Chemical Engineering Science 61 (2006) 3435 – 3451

www.elsevier.com/locate/ces

Granular attrition in a rotary valve: Attrition product size and shape

Jun Yao a , Chi-Hwa Wang a,b,∗ , Eldin Wee Chuan Lim b , John Bridgwater c
a Singapore-MIT Alliance, E4-04-10, 4 Engineering Drive 3, Singapore 117576, Singapore
b Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576, Singapore
c Department of Chemical Engineering, University of Cambridge, Pembroke Street, Cambridge CB2 3RA, UK

Received 22 August 2005; received in revised form 20 October 2005; accepted 10 December 2005
Available online 15 February 2006

Abstract
The rotary valve is a widely used mechanical device in solids-handling industrial processes, but it is responsible for much attrition. Here, the
attrition occurring in a rotary valve operating both as a stand-alone device and as part of a pneumatic conveying system was, for the first time,
investigated. In the former case, attrition at three rotary valve speeds was consistent with the Gwyn correlation. For polypropylene, attrition
was dependent on the number of rotations of the valve, but for PVC there was also a further rate dependent effect. In the latter case the Gwyn
parameter was higher than those for higher air flow rates. This may be ascribed to a greater amount of material accumulating at the exit of the
rotary valve.
The attrition product tended to assume a narrow, elongated morphology. Attrition products were found to be in five basic shapes, these being
dependent on the shearing action of the vanes in the rotary valve. The new concepts of shear frequency and attrition frequency are proposed.
Over a wide range of attrition product sizes and shapes, the principles of attrition in the rotary valve were unified in a remarkably simple
manner. As such, these concepts described well all findings and offered a characterisation of attrition in complex systems.
䉷 2006 Elsevier Ltd. All rights reserved.

Keywords: Attrition; Rotary valve; Granules; Pneumatic conveying

1. Introduction followed. Along with these experimental studies, several em-

Granular material is widely processed and attrition of such
material due to mechanical effects is commonly observed as
reviewed by Bemrose and Bridgwater (1987). Attrition may
lead to significant changes in physical characteristics and flow
behaviour (Valverde et al., 2003; Blair and Kudrolli, 2003).
This is important to many industrial processes but remains far
from being completely understood.
As attrition in process equipment is extensively caused by
shear, testing techniques that produce shear strain have been
proposed. Among these, the annular shear cell test has be-
come commonly used. The equipment was developed originally
by Hvorslev (1939) to study shearing resistance in soils that
occurs after continued straining in one direction. The use of
the annular shear cell for attrition testing was developed first
by Paramanathan and Bridgwater (1983a,b) and others have
∗ Corresponding author. Tel.: +65 6874 5079; fax: +65 6779 1936.
E-mail address: chewch@nus.edu.sg (C.-H. Wang).
0009-2509/$ - see front matter 䉷 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2005.12.013
pirical models have been developed to characterise the extent
of attrition in various facilities. For example, Gwyn (1969) de-
scribed attrition of a bed of solids held in a cylindrical vessel
into which an air jet was injected at high velocity. He stated
that the attrition of initially single-sized particles could be de-
scribed empirically by
W = K · t m, (1)
where W is the mass that has undergone attrition at time t and
m is an empirical constant. K is another constant which he
argued was a function of initial particle size. This model was
found by Paramanathan and Bridgwater to represent well the
attrition occurring in a shear cell. Ouwerkerk (1991) carried
out studies using an annular cell to understand the relationship
between the deformation of individual particles and breakage.
Neil and Bridgwater (1994) examined the attrition occurring
for a wide range of materials such as urea prills, various
forms of sodium chloride, molecular sieve beads and alu-
mina extrudates. Their work shows that m is a constant for a
3436 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

