Numerical investigation of the de-agglomeration mechanisms of ne

powders on mechanical impaction

Z.B. Tong
a
, S. Adi
b
, R.Y. Yang
a,n
, H.K. Chan
b
, A.B. Yu
a
a
Labarotary for Simulation and Modelling of Particulate System, School of Materials Science and Engineering, University of New South Wales, Sydney,
NSW 2052, Australia
b
Faculty of Pharmacy, University of Sydney, NSW 2006, Australia
a r t i c l e i n f o
Article history:
Received 8 February 2011
Received in revised form
8 July 2011
Accepted 8 July 2011
Available online 19 July 2011
Keywords:
Powder dispersion
Impact angle
Agglomerates
Computational uid dynamics
Discrete element method
a b s t r a c t
This paper numerically investigated the mechanisms of powder de-agglomeration on
mechanical impaction, aiming to explain the experimental observations in our previous
study (Adi et al., 2010). A numerical model based on a coupled computational uid
dynamics (CFD) and discrete element method (DEM) approach was developed to simulate
the dispersion of drug mannitol agglomerates in the customised impaction throats
containing one or two angles with different ow rates. Information in terms of particle-
throat and particle-uid interactions, number of fragments, ne particle fraction (FPF) and
powder deposition was monitored over the whole process and quantitatively analysed.
The results indicated that the breakage of the agglomerate was mainly attributed to the
mechanical impaction and less affected by the shear effect from the ow-particle
interaction. While the rst impaction caused the major damage to the agglomerate, the
second impaction in fact generated more ne particles with size less than 5 mm, resulting
much improved dispersion performance for the throats with two angles. Powder
deposition, which is dependent on impaction velocity and angle and fragment size, was
another important factor affecting the dispersion. The analysis of dispersion mechanisms
indicated that de-agglomeration at different conditions can be characterised by the ratio
of the particle-wall impaction energy and agglomerate strength.
& 2011 Elsevier Ltd. All rights reserved.
1. Introduction
Powder dispersion in dry powder inhalers (DPIs) is a complex process controlled by interparticle cohesion, powder-ow
interaction and powder-device impaction. It has been widely reported that the mechanical impaction with device is a
major contribution to agglomerate breakage (Dunbar et al., 1998; Finlay, 2001; Voss & Finlay, 2002; Xu & Zhu, 2006).
Moreno et al. (2003) and Moreno and Ghadiri (2006) studied the effect of impact angle on the breakage of agglomerates
and found the normal component of impact velocity is the dominant factor. However, using more plastic and softer
particles, Samimi et al. (2004) found that at low impact velocity the normal component of impact velocity determines the
extent of breakage, independent of the impact angle. At high impact velocity, its tangential component becomes
increasingly important. Our recent attempts to understand mannitol agglomerate break-up using numerical simulations
showed that increasing impact velocity improves agglomerate breakage and a 451 impact angle results in the maximum
breakage for a given velocity (Tong et al., 2009; Yang et al., 2008).
However, a few important issues, such as the effects of air ow, powder deposition and multiple impactions, were not
considered in those studies. In fact, air ow can be very important as it is the main driving force for powder movements
Contents lists available at ScienceDirect
journal homepage: www.elsevier.com/locate/jaerosci
Journal of Aerosol Science
0021-8502/$ - see front matter & 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jaerosci.2011.07.004
n
Corresponding author.
E-mail address: r.yang@unsw.edu.au (R.Y. Yang).
Journal of Aerosol Science 42 (2011) 811819
(Tong et al., 2010). Powder deposition (powders retained by devices) and multiple impactions also affect the nal results.
To address these issues, we recently carried out experimental studies on the de-agglomeration of powders in the specially
designed impaction throats containing one or two angles (Adi et al., 2010). The results showed that mechanical impaction
had a signicant effect on agglomerate breakage. For the two-angle throats, there existed an optimal throat angle (451) and
air ow (120 l min
1
) to obtain maximum dispersion efciency characterised by maximum ne particle fraction (FPF), a
balanced result between improved breakage and increased deposition with increasing air ow rates. The throats with two
angles had better agglomerate breakage than those with a single angle.
Several questions, however, remain from that study. For example, what are the exact roles of the rst and second
impactions? How does the turbulence affect the powder dispersion and why does the larger ow rate not always improve the
amount of ne powders (o5 mm) coming out from the throats? To answer these questions, the detailed knowledge of the
particle and ow information over the process is required. Such information, however, is impossible to obtain from experiments.
Therefore, while possible hypotheses/explanations were proposed, they were not conrmed in our previous work.
This work is the follow up of our previous experimental study (Adi et al., 2010) by carrying out the coupled
computational uid dynamics (CFD) and discrete element method (DEM) simulations of dispersion process. The
microdynamic information of particles and ow is analysed to understand the underlying mechanisms and to be used
to explain the experimental observations. Furthermore, a quantitative index based on the ratio of interparticle cohesion
and mechanical impaction is proposed to describe the dispersion performance.
2. CFD-DEM modelling and validation
A coupled CFD-DEM model was developed to simulate the dispersion process. Detailed description of the model has
been given in our previous studies (Tong et al., 2010) and is not repeated here. However, it should be noted that a fully
coupled method was adopted here, which means the data from DEM and CFD were exchanged at each time step. Therefore,
the full dynamics and instantaneous variation of particles and ow can be captured.
The simulation conditions were similar to those in the experiments (Adi et al., 2010). The setup of the de-agglomeration
apparatus is shown in Fig. 1. In the simulations, air of different owrates entered the impaction throat fromthe right side air inlet
and an agglomerate was introduced via the feed apparatus (as indicated by B in Fig. 1). The agglomerate moved along with the
air owand impacted with throats containing two angles (Fig. 1a and b) or a single angle (Fig. 1ce). The agglomerate used in this
work was formed with mannitol powders under an assumed centripetal force as described in our previous work (Yang et al.,
2008). The mannitol powder had the size distribution as shown in Fig. 2a with the mass mean diameter of 3.27 mm. The formed
agglomerate (Fig. 2b) had a diameter of 51 mmwith porosity of 0.5 and a theoretical tensile strength of 1.21 kPa fromthe Rumpfs
model (Rumpf, 1962; Yang et al., 2008). Details of the parameters used in the simulations are provided in Table 1.
As reported in our previous work (Adi et al., 2010), the numerical model was validated by comparing the simulated results,
such as the trajectory of the agglomerates and the amount of ne particles less than 5 mm (FPF) generated, with those from
the experiments. The comparisons on FPF are shown in Fig. 3 to provide a background for the later discussion. Here FPF
load
is
dened as the mass fraction of particles smaller than 5 mm in the exiting aerosol, referenced against the total mass of powder
loaded into the impaction throat. The powders deposited on the throat wall are not considered. The simulated results are
qualitatively comparable with the experimental observations. For the two-angle throats (A and B) and the single angle throat
C with 901 impaction angle, FPF increases with impact angles at low ow rates (60 and 120 l min
1
) but decreases at the high
ow rates of 150 l min
1
. For the single angle throats D and E, FPF increases monotonically with ow rate. As shown later on,
60 cm
A
A
60 cm
2
0

