) ing concentration of SiO2 nanoparticles. It was found that

k

the mass transfer rates for the nanoﬂuids were improved

E0c shows the start of internal circulation of droplets and is by 4–21%, 5–47% and 5–60% for 0.01, 0.05 and 0.1 vol%,

given by: respectively. This enhancement is likely due to turbulence

caused by Brownian motion of nanoparticles inside droplets

gd2

(Krishnamurthy et al., 2006). In particular, this enhancement

E0c = (15) was more signiﬁcant at a lower PI, an effect that may be

attributed to the larger drop size obtained at a lower PI. Con-

Temos et al. (1993) present the relationship between eddy versely, the decreased mass transfer enhancement observed

diffusivity and molecular diffusivity in a simple way: at a high PI could be explained by the reduced droplet size,

which leads to reduced turbulence.

0.44DE Moreover, a clear peak in the mass transfer rate was

R=1+ (16)

Dd observed for a pulsation intensity of 1.8 cm/s and a

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

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Fig. 2 – Extraction efﬁciency for all systems at PI’s of (a) 0.3, (b) 0.7, (c) 1.3 and (d) 1.8 cm/s; mass ﬂux ratio = 1.2.

nanoparticle concentration of 0.05 vol%, suggesting that the nanoparticles. Small drops are usually treated as rigid spheres

mass transfer rate may not improve above a certain PI (1.8 cm/s with negligible internal circulation; mass transfer inside the

in the present experiment). This peak could be due to the pro- drop is controlled by molecular diffusion (Newman model).

duction of small droplets at high PIs. Because small droplets Therefore, the average error of the Newman equation at

behave as rigid spheres, molecular diffusion governs the mass higher PIs, at which molecular diffusion governs the system,

transfer in the system. is less than the error at lower PIs.

Although the Handlos–Baron equation is more accurate

5.2. Comparison with previous models compared to the other available equations, an interesting

observation can be made when comparing different nanopar-

The mass transfer coefﬁcient (Kd ) was calculated for the vari- ticle contents and PIs. Having established that the Kd s

ous systems tested using the theoretical equations presented calculated using the Newman and Kronig–Brink equations

in Section 4. These results were then compared with the are strongly affected by nanoparticle presence, we expected

experimentally measured mass transfer coefﬁcients, and the a similar nanoparticle inﬂuence on the mass transfer coef-

absolute errors are presented in Table 4. ﬁcient calculated by the Handlos–Baron equation. However,

The Newman and Kronig–Brink equations underestimate such an inﬂuence was not observed and may be explained

the mass transfer coefﬁcient by 48% and 34%, respectively, by the theoretical background of the Handlos–Baron equation,

regardless of the nanoparticle concentration and pulsation which considers turbulent circulation in each drop in addition

intensity. This difference is likely because these models do to the circulation from Brownian motion of the nanoparti-

not consider circulation within the drop. Interestingly, the cles. In other words, the Handlos–Baron equation overpredicts

mass transfer coefﬁcient obtained from the Handlos–Baron the data because it is based on fully turbulent internal circu-

equation is on average 24% higher than the experimentally lations, a condition which is not reached in practice: drops

measured value. The Handlos–Baron equation therefore yields experience a transition state between laminar and fully turbu-

a more precise and accurate estimate of the mass transfer lent ﬂow. This suggests that the Newman equation is the most

coefﬁcient, likely due to the model’s consideration of turbulent proper equation for the modelling of mass transfer coefﬁcients

circulation within the drop. in the presence of nanoparticles.

It can also be observed that regardless of the chemical The mass transfer coefﬁcient in drops is a strong function

system, the absolute errors calculated from the Newman of drop size; therefore, the comparison between experimen-

and Kronig–Brink equations are larger for lower PIs (0.7 and tal dispersed phase mass transfer coefﬁcients and the results

1.3 cm/s) and lower at higher PIs (1.8 and 2.3 cm/s). The obtained from previous equations is shown in Fig. 3 as a func-

average absolute error calculated from the Newman model tion of drop diameter.

is approximately −66% at low PIs (PI ≤ 1.3 cm/s) and −24% at The results of Fig. 3 support the hypothesis that the

high PIs (PI ≥ 1.8 cm/s). In fact, higher PIs result in a smaller Brownian motion of the nanoparticles increases the internal

Sauter mean diameter and lesser Brownian motion of the circulation within drops. The experimental results are in good

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

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CHERD-1483; No. of Pages 11

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Table 4 – Calculated values for the mass transfer coefﬁcients, Kd × 105 (m/s), and percentage of errors.