given material and the constant of proportionality K is related et al. (2002) investigated the changes to granules during re-
to the normal stress. Later, Neil and Bridgwater (1999) em- peated pneumatic transport, along with the factors that affect
ployed the Gwyn equation to characterise three particulate sys- these changes.
tems: heavy soda ash (0.36–0.50 mm), TAED (1.0–1.6 mm) and The rotary valve is a widely used volumetric feeder in the
TAED (0.50–0.71 mm) subjected to attrition using a laboratory food, chemical, cement and textile industries (Al-din and Gunn,
fluidised bed, a screw pugmill, and an annular shear cell. For 1983; Mehmet, 2004) and has also been used for studies on
each material, one characterisation parameter, m of the Gwyn pneumatic conveying of granular materials (Rao et al., 2001;
formulation, was found to be independent of the equipment Zhu et al., 2003, 2004; Yao et al., 2004). During its operation
type. More recently, Ghadiri et al. (2000) also used an annular (Yao et al., 2004), especially at a low air flow rate, the rotary
cell and evaluated on the role of fragmentation and surface dam- valve has been observed to cause significant attrition to the
age (quantified the dependence of the applied load and strain). granular material used. Here a series of experiments have been
Bridgwater et al. (2003) used particles made of one material carried out using a rotary valve (both on its own and integrated
but with different shapes to study the relationship between the with a pneumatic conveying system) to develop understand-
applied stress, strain, particle shapes and the products of attri- ing of the rate of attrition and its relationship to operating
tion and showed that the mechanics of attrition, as given by conditions.
the full size distribution can be unified. Crutchley and Bridg-
water (1997) studied particle attrition in small clearances via a
2. Experimental design
cone cell and found that the breakage rate of particles changes
dramatically with gap size. Maxima in the attrition rate were
2.1. Granules
found with gap widths of about one and about two particle
diameters.
Two types of granular materials, polyvinyl chloride (PVC)
Two-dimensional numerical simulations following attrition
and polypropylene (PP) were used; physical properties are listed
in an annular shear cell were reported by Potapov and Camp-
in Table 1. The size fraction was obtained using the particle
bell (1997) who showed that the extent of breakage was pro-
size/shape analyzer (Analytical Technologies Pte Ltd, Singa-
portional to the work done during the shearing process for their
pore). The standardised flow time was measured using a Gran-
system. Potapov and Campbell (2001) studied the breakage in-
ulate Tester ERWEKA (GT/GTB, ERWEKA GmbH, Heusen-
duced by two mechanisms. Mechanism I covered breakage re-
stamm, Germany). Granules flowed from a hopper through a
sulting from stresses that are induced in an unbroken particle
25 mm diameter orifice into a collecting vessel resting on a
and accounts for the larger fragments. Mechanism II involved
weighing balance. The time taken by the granules to flow and
buckling of fragments obtained from Mechanism I and gener-
weight of granules collected were recorded. In addition, the in-
ated most of the fines. Ghadiri and Zhang (2002) studied im-
ternal angle of friction
of each type of granular material was
pact attrition with a single particle by allowing well-defined
determined using a triaxial tester (Wykeham Farrance, Slough,
and controlled loading to be applied to a single particle. Based
England). Each test was applied to three specimens, consisting
on indentation fracture mechanics and impact damage analysis,
of particles and water in the form of right cylinders of nomi-
a model (Ghadiri and Zhang, 2002) of impact attrition due to
nal diameter (50 mm) and height (100 mm). Particle hardness
chipping of particulate solids was developed. Single crystals of
was measured automatically using Digital Rockwell Hardness
KCl, NaCl and MgO (Zhang and Ghadiri, 2002) were impacted
Tester TH 301 (Micro Photonics Inc. Allentown, PA).
against a rigid target at a specified velocity and at a normal di-
In Table 1, both the standardised flow time and particle inter-
rection to quantify material removal from the particles and the
nal friction angle show that PP possess higher flowability than
results were consistent with the model.
PVC. The reported 10% variation in internal friction angle be-
Attrition occurs during pneumatic conveying. Davuluri and
tween PP and PVC particles resulted in about 30% difference
Knowlton (1998) dealt with particle degradation in standard-
in their standardised flow times. This highly nonlinear sensitiv-
ised bulk attrition tests to determine the relative tendency of
ity of flow time to internal friction angle is more significant for
materials to attrite. These so-called friability tests are quite