c
m

60 cm
A
B
45
B 15 B
30 cm 30 cm 30cm
A
A
30 cm 30 cm
Fig. 1. Schematics of impaction throats: (a) throat A; (b) throat B; (c) throat C; (d) throat D; and (e) throat E. A is the impact point, which is located 60 cm
from the inlet of the main section. B is feed apparatus used to feed agglomerate into the throat via a 4 mm opening.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 812
the decrease in FPF at high ow rate for throats A, B and C is caused by the increased powder deposition. In general, the
throats with two angles (A and B) result in better dispersion than those with a single angle (C, D and E), showing that the
multiple impactions can improve powder de-agglomeration.
In the following, the micro-dynamics of the dispersion process will be analysed to investigate the roles of uid ow,
mechanical impactions and powder dispersion. Finally, an energy based equation will be given to quantify these effects.
3. Results and discussion
3.1. Effect of uid ow
It has been reported that turbulence can be a major cause for the agglomerate break-up because of the aerodynamic lift,
drag and shear force generated by the eddies (Brown et al., 2003; Coates et al., 2005; French et al., 1996; Li et al., 1996;
Timsina et al., 1994). To investigate the effect of air ow on dispersion under the current condition, Fig. 4 shows the
0
0.0
0.1
0.2
0.3
0.0
0.2
0.4
0.6
0.8
1.0
C
u
m
u
l
a
t
i
v
e

