Beruflich Dokumente
Kultur Dokumente
Department of Biological Systems Engineering, University of Wisconsin, Madison, 460 Henry Mall, Madison, WI 53706, United States
Department of Food Science, University of Wisconsin, Madison, 1605 Linden Drive, Madison, WI 53706, United States
a r t i c l e
i n f o
Article history:
Received 22 January 2012
Received in revised form 27 February 2012
Accepted 1 March 2012
Available online 20 March 2012
Keywords:
Lactose
Cooling crystallization
Metastable zone
Computational uid dynamics
Secondary nucleation
Encrustation
a b s t r a c t
In the dairy industry, lactose crystallization during rening typically generates a large number of nes
(<100 lm), which greatly reduces the efciency of downstream processes. To overcome this problem,
a strategy to minimize nes production was developed. On lab scale units, lactose crystals were produced
from three crystallizers (draft-tube bafed, anchor and paddle) operated with three cooling proles (at
different region inside metastable zone (MSZ)). Computational uid dynamics was used to simulate
the ow prole. Among all combinations investigated, anchor crystallizer (lowest shear) operated at slow
cooling rate (in upper MSZ) produces the largest crystals with minimal nes. Then, the design strategy
was applied in industrial scale crystallizer. The 13 h cooling prole created for operation in the medium
MSZ region successfully produced crystals with 28% less nes than the typical process. Therefore,
depending on the crystallizer design and operational region (in MSZ), production of nes can be
minimized.
2012 Elsevier Ltd. All rights reserved.
1. Introduction
Lactose is produced from whey permeates obtained after the
production of cheese and/or whey proteins. The three main steps
in lactose production are concentration, crystallization and separation. The concentration process involves the evaporation of water
in whey permeate to increase lactose concentration. Concentrated
whey permeate has about 6570% total solids, with about 80% of
the total solids as lactose. The mixture is then cooled during the
crystallization process where the lactose is separated as a-lactose
monohydrate crystal. Crude/food grade lactose is obtained after
two stages of centrifugation, and nal drying. Pharmaceutical
grade lactose is produced by a subsequent rening process, which
includes a series of washing, evaporation, drying and centrifugation steps to remove trace impurities.
Among all processing steps, crystallization is the most important separation step, but the crystallization process in the dairy
industry is far from optimized. The lling of the tank takes about
6 h, followed by gradual cooling and crystallization that lasts for
1418 h, which means the crystallization process lasts for 20
24 h (Shi et al., 2006). The process is usually carried out in a large
Abbreviations: MSZ, metastable zone; ML, metastable limit; MSZW, metastable
zone width; CFD, computational uid dynamics.
Corresponding author at: 1605 Linden Drive, Madison, WI 53706, United States.
Tel.: +1 608 263 1965; fax: +1 608 262 6872.
E-mail address: rwhartel@wisc.edu (R.W. Hartel).
1
Current address: Solae LLC, 4300 Duncan Avenue, St. Louis, MO 63110, United
States.
0260-8774/$ - see front matter 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jfoodeng.2012.03.003
(a)
(b) 80
Temperature (oC)
70
UNDERSATURATED
ZONE
60
50
LABILE
ZONE
40
30
Extrapolated T
TD
D
0.5% Tr
20
1% Tr
Industrial operation
10
0.1
643
0.2
0.3
0.4
0.5
0.6
This study was split into four parts. The rst three parts were
lab scale studies (Sections 2 and 3), while the last part involved
industrial verication and plant trials (Section 4). For the lab scale
studies, lactose crystallization experiments with three distinct
cooling proles were rst conducted using three crystallizer
types/impellers with different ow proles. Then, a model capable
of predicting the concentration prole according to the cooling
prole and initial lactose solution concentration was developed. Finally, the uid ow proles were analysed via CFD simulations.
2.1. Crystallizer design
2) The other two reference lines, 0.5% and 1% DTr, indicate the
temperatures at different levels of transmittance change
(DTr) (via spectroscopy test) when lactose solution was
cooled at 1 C/min. Higher changes in transmittance (relative to the seeded lactose solution) suggests the presence
of higher numbers of nuclei in the solution and, thus, higher
extent of secondary nucleation. The upper ML, dened by
the region between solubility and 0.5% DTr or 1% DTr lines,
have low or medium levels of secondary nucleation,
respectively.