the dense flow (used for measurements in a hopper) than dilute
useful in the first assessment of a candidate conveying mate-
flow (dispersed pneumatic conveying). In general, flow time in-
rial. Kalman (2000) examined the effects of experimental pro-
creases slowly as the diameter of particles decreases. This may
cedure, bend structure and conveying parameters on attrition
rate. He concluded that air velocity, loading ratio, bend struc-
Table 1
ture (including factors such as curvature, materials, number of Physical properties of granular material
bends) and number of collisions were the main factors influ-
encing the rate of attrition. More recently, Salman et al. (2002) PVC PP
used a continuous-flow gas gun to study single particle im- Size fraction (mm) 3.35–4.1 2.8–3.35
pacts and examined the characteristics of particle fragmenta- Particle standardized flow time (s/100 g) 1.03 0.7
tion. The effects of particle velocity, impact angle, particle size Particle internal friction angle (
) 31.2◦ 29.2◦
and number of impacts on the percentage of unbroken particles Particle friction coefficient (tan
) 0.61 0.56
Particle hardness—Rockwell R113 R90
were investigated and a numerical model was successfully de-
Particle density (kg/m3 ) 1400 1123
veloped to predict the probability of particle breakage. Konami
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451
Fig. 1. Schematic of the pneumatic conveying facility (Attrition I: at the rotary valve entrance; Attrition II: at the rotary valve exit): 1: air control valve;
2: air dryer (silica gel with indicator-blue); 3: rotameter; 4: rotary valve (dimensions: R0 : 105 mm; R1 : 104 mm; W : 248 mm; h1 : 25 mm; D2 : 70 mm;
vane width: 5 mm)
be due to a strong dependence of flow time on the shape of
particles and the fact that attrited particles become much more
irregular in shape than original particles. The flowability of PP
bead is much better than that of PVC cylinder. This may also
be attributed to the shape of particles. PP beads are ellipsoidal
but PVC particles are cylindrical.
2.2. Rotary valve
The device has eight pockets (General Resource Corp, Hop-
kins, Minnesota) and its structure and dimensions are shown in
Fig. 1. To vary the speed of the rotary valve, a three phase fre-
quency inverter (HF-320 Series, Sumitomo Heavy Industries,
Ltd) was used to change the power frequency and three speeds
were used: 15.8, 25.0 and 30.4 rpm.
The procedure was as follows. The pneumatic system was
disconnected and only the rotary valve itself was used. The
bottom pipe inside the rotary valve vessel (Fig. 1) was filled
with granular material to a level just below the vanes. The
rotary valve was then run at a constant speed and granular
material added slowly to maintain a constant level. At ap-
propriate time intervals, the rotary valve was stopped and all
granular material removed for weight-size distribution anal-
ysis by sieving. The process was repeated for each rotary
valve speed.
Care had to be taken to ensure that stresses arising during
attrition could be sustained by the equipment without the pos-
sibility of failure. For example, clogging by granular material
in the gap between the rotary valve vanes and casing wall could
result in high stresses thereby causing fracture of the vanes.
3437
On the other hand, for the rotary valve running at a low speed,
clogging may then stop the vanes and damage the electric mo-
tor valve. These issues defined the three rotary valve speeds
chosen.
Weight-size distribution analyses were carried out using man-
ual sieving rather than with a sieve shaker because some gran-
ules whose sizes are of about the same scale as a particular
sieve size may block the sieve apertures due to their irregular
shape and prevent smaller granules from being separated out.
Manual sieving allows for human intervention to minimise the
occurrence of such problems.
2.3. Pneumatic conveying system
The experimental setup used the full equipment shown in
Fig. 1. The inner diameter of the pipe was 40 mm and the length
of the vertical pipe section between two smooth 90◦ elbows
(bend curvature: 2) was 2.97 m, while the horizontal section
was 4.12 m in length. The conveying pipe was made of PVC
that was transparent, to allow visual observation and had a wall
thickness of 5 mm. The entire configuration was held in position
using metal castings and supports with various pipe segments
joined by connectors and reinforced by silicone gel. Only PVC
was used throughout the experiments.
Air from the compressor mains (air pressure: 75 psi) flowed
through the rotary feeder, driving granules fed into the convey-
ing system. A valve (1) was used to adjust the air flow rate.
The air flow rate was also controlled via a rotameter (3) which
allowed a maximum flow rate of 2000 l/min. Based on previ-
ous work (Yao et al., 2004) three air flow rates were chosen:
3438 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