PI (cm/s) d32 (mm) Experimental Newman Kronig and Brink Handlos and Baron

W-AA-K system

0.3 3.7 7.10 2.64 −63 3.20 −55 8.67 23.3

0.7 3.37 3.15 1.26 −60 1.77 −44 3.91 24.2

1.3 3.17 2.71 1.59 −41 1.89 −30 3.36 24.3

1.8 2.11 1.48 1.07 −28 1.25 −16 1.84 24.5

2.3 1.61 1.07 0.81 −24 0.92 −14 1.33 24.5

W-NF1 system

0.3 3.47 3.11 1.15 −63 1.76 −43 3.86 24.2

0.7 3.12 2.56 1.03 −60 1.54 −40 3.18 24.3

1.3 2.60 1.94 0.84 −57 1.28 −34 2.41 24.4

1.8 1.94 1.26 0.82 −35 0.94 −25 1.57 24.5

2.3 1.18 0.69 0.51 −27 0.53 −24 0.87 24.6

W-NF2 system

0.3 3.82 4.21 1.17 −72 1.65 −61 5.22 24.0

0.7 3.32 2.72 1.02 −62 1.42 −48 3.38 24.3

1.3 2.83 2.01 0.88 −56 1.21 −40 2.50 24.4

1.8 2.20 1.28 0.81 −37 0.95 −26 1.59 24.6

2.3 1.76 0.81 0.61 −25 0.69 −15 1.01 24.7

W-NF3 system

0.3 3.78 4.44 1.12 −75 1.58 −64 5.50 23.9

0.7 3.30 2.55 0.95 −63 1.30 −49 3.17 24.3

1.3 2.67 1.87 0.76 −59 1.19 −36 2.32 24.4

1.8 2.09 0.90 0.71 −21 0.77 −14 1.12 24.7

2.3 1.67 0.62 0.59 −5 0.65 6 0.77 24.7

agreement with the Handlos–Baron equation, while other cor- Similar to the parameters for the molecular diffusion, the

relations underpredict the mass transfer coefﬁcients of the effective Prandtl number (Pr) and Schmidt number (Sc) are

nanoﬂuids that were investigated in this study. There is no introduced for heat and mass transfer inside a nanoﬂuid with

signiﬁcant variation of mass transfer coefﬁcient between the effective viscosity vnf

experimental data and the values obtained from previously

published correlations for smaller drops. This agreement can nf nf

be attributed to the fact that the internal circulation within Prnf = and Scnf = (21)

˛nf Dnf

very small drops is negligible (Re < 1), and the mass transfer

mechanism within these drops is molecular diffusion (New-

man model). On the other hand, for a larger drop diameter, in It is assumed that the analogous functional relationship

which turbulent circulation occurs within the drop, the New- between temperature and concentration in the differential

man and Kronig–Brink equations fail to predict the dispersed equations for heat and mass transfer allows for the heat trans-

phase mass transfer coefﬁcient of the investigated nanoﬂuids. fer equation to be converted to a mass transfer equation by

This may be because these correlations assume molecular dif- simply replacing the Prandtl number with the Schmidt num-

fusion and laminar circulation inside the drops while ignoring ber and the Nusselt number (Nu) with the Sherwood number

Brownian motion of the nanoparticles. (Sh) (Eckert et al., 2001). The heat and mass transfer analogy

means that the Nusselt number for heat transfer and the Sher-

wood number for mass transfer inside a binary nanoﬂuid can

5.3. Predictive correlation for the effective diffusivity of

be described by Nunf = f (Renf , Prnf ) and Shnf = f (Renf , Scnf ).

nanoﬂuids by means of a heat and mass transfer analogy

An appreciation for the similarity between heat and mass

transfer can be gained using dimensional analysis.