Typical operating conditions for an industrial lactose rening
operation (Shi et al., 2006) are also shown in Fig. 1b. The bulk of
the operation operates in the lower ML between forced crystallization and the supersolubility lines, which is a region prone to secondary nucleation under agitated conditions. Therefore, commercial
operating conditions result in the production of lactose crystals
with wide range of size and numerous small crystals (Shi et al.,
2006), as shown in Fig. 1a. In short, for a seeded crystallization process, the ideal operating region would be the upper metastable region, which is characterized by the area between the solubility
and the TD, 0.5% DTr or 1% DTr lines, depending on the tolerance
to the extent of secondary nucleation.
In addition, uid mixing during the crystallization process is
also important in all aspects of transport properties, including
momentum, energy and mass. A few areas of concern for momentum transport include the homogeneity of crystal slurry, secondary
In this study, three crystallizers with different types of impellers, shown in Fig. 2, were used. The rst design (Fig. 2a) was a
draft tube bafe (DTB) crystallizer. It consisted of a tall form
250 ml beaker, a polycarbonate draft tube bafe set, and a three
blade propeller attached to a stainless steel shaft. The crystallizer
was placed in a water bath (Haake DC30) and the temperature of
the crystallization process was controlled by the bath temperature.
The draft tube bafe system was constructed so that both mother
liquor and suspension were well mixed. This system allowed axial
ow (of solution) inside the crystallizer: ow was down inside the
draft tube and up in the annular region. However, a minimum rotational speed of 440 rpm was required to suspend the crystals,
resulting in signicantly higher shear rate (around the impeller region) compared to the other two designs.
The second and third designs had close-clearance impellers,
with diameters nearly the same size as crystallizer tank diameter
to provide macro-scale blending of liquids at low shear (Paul
et al., 2004). The clearance between the impeller and the crystallizer (bottom and side) wall was ca. 3 mm. Due to the close clearance, the rotational motion of the impeller sweeps the wall and
prevents build-up of encrusted crystals on the wall. In addition,
this also improves heat transfer through the jacket.
The anchor crystallizer (Fig. 2b) consisted of a tall form 250 ml
jacketed beaker and an anchor stirrer. The temperature of the crystallization process was controlled by the circulating water bath
(Thermo Electron Neslab RTE7) connected to the jacketed beaker.
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speed
95 rpm
speed
440 rpm
speed
110 rpm
Baffle
Draft
tube
Propeller
Total Volume
= 206 ml
Total Volume
= 206 ml
(b)Anchor
Total Volume
= 300 ml
(c) Paddle
The paddle assembly conguration (Fig. 2c) was similar to the anchor stirrer, with additional two-blade propellers at the top and
bottom of the assembly. This crystallizer consisted of a 350 ml beaker and the paddle assembly. Similar to the DTB crystallizer, the
paddle crystallizer was placed in the same water bath (Haake
DC30). The working volumes of the three crystallizers were 206,
206 and 300 ml, respectively. The three crystallizers were selected
to represent different mixing proles and impeller designs, which
can be further examined through CFD simulations.
75
70
Temperature (o C)
65
60
55
50
45
40
35
30
25
0
10
12
14
16
18
20
22
24
Time (hr)
Fig. 3. Three cooling proles investigated (SLOWC, MEDIUMC and FASTC are
cooling proles with cooling rates of 0.031, 0.055 and 0.43 C/min,
respectively).
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Lactose crystals were produced as cooling progressed. The concentration of the lactose solution was measured following every
10 C drop in temperature. For this measurement, a small volume
(1 ml) of lactose slurry was rst ltered through a Whatman
GD/X syringe lter. The refractive index of the ltrate was measured (refractometer, Bausch and Lomb) and converted into lactose
concentration using pre-calibrated standard curve. At the end of
the cooling cycle, the crystallizer was emptied and the lactose crystals were separated by vacuum ltration (Whatman No. 42 lter
paper, 2.5 lm). The crystals were washed with 2-propanol (nonsolvent) and dried overnight in a 60 C oven. The crystal size distribution (CSD) was measured by laser diffraction via Malvern MasterSizer 2000 (Wong et al., 2010). In addition, the crystal shape
characteristic was examined by microscope (Nikon Labophot-2)
with 40 magnication.
The encrustation amount (g) and yield (g) were also measured.
Encrustation is dened as the coating/scaling of lactose crystals on
the surface of the crystallizer assembly (wall, bafes, and draft
tube). To measure the level of encrustation, the emptied crystallizer (after vacuum ltration of the slurry) was dried in a 60 C
oven overnight and the weight of encrusted lactose crystals measured. The yield of the crystallization process was calculated by
two approaches. The recovery percentage (Eq. (1)) denotes the ratio of lactose crystals produced and the amount of lactose initially
present in the solution. This is the approach commonly used in the
lactose rening industry.