12

Attrited weight (%)

9

140
6 110
80 i n)
3 (m
50 e
m
30 Ti
0

0
.1

.4

.0

.3

.8
<1

-1

-2

-2

-2
18

41

00

36
1.

1.

2.

2.
(a) Sieve aperture (mm)

6
Attrited weight (%)

4
30.4
)
m
25 (rp
2
e ed
15.8 sp
e
0 alv
ryv
ta
1

0
Ro
8

.4

.0

.3

.8
.1

-1

-2

-2

-2
<1

18

41

00

36
1.

1.

2.

2.

(b) Sieve aperture (mm)

15
Attrited weight (%)

12

9 200
160
6
120 )
in
3 80 (m
e
m
0
40
Ti
8

5
.1

.4

.0

.3

.8

.3
<1

-1

-2

-2

-2

-3
18

41

00

36

80
1.

1.

2.

2.

2.

(c) Sieve aperture (mm)

12
Attrited weight (%)

3 30.4 )
rpm
e d(
0
25
s pe
15.8 lve
va
8

ay
.1

.4

.0

.3

.8

.3

otr
<1

-1

-2

-2

-2

-3
18

41

00

36

80

R
1.

1.

2.

2.

2.

(d) Sieve aperture (mm)

Fig. 2. Attrition product size distribution: (a) rotary valve speed at 25.0 rpm (PP); (b) after 30 min (PP); (c) rotary valve speed at 25.0 rpm (PVC); (d) after
120 min (PVC).

1600, 1100 and 950 l/min, and the corresponding air superficial digital thermo-hygrometer (RH411, OMEGA Technologics
velocity inside the pipe was 21.20, 14.59 and 12.60 m/s. The Ltd.) before and after each test. Ambient temperature was
air humidity was controlled by the dryer at a relative humid- controlled at 28–30 ◦ C. For all cases conducted, the mass of
ity, RH = 5% and this was checked using a high performance granular material was 1100 g.
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3439

Table 2
Attrition product size distribution analysis for single rotary valve

Granular material Rotation speed (rpm) Time (min) Sieve aperture (mm) Total percentage attrited