Although enhancement effects in binary nanoﬂuids have been

For spherical nanoparticles, the Nusselt number may be

observed, no sophisticated theory has been established to

deduced from previous work (Xuan and Li, 2003):

describe mass transport process inside binary nanoﬂuids. It

is now acknowledged that the stochastic Brownian motion of

m m

suspended nanoparticles and induced microscopic convection Nunf = 2 + cm1 Renf2 Prnf3 (22)

of the ﬂuids around the nanoparticles are the two most impor-

tant factors for the enhancement of mass transport processes

in binary nanoﬂuids. where m3 is dependent upon the heat transfer mode of ﬂuid

One possible approach to determine the mass diffusivity of cooling or heating. The coefﬁcient c and the exponents m1 and

a binary nanoﬂuid involves the heat and mass transfer anal- m2 can be determined from the experimental data by a proper

ogy. The Reynolds number of a nanoparticle can be expressed data-reduction procedure.

as (Nagy et al., 2007) The analogy principle between heat and mass transfer

leads to the Sherwood number:

vp dp 1 18KB T

Renf = = (20)

nf nf dp Shnf = 2 + cm1 Rem 2 m3

nf Scnf (23)

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

ARTICLE IN PRESS

8 chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx

function of droplet diameter for the (a) W-NF1 (0.01 vol%),

(b) W-NF2 (0.05 vol%) and W-NF3 (0.1 vol%) systems.

around a sphere in the laminar ﬂow regime was described by

Bird et al. (2002).

With regard to heat transfer enhancement, the microcon-

vection of nanoparticles increases the macroscopic thermal

conductivity of nanoﬂuids. Similar to Prasher’s formula

(Prasher et al., 2006), the apparent thermal conductivity of

binary nanoﬂuids can be expressed as: Fig. 4 – Comparison of the experimental data with the

calculated values for the (a) W-NF1 (0.01 vol%), (b) W-NF2

(0.05 vol%) and W-NF3 (0.1 vol%) systems.

m m

knf = kf (1 + cm1 Renf2 Prnf3 ) (24)

By introducing the auxiliary diffusivity Dad , the effective

From the analogy of mass and heat transfer, Eqs. (22) and mass diffusivity of the binary nanoﬂuid can be expressed as:

(23), the apparent mass diffusion coefﬁcient of binary nanoﬂu-

ids can be derived: Dnf = D0 + Dad (26)

Dnf = Df (1 + cm1 Rem m3

nf Scnf )

2 (25)

tem (0.0 vol%) calculated at various PIs using the Newman

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

ARTICLE IN PRESS

chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx 9

Fig. 5 – Illustration of the inﬂuence of the pulsation intensity on the size of droplets.

equation, which is based on the continuity equation with As shown in Fig. 4, it is obvious that the previously

appropriate initial and boundary conditions. published correlations have relatively high average absolute

The main advantage of this approach is that the princi- errors (98%) when used to calculate mass transfer coefﬁcients.

pal effects of external forces (e.g., PI) and Brownian motion The coefﬁcients calculated from the correlation proposed by

from nanoparticles are taken into consideration in terms of D0 Steiner, Davis, and Temos et al. are much higher than the true

and Dad , respectively. Without these considerations, the exper- coefﬁcients. The Handlos–Baron equation shows less average

imental data could not be ﬁtted with acceptable accuracy. error than the other equations, but the average error (24%)

A comparison between Eqs. (25) and (26) yields of this equation is relatively high and unacceptable for pre-

cise design. In contrast, the ﬁgures indicate that the equation

proposed in this work can accurately estimate the dispersed

Dad = cn1 Rennf2 Scnf

n3

D0 (27)

phase mass transfer coefﬁcient. The dispersed phase mass

transfer coefﬁcient calculated with this model reproduces the

To develop a new predictive correlation for the effective experimental data with an average error of only 5.3%. Table 5

mass diffusivity of nanoﬂuids, experimental data were ﬁt to shows the average error (%AARE) of the predicted Kd s for pre-