m
a
s
s

d
i
s
t
r
i
b
u
t
i
o
n
P
r
o
b
a
b
i
l
i
t
y

d
e
n
s
i
t
y

f
u
n
c
t
i
o
n

(
m
a
s
s
)
Diameter (m)
1 2 3 4 5 6 7 8 9
Fig. 2. (a) Mass based size distribution and cumulative mass distribution of parimary powder; and (b) the morphology of the formed agglomerates
(colours represent particle diameters).
Table 1
Values of the key parameters used in the simulations.
Parameter Value
Number of particle, N
p
3000
Particle density, r
p
1490 kg m
3
Youngs modulus, Y 110
8
N m
2
Poissons ratio, ~ s 0.29
Sliding friction coefcient, m
s
0.3
Rolling friction coefcient, m
r
0.0002 m
Normal damping coefcient, g 210
6
s
1
Hamaker constant, H
a
1.210
19
J
Air ow rate, Q 60, 120, 150 l min
1
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 813
integral scale strain rate (ISSR) of throat C with a ow rate of 150 l min
1
. ISSR is a measure of the velocity gradient across
the integral scale eddies (the most energetic occurring in a turbulence ow) and has been demonstrated to be more
relevant to powder dispersion (Finlay, 2001). It can be seen that ISSR is larger near the wall and has a maximum value at
the inner intersection where the ow starts to change direction. ISSR shows similar patterns for other throats but the
maximum ISSR decreases with decreasing ow rate and impaction angle.
Since ows consisting of eddies that exhibit large ISSR exert large aerodynamic forces on the agglomerate, the
agglomerate is more likely to be broken in this region. Therefore, the effect of ow on powder dispersion can be quantied
in terms of the maximum shear stress generated from the ow on the agglomerate. As proposed by Bagster and Tomi
(1974), the maximum shear stress, t
max
, acting on a spherical particles is in the central plane parallel to uid direction,
given by
t
max
F
f
F
i
=A 1
where F
f
and F
i
are the total particle-uid force and inertial force, respectively, applied on the half of the agglomerate
above the central plane with the area A. Fig. 5 shows the maximum shear stress on the agglomerate under different
conditions. Similar to the maximum ISSR, the maximum shear stress also increases with the air ow rate and impaction
angle (throat C4A4B4E4D). Comparing with the tensile strength of the agglomerate, however, the maximum shear
0
10
20
30
40
Second impaction
60 L/min
F
P
F
l
o
a
d
e
d

(
%

M
a
s
s
)
A D E
Impaction throat
120 L/min 150 L/min
Experiments
B C
Fig. 3. FPF generated at different impaction conditions and ow rates. The experimental data (Adi et al., 2010) are also plotted for comparison.
Fig. 4. Contour of integral scale strain rate of throat C at 150 l min
1
.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 814
stress is much lower. Even the largest value (throat C at 150 l min
1
) is less than half of the agglomerate tensile strength of
1.21 kPa. Therefore, the break-up of the agglomerate due to the turbulence ow is minimum in the current work.
3.2. Mechanical impactions and effect of second impaction
The dispersion process can be further investigated by plotting the variations of the number of fragments and particle-
wall impact force with dispersion time as shown in Fig. 6. Note different scales are used for different throats. The
dispersion time is normalised against the residence time of the agglomerate in the throat when the particles are
discharged from the outlet. As mentioned above, the uid has no visible effect on the powder dispersion so there is no
breakage for the agglomerate before the rst impaction with the throats. During the rst impaction, a strong spike is
shown in the agglomerate-wall impact force. In the mean time, there is a rapid increase in the number of fragments. The
fragment numbers gradually become saturated for throats C, D and E. For throats A and B, there are second impaction at
the normalised time of 0.72 and 0.37, respectively, which causes a step change in the number of fragments. For throat A,
the second impaction is even stronger than the rst one (125 mN vs. 65 mN). The second impaction also lasts longer, and
therefore causes more severe breakage as reected from the sharp increase in the number of fragments. In contrast, the
second impaction for throat B is much weaker than the rst one. This is because the agglomerate has already broken into
60
0.0
0.2
0.4
0.6
0.8
1.0
1.2
M
a
x
i
m
u
m