< 1.18 1.18–1.41 1.41–2.00 2.00–2.36 2.36–2.80 2.80–3.35

PP 15.8 30 0.01% 0.03% 0.39% 0.90% 3.91% – 5.24%

PP 15.8 60 0.02 0.05 0.69 1.61 5.90 – 8.27
PP 15.8 90 0.02 0.08 1.04 2.43 6.47 – 10.04
PP 15.8 120 0.03 0.10 1.27 2.95 7.63 – 11.98
PP 25.0 30 0.03 0.05 0.75 1.39 4.29 – 6.51
PP 25.0 50 0.04 0.07 1.14 2.12 5.14 – 8.51
PP 25.0 80 0.09 0.11 1.90 3.57 7.26 – 9.93
PP 25.0 110 0.14 0.22 2.60 5.00 9.03 – 16.99
PP 25.0 140 0.20 0.31 3.42 6.55 11.10 – 21.58
PP 30.4 30 0.04 0.08 0.98 2.17 4.38 – 7.65
PP 30.4 60 0.07 0.13 1.82 3.82 5.70 – 11.54
PP 30.4 90 0.13 0.24 3.02 5.78 8.43 – 17.60
PP 30.4 120 0.22 0.27 4.45 7.28 9.04 – 21.26
PVC 15.8 60 0.14% 0.09% 0.50% 0.52% 1.21% 2.46% 4.92%
PVC 15.8 90 0.23 0.13 0.67 0.64 1.74 3.38 6.79
PVC 15.8 120 0.29 0.16 0.87 0.88 2.33 4.26 8.79
PVC 15.8 150 0.36 0.18 0.97 1.10 2.67 5.19 10.47
PVC 15.8 180 0.40 0.19 1.03 1.24 3.06 5.96 11.88
PVC 15.8 210 0.47 0.24 1.29 1.58 3.84 6.91 14.33
PVC 15.8 240 0.92 0.29 1.54 1.94 4.87 8.03 17.59
PVC 25.0 40 0.19 0.17 0.81 1.08 2.07 3.55 7.87
PVC 25.0 80 0.31 0.28 1.67 1.70 4.36 6.50 14.82
PVC 25.0 120 0.50 0.40 1.99 2.25 5.56 7.40 18.10
PVC 25.0 160 0.93 0.78 3.77 4.24 9.74 11.97 31.43
PVC 25.0 200 1.23 1.02 5.05 5.71 12.81 13.04 38.86
PVC 30.4 9 0.04 0.02 0.15 0.14 0.50 2.01 2.86
PVC 30.4 30 0.23 0.13 0.88 1.15 2.77 4.85 10.01
PVC 30.4 60 0.41 0.24 1.71 2.13 4.98 6.90 16.37
PVC 30.4 90 0.58 0.39 2.74 3.05 6.66 9.94 23.36
PVC 30.4 120 0.83 0.59 4.20 4.53 9.21 10.90 30.26
PVC 30.4 150 1.77 0.68 4.83 5.44 10.95 12.17 35.84

The experimental procedure is summarised as follows. Gran-
ular material was introduced into the rotary valve and entrained
by air flowing from the compressor mains. A specific air flow
rate was used to transport a sample of granular material through
the pneumatic conveying system for a given time (360 min). At
pre-defined time intervals (60 min), air flow and the rotary valve
were stopped and the granular material was emptied from the
system. A weight-size analysis was carried out by sieving on
a representative sample of the material. The procedure was re-
peated for different air flow rates using fresh granular material
samples for each separate experiment.
wall at the entrance varies throughout a cycle of rotation. This
results especially for granules of low flowability (i.e., PVC) in
severe attrition. Attrition was always accompanied with loud
noises and violent shaking of the device. As granules moved
through the rotary valve, attrition may also occur in the clear-
ance between the vanes and casing wall (Crutchley and Bridg-
water, 1997). Some attrition may be brought about by direct
impacts between the granules and rotary valve vanes or other
granules (Konami et al., 2002).
3.2. Rotary valve

The size of the attrition product formed was mainly in the

3. Results and discussion
3.1. Physical analysis of granular attrition due to rotary valve
The rotary valve was operated either as a stand-alone de-
vice or as part of a pneumatic conveying system. In the former
mode, attrition occurred at the exit of the rotary valve (depicted
attrition II in Fig. 1) while in the latter mode, attrition also oc-
curred at the entrance (depicted as attrition I in Fig. 1) to the
rotary valve. In particular, the gap between the vanes and casing
range 1.18–2.8 mm for PP granules and 1.18–3.35 mm for PVC
granules. It was deemed appropriate to use the golden section
principle to choose sieve size intervals for size analysis. The
golden section method is usually applied to problems of propor-
tional division of the whole on unequal harmonic parts. Using
this method of sectioning, the ratio of the length of the smaller
section (1 − x, say) to that of the larger one (x) is equal to the
ratio of the length of the larger section (x) to that of the whole
(1). The resulting golden section value is taken as x =0.618. As
the size distribution of the attrition product was unknown, the
3440 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

(a) (b)

(c) (d)

(e) (f)

Fig. 3. Particle size distribution obtained at various times in the attrition of granules PP: 2.8–3.35 mm, sample mass 938.17 g and rotary valve speed (a)
15.8 rpm; (b) 25.0 rpm; (c) 30.4 rpm; PVC: 3.35–4.1 mm, sample mass 742.42 g and rotary valve speed (d) 15.8 rpm; (e) 25.0 rpm; (f) 30.4 rpm.