Eq. (27) to determine the curve ﬁt coefﬁcients c, n1 , n2 and n3 vious and present correlations. The %AARE for the N data is

using least squares, yielding Eq. (28): calculated as follows:

1 model − experiment

N

Dad = 16500.203 Re0.039 Sc−1.064 (28)

%AARE =

N

experiment

× 100 (29)

i=1

The calculated values of the effective diffusivity were then

used in Eq. (8) to calculate the mass transfer rate enhance- The effective mass diffusivity is also calculated by the cor-

ment. The overall mass transfer coefﬁcients of the dispersed relation presented above, and the results are shown in Fig. 6 .

phase were then calculated using Eq. (3).

It should be noted that the Schmidt number physically

relates the relative thickness of the hydrodynamic layer and

the mass transfer boundary layer. The negative power for

the Schmidt number in Eq. (28) may be ascribed to liquid

molecular layering and suggests that the liquid–nanoparticle

interface decreases the mass boundary layer and lowers the

effective mass diffusivity. This view is in line with the works

of some investigators (Shenogin et al., 2004a,b; Nan et al.,

2003; Gao et al., 2007), who have ascribed the adverse effect of

liquid–nanoparticle interface to Kapita interfacial resistance.

In Fig. 4, the experimentally determined dispersed phase

overall mass transfer coefﬁcients are compared with theo-

retical models and the proposed model for three chemical

systems with different nanoparticles contents of 0.01, 0.05 and

0.1 vol%, corresponding to W-NF1 , W-NF2 and W-NF3 , respec-

tively.

Overall, Kd decreases with increasing PI. Based on experi-

mental observations, the mean drop diameter decreases with

increasing PI, leading to a longer drop residence time. How-

ever, as expressed by Eq. (3), Kd decreases with both effects Fig. 6 – Comparison of the experimental Dnf with present

(Fig. 5). and previous equations.

Please cite this article in press as: Bahmanyar, A., et al., Mass transfer from nanoﬂuid drops in a pulsed liquid–liquid extraction column. Chem.

Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2014.01.024

CHERD-1483; No. of Pages 11

ARTICLE IN PRESS

10 chemical engineering research and design x x x ( 2 0 1 4 ) xxx–xxx

Table 5 – The %AARE of the predicted Kd for previous and present correlations.

System’s name Eq. (28) Eq. (8) Eq. (9) Eq. (10) Eq. (11) Eq. (12) Eq. (17)

This New- Kronig Handlos Steiner Davis Temos

work man and Brink and Baron

W-NF2 4.0 50.4 38.0 24.4 113.4 263.6 137.2

W-NF3 6.3 44.6 33.8 24.6 115.7 263.4 129.7

dict mass transfer enhancements is shown in Fig. 7. This

ﬁgure depicts the variation of the mass transfer enhancement

at various PIs compared to experimental data for all chemi-

cal systems. According to the average of the residuals, very

good agreement between the experimental data and corre-

lated curves is achieved for all chemical systems.

6. Conclusions

drops were investigated experimentally in a pulsed

liquid–liquid extraction column. Different pulsation intensi-

ties were maintained for ﬁxed mass ﬂow rates of dispersed

(Qd ) and continuous (Qc ) phases (with ratio Qc /Qd = 1.2). Mass

transfer occurred from the dispersed to the continuous

phase. The experimental results showed that the suspended

nanoparticles remarkably increase the mass transfer per-

formance of the base ﬂuid. The addition of 0.1 vol% silica

particles to kerosene enhanced the mass transfer rate by 60%.

A new correlation was proposed to calculate the effective

mass diffusivity in terms of the nanoparticle volume fraction,

the Reynolds number, and the Schmidt number. It was shown

that the mass transfer coefﬁcients calculated using this

correlation agreed well with the experimentally determined

values. Compared with other theoretical models that are

available in the literature, the model presented here displays

higher accuracy and precision.

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