s
h
e
a
r

s
t
r
e
s
s

(
k
P
a
)
Airflow rate (l/min)
Throat A
Throat B
Throat C
Throat D
Throat E
Agglomerate tensile strength
90 120 150
Fig. 5. Agglomerate tensile stress and maximum shear stress of throats AE at different air ow rates.
0.0
0
240
480
720
0
260
520
0
500
1000
0
240
480
0
200
400
0
240
480
720
0
40
80
0
200
400
0
60
120
(a)
(b)
(c)
(d)
(e)
0
240
480
Number
Force
F
r
a
g
m
e
n
t

n
u
m
b
e
r
N
o
r
m
a
l

c
o
n
t
a
c
t

f
o
r
c
e

p
a
r
t
i
c
l
e
-
w
a
l
l

(
m
N
)
Normalized time ()
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Fig. 6. Time evolution of the number of fragments and agglomerate-wall impact force for agglomerates impacted at 120 l min
1
using different throats
AE. Note different scales are used.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 815
many small fragments on the rst impaction. This is evident from Fig. 7 which superimposes the breakage conditions after
the rst and second impactions for the throats A and B.
It was postulated in our previous paper (Adi et al., 2010) that the rst impaction more likely causes major breakage
while the second one acts as a facilitator for further break-up. To test this assumption, the cumulative mass distributions
of the fragments after each impaction are plotted in Fig. 8. For throat A, the total fraction of ne particles less than 5 mm
(including those deposited on the wall) is 8% and 35%, respectively, after the rst and second impactions (also see Fig. 3).
For throat B, the total ne particle fraction after the rst and second impaction is 14% and 38%, respectively. It
demonstrates that the second impaction is more important in generating ne powders, which improves the dispersion
efciency signicantly.
3.3. Effect of powder deposition
Powder deposition (amount of powder retained in the throats) also affects the dispersion performance. As shown in
Fig. 3, although larger ow rates have better breakage, FPF actually decreases at the high ow rate of 150 l min
1
for
throats A, B and C. This is mainly due to the increased deposition on throat wall at large ow rates, which reduces the
amount of ne powders exiting from the outlet and thus leads to an overall reduction in FPF. An optimal dispersion is the
combined result of de-agglomeration and deposition.
Fig. 9 shows the powder deposition under different impaction conditions. Again the simulated total depositions are
comparable with experimental results, further conrming the validity of the model. It is observed that the deposition is
dependent on both impaction angle and inertial energy (mass and velocity) of fragments. The general trend is that smaller
impaction angles have less powder deposition for single impaction (i.e. throats AEDoBEEoC). However, the second
impaction also plays an important role in the deposition. For throat A with the second impact angle of 751, large deposition
occurs at the second impaction region, which is consistent with the experimental observation (Adi et al., 2010). In
comparison, the deposition in throat B is smaller in the second impaction than in the rst one because of the relatively
smaller fragment size in the second impaction. This can be further conrmed in Fig. 10, which shows the amount of
deposition at different positions for throats A and B. The dotted-lines show the starting points of the two impactions.
While throat A has more particle deposition after the second impaction, throat B shows a large amount of deposition after
Before
impaction
First impaction
Second
impaction
Before second
impaction
Fig. 7. Snapshots of agglomerate dispersion at 120 l min
1
(a) throat A and (b) throat B. (The colours represent the magnitude of particle velocity.) (For
interpretation of the references to colour in this gure legend, the reader is referred to the web version of this article.)
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 816
0
0
20
40
60
80
100
F
r
a
g
m
e
n
t