Recovery %
Experimental yield g
initial mass of lactose in solution @t 0g
V I 1 C I V F 1 C E 0:05 M crystal
Theoretical yield %
Experimental yield g
100
Mcrystal M seed g
dx1
dx3
0:05
dt
dt
dx2
dx3
0:95
dt
dt
100
1
Theoretically, the maximum yield (Mcrystal) is limited by the saturation concentration of lactose (Cs) at the nal cooling temperature (TF). The lactose crystallization process is dened as:
dx3 qpNGx24
dt
2
Lactose
H2O
Initial
Mseed
Final
Mcrystal
(Equilibrium
+ Mseed
@ TF)
Used
VI CI VF CS VI (1 CI) VF (1 CS)
Here, VI and VF are the initial and nal volumes (ml) of the lactose solution. CI and CS are the initial and saturation (equilibrium at
TF) concentrations (g lactose/ml solution) of the lactose solution. Cs
can be calculated from (Eq. (2)) (Visser, 1982). Mseed is the mass of
seed added initially (=25 mg). Mcrystal is the maximum yield (g) of
crystals if the system achieves equilibrium at TF.
Cg
V I C I V F C E 0:95 Mcrystal
Mass balance of water,
11:4
dN
B 1:2 1018 eRT273 S 11:5 x3 =a2
dt
10
C
C s FK m C C s
F exp
2374:6
4:5683
Tk
K m 0:002286T 2:6371
11
75
Modeled
Experimental (Anchor)
Experimental (DTB)
Experimental (Paddle)
65
Temperature (oC)
646
55
45
35
12
25
0.2
13
0.3
0.4
0.5
0.6
Given the cooling proles (Fig. 3), all equations were solved
simultaneously by the ODE solver in Matlab R2008a to predict solution concentration and yield as function of time and temperature.
Modeled
Experimental (Anchor)
Experimental (DTB)
Experimental (Paddle)
ND2 q
45
25
0.2
14
Here, N is the impeller speed (rev/s) and D is the impeller diameter (m). For all crystallizers, the modied Reynolds numbers (Re)
were greater than 5000, which indicated that all ows were in the
turbulent regime. Thus, the Reynolds stress model (RSM) (Deen,
1998) was used to model the relationship between the turbulent
uxes and the smoothed eld variables.
The cooling prole for FASTC (Fig. 3) was used for the CFD simulation. The prole was implemented as temperature boundary
conditions to the side and bottom wall of the crystallizers. The time
step size for the unsteady simulation was 60 s, and the total number of time steps was 130, which was equivalent to a total simulation time of 130 min (2.17 h).
55
35
0.3
0.4
0.5
0.6
75
Modeled
Experimental (Anchor)
Experimental (DTB)
Experimental (Paddle)
65
Temperature (oC)
Re
Temperature (oC)
65
55
45
35
25
0.2
0.3
0.4
0.5
0.6
From Fig. 4, the concentration proles predicted from the crystallization model were close to the experimental proles at all
cooling rates for the anchor and paddle crystallizers even though
crystallization kinetics were predicted based on the FASTC cooling
prole. This suggests that the kinetic models used here adequately
t lactose crystallization kinetics over a broad range of conditions.
SLOWC
75
MEDIUMC
FASTC
Temperature (oC)
65
55
Increased
cooling
time
45
Increased
extent of
secondary
nucleation
35
25
0.2
0.3
0.4
0.5
0.6
647
648
Table 1
Experimental yield and encrustation amount from all crystallizers at different operating conditions.
Operating conditions
DTB crystallizer
SLOWC
MEDIUMC
FASTC (Tf = 27 C)
0.18
0.43
1.61
0.20
0.49
1.82
80.31
76.20
48.69
Anchor crystallizer
SLOWC
MEDIUMC
FASTC (Tf = 25 C)
78.80
74.29
54.33
90.34
85.17
60.68
1.50
2.51
2.42
Paddle crystallizer
SLOWC
MEDIUMC
FASTC (Tf = 27 C)
82.66
82.04
39.33
94.77
94.06
44.38
1.95
1.79
3.93
Fig. 7. Crystal size distribution of crystals obtained from the draft tube with bafes
(DTB) crystallizer at three operating conditions.