m
a
s
s

c
u
m
u
l
a
t
i
v
e

(
%
)
Fragment diameter (m)
After 1st impaction (throat A)
After 2nd impaction (throat A)
After 1st impaction (throat B)
After 2nd impaction (throat B)
2 4 6 8 10 12 14 16 18 20 22
Fig. 8. Cumulative mass distribution of fragments after rst and second impactions for throat A and B at 120 l min
1
(powders deposited on the wall are
also considered).
0
10
20
30
40
50
60
70
A
120 L/min
T
h
r
o
a
t

d
e
p
o
s
i
t
i
o
n

(
%

M
a
s
s
)
Impaction throat
Experiments Second impaction
60 L/min 150 L/min
B C D E
Fig. 9. Mass fraction of powder deposition in different impaction throats at different ow rates. The experimental results (Adi et al., 2010) are shown for
comparison.
0.40
0
1
2
3
4
5
0
5
10
15
20
Second
impaction
First
impaction
First
impaction
Second
impaction
Throat B
D
e
p
o
s
i
t
i
o
n

(
%

M
a
s
s
)
Distance from feeding point (m)
Throat A
0.45 0.50 0.55 0.60 0.65
Fig. 10. Deposition mass distribution on the axial direction in throats A and B.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 817
the rst impaction but before the second one. Therefore to reduce deposition, both device design (e.g. impaction angle) and
the ow condition (e.g. ow rate) have to be carefully considered.
3.4. Dispersion mechanisms
The above results show that the breakage of the agglomerate in the throats is mainly due to the particle-wall impaction
while the ow has no obvious effect on the breakage. Another important property to affect the breakage is the strength of
the formed agglomerate. Our previous studies (Tong et al., 2009, 2010) indicated that the dispersion performance can be
characterised in terms of particle-wall impaction energy E
pw
and agglomerate tensile energy E
ad
. The particle-wall impact
energy is given by
E
pw

X
K
i
Z
t
0
v
i,n
UF
i,n
dt
Z
t
0
v
i,t
UF
i,t
dt

2
where K is the number of particles impacting on the wall, and F
i,n
, F
i,t
, v
i,n
and v
i,t
are the forces and velocities of particle i in
the normal and tangential directions, respectively. The tensile energy of an agglomerate E
ad
is calculated from the Rumpfs
model (Rumpf, 1962). Details can be found from our previous papers (Tong et al., 2009; Yang et al., 2008).
Fig. 11 shows FPF
load
obtained under different conditions as a function of the ratio of impaction and tensile energy
f(E
pw
/E
ad
). It is observed the results collapse on a single master curve which can be tted by an error function, given by
FPF
load
FPF
load,1
erf kf
n
3
where FPF
load,N
is the limiting value when the energy ratio f is innitely large, k and n are two empirical parameters. With
the current results, FPF
load,N
0.25, k0.92 and n0.86. The results further indicate that agglomerate breakage is
governed by the same mechanisms at different throats.
4. Conclusions
This work studied the effect of impact angles on powder dispersion at the presence of air ow by using CFD-DEM
approach. By analysing the ow eld and micro-dynamics of particles, the dispersion mechanisms were investigated at the
particle level. The main ndings can be summarised as follows:
The generation of ne particles with size less than 5 mm was mainly attributed to the second impaction instead of the
rst one. After the rst impaction, the agglomerate was broken up into many small fragments with weak strength;
second impaction further disintegrated them into smaller fragments.
Powder deposition was dependent on impaction angle and the inertial energy (mass and velocity) of fragments.
While increasing ow rate and the number of impactions increased breakage, they also resulted in larger powder
deposition. To have optimal dispersion, both device design and ow condition should be considered.
Agglomerate breakage at different conditions was governed by the same mechanisms, which can be described by a
unied error function in terms of the ratio of agglomerate-wall impaction and agglomerate strength.
0
0.00
0.05
0.10
0.15
0.20
0.25
Throat A
Throat B
Throat C
Throat D
Throat E
F
P
F