Fig. 8. Crystal size distribution of crystals obtained from the anchor crystallizer at
three operating conditions.
Fig. 9. Crystal size distribution of crystals obtained from the paddle crystallizer at
three operating conditions.
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Draft tube
baffle
(DTB)
Crystallizer
Anchor
Crystallizer
Paddle
Crystallizer
Fig. 10. Microscopic images of the lactose crystals obtained from different crystallizers under different operating conditions.
Fig. 11. Path lines plots (colored by velocity (m/s)) of mass-less particles released from plane y = 0 for all crystallizers (Step size = 0.005 m, number of steps = 200, equivalent
to a tracked distance of 1 m). (For interpretation of the references to colour in this gure legend, the reader is referred to the web version of this article.)
During the crystallization process, the driving force (supersaturation) required for the production of crystals is created by cooling.
The mixing proles will have an impact on the temperature and,
thus, the local supersaturation prole inside the crystallizers (Tung
et al., 2009). The simulated temperature proles at 1 h into the
cooling prole for FASTC operation are shown in Fig. 13. Due to
the presence of axial ow prole, the temperatures were mostly
uniform in DTB and paddle crystallizers. The highest average temperature was found inside the anchor crystallizer, where the heat
transfer from the center of the crystallizer to the wall is the slowest. Note that, the maximum temperature difference between the
wall and the center was less than 0.4 C for any of the crystallizer
congurations.
650
Fig. 12. Axial velocity (m/s) prole at the center plane of all crystallizers.
Fig. 13. Temperature distribution (1 h into the cooling cycle with FASTC operation) at the cross sectional plane (x = 0 or y = 0) of all crystallizers.
2004; Soos et al., 2008; Tung et al., 2009; Wong et al., 2010). In
general, the rate of secondary nucleation, which in turn determines
the number of nuclei formed, increases following shear treatment.
In a stirred tank, the high shear rates are generated in the immediate vicinity of the impeller (Paul et al., 2004). Fig. 15 shows the
contours of wall shear stress on the impeller assembly for each
crystallizer. The wall shear stress is dened as the force acting
tangential to the surface due to friction. It is proportional to the
velocity (gradient) parallel to the wall and, thus, the highest shear
stresses are found at the tips of the impellers. Among all crystallizers, the highest wall shear stress was observed in the propeller of
DTB crystallizer (Fig. 15a), since it had the highest rotational speed.
The lowest shear stress was found in the anchor crystallizer
(Fig. 15b). Although the paddle impeller had an intermediate level
of shear stress, it had the highest surface area of high shear stress
zones (non-blue region) (Fig. 15c). That means there will be higher
probability of (high shear) collisions between the lactose slurry
and the paddle impeller assembly.
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Fig. 14. Velocity (m/s) contour plot in the lower velocity range (00.01 m/s) of the DTB crystallizer (All colored zones are prone to encrustation).
Fig. 15. Wall shear stress (Pa) on the impeller assembly of all crystallizers.
Table 2
Flow properties of all crystallizers (The cumulative volume fraction (%) of nes was calculated as the sum of the volume fraction (%) of all crystals of size less than 100 lm).
DTB crystallizer
Anchor crystallizer
Paddle crystallizer
440
0.58
15.71
95
0.25
4.83
110
0.38
18.77
3.53
2.31
50.39
4.41
6.31
21.07
17.80
18.36
18.59
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Fig. 16. CFD analysis on Industrial scale crystallizer (a) Path lines plot of mass-less particles released from plane y = 0; (b) Wall shear stress (Pa) on the impeller assembly of
the crystallizers (c_ is the volume average shear rate).
Fig. 17. Proposed and existing industrial cooling and concentration proles (The proposed (13 h) prole is proposed by establishing a cushion of 1 C higher than the
concentration prole of 0.5% DTr).
4. Industrial validations
From the lab scale (200300 ml) study, a good understanding
of the crystallizer designs, and the appropriate regions of operation
were established with model lactose in water solution systems.
However, in the dairy industry, lactose is produced in an industrial
scale crystallizer (2.6 107 ml) from whey permeate that
contains other components (e.g., residual whey protein, minerals,
riboavin, etc.). To verify the applicability of this study in industrial
653
(b)
(a)
Typical process
13 hr plant trial
Fig. 18. (a) Polarized light microscope images; (b) Cumulative crystal size distribution (CSD) of the lactose crystals obtained from 13 h industrial trial (The typical process is
representative of the current industrial operation with 14 h cooling prole).
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