(
%

M
a
s
s
)
1 2 3

Fig. 11. Correlation between ne particle fraction (FPF) and the ratio between the impact energy and agglomerate cohesion energy (f) in different
throats.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 818
Acknowledgements
Authors are grateful to the Australia Research Council (ARC) for the nancial support for this work.
References
Adi, S., Tong, Z.B., Chan, H.K., Yang, R.Y., & Yu, A.B. (2010). Impact angles as an alternative way to improve aerosolisation of powders for inhalation?
European Journal of Pharmaceutical Sciences, 41, 320327.
Bagster, D.F., & Tomi, D. (1974). The stresses within a sphere in simple ow elds. Chemical Engineering Science, 29, 17731783.
Brown, D.P., Kauppinen, E.I., & Jokiniemi, J.K. (2003). Agglomerate deaggregation potential during dry powder inhaler operation and characterization
under steady and unsteady conditions. Journal of Aerosol Science, 34, 14171428.
Coates, M.S., Fletcher, D.F., Chan, H.-K., & Raper, J.A. (2005). The role of capsule on the performance of a dry powder inhaler using computational and
experimental analyses. Pharmaceutical Research, 22, 923932.
Dunbar, C.A., Hickey, A.J., & Holzner, P. (1998). Dispersion and characterization of pharmaceutical dry powder aerosols. Kona, 16, 745.
Finlay, W.H. (2001). The Mechanics of Inhaled Pharmaceutical Aerosols, An Introduction. Academic Press: London.
French, D.L., Edwards, D.A., & Niven, R.W. (1996). The inuence of formulation on emission, deaggregation and deposition of dry powders for inhalation.
Journal of Aerosol Science, 27, 769783.
Li, W.-I., Perzl, M., Heyder, J., Langer, R., Brain, J.D., Englmeier, K.H., Niven, R.W., & Edwards, D.A. (1996). Aerodynamics and aerosol particle deaggregation
phenomena in model oral-pharyngeal cavities. Journal of Aerosol Science, 27, 12691286.
Moreno, R., & Ghadiri, M. (2006). Mechanistic analysis and computer simulation of impact breakage of agglomerates: effect of surface energy. Chemical
Engineering Science, 61, 24762481.
Moreno, R., Ghadiri, M., & Antony, S.J. (2003). Effect of the impact angle on the breakage of agglomerates: a numerical study using DEM. Powder
Technology, 130, 132137.
Rumpf, H. (1962). The Strength of Granules and Agglomerates. Interscience: New York.
Samimi, A., Moreno, R., & Ghadiri, M. (2004). Analysis of impact damage of agglomerates: effect of impact angle. Powder Technology, 143, 97109.
Timsina, M.P., Martin, G.P., Marriott, C., Ganderton, D., & Yianneskis, M. (1994). Drug delivery to the respiratory tract using dry powder inhalers.
International Journal of Pharmaceutics, 101, 113.
Tong, Z.B., Yang, R.Y., Chu, K.W., Yu, A.B., Adi, S., & Chan, H.K. (2010). Numerical study of the effects of particle size and polydispersity on the agglomerate
dispersion in a cyclonic ow. Chemical Engineering Journal, 164, 432441.
Tong, Z.B., Yang, R.Y., Yu, A.B., Adi, S., & Chan, H.K. (2009). Numerical modelling of the breakage of loose agglomerates of ne particles. Powder Technology,
196, 213221.
Voss, A., & Finlay, W.H. (2002). Deagglomeration of dry powder pharmaceutical aerosols. International Journal of Pharmaceutics, 248, 3950.
Xu, C.B., & Zhu, J. (2006). Parametric study of ne particle uidization under mechanical vibration. Powder Technology, 161, 135144.
Yang, R.Y., Yu, A.B., Choi, S.K., Coates, M.S., & Chan, H.K. (2008). Agglomeration of ne particles subjected to centripetal compaction. Powder Technology,
184, 122129.
Z.B. Tong et al. / Journal of Aerosol Science 42 (2011) 811819 819