golden section principle was deemed an appropriate method for
choosing sieve sizes in a narrow cut range. A random choice
of sieve sizes does not seem to be appropriate.
For PP in the size range 2.8–1.18 mm corresponding to a
size interval length of 2.8 − 1.18 = 1.62 mm, the golden section
length can be calculated as: 1.62 × 0.618 = 1.00 mm (golden
section value 0.618). Thus, the first sieve cut was calculated as:
1.18 + 1.00 = 2.18 mm. Based on this calculated value, a sieve
with the closest cut value of 2.00 mm, which was available in
our laboratory, was selected. Other sieve cuts were chosen in
a similar fashion and the results are presented in Fig. 2. The
relevant experimental data are listed in Table 2.
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3441

Fig. 4. Gwyn plots for sieve granules: sample mass (a) PP (2.8–3.35 mm): 938.17 g; (b) PVC (3.35–4.1 mm): 742.42 g; attrition product weight via rotation
number of rotary valve (c) PP (2.8–3.35 mm): 938.17 g; (d) PVC (3.35–4.1 mm): 742.42 g.

Fig. 2(a) shows the size distribution of attrited PP granules Table 3

obtained when the speed of the rotary valve was 25.0 rpm. It Gwyn function parameter for the rotary valve
is seen that there is a higher distribution of attrition product Material Rotary valve speed Parameters from Gwyn function
among the larger sieve cuts (> 1.18 mm) than in the lower (rpm)
ranges (< 1.18 mm). This can be logically linked to the gap size m (–) K/10−4 (g s−m )
between the vanes and casing wall, which equals the difference
PP 15.8 0.62 5.08
between R1 and R0 , 1 mm. Fig. 2(b) shows that the amount of 25.0 0.69 3.90
attrition product formed in each and every sieve cut increases (2.8–3.35 mm) 30.4 0.70 4.19
with increasing rotary valve speed. This is a result of higher PVC 15.8 0.84 0.52
attrition frequency and larger mechanical impacts between the 25.0 0.92 0.64
(3.35–4.1 mm) 30.4 0.94 0.76
granules and vanes at higher rotary valve speeds.
Fig. 2(c) shows the corresponding size distributions of attr-
ited PVC granules for a rotary valve speed of 25.0 rpm. The
observation the product is larger than 1.18 mm again pertains.
Fig. 2(d) shows that the amount of attrition product formed is especially so for the 1.41–2.36 mm sieve cut. In addition,
from PVC granules at each sieve cut also increases with in- PVC forms a larger proportion of products in the sieve cuts
creasing rotary valve speed. 0–1.18 mm and 1.18–1.41 mm. These observations point to the
Comparing the behaviour of the materials, for each sieve cut fact that PVC granules have higher attritability than the PP
PVC exhibits a smaller variation with rotary valve speed. This granules.
3442 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

Table 4
Attrition product size distribution analysis in the pneumatic conveying system

Granular material Air flow rate (l/min) Time (min) Sieve aperture (mm) Total percentage attrited

< 1.18 1.18–2.00 2.00–2.36 2.36–2.80 2.80–3.35

PVC 950 60 0.37% 1.23% 1.43% 2.85% 5.95% 11.83%

PVC 950 120 0.69 2.34 2.71 5.38 10.18 21.30
PVC 950 180 1.30 4.97 5.61 11.17 17.83 40.88
PVC 950 240 1.89 6.94 8.04 17.19 22.45 56.51
PVC 950 300 2.58 9.80 11.12 23.06 24.37 71.15
PVC 950 360 3.15 13.46 14.56 25.84 23.50 80.51
PVC 1100 60 0.61 1.92 2.13 4.65 8.83 18.13
PVC 1100 120 0.91 3.83 3.99 8.71 14.37 31.81
PVC 1100 180 1.37 5.79 6.04 13.17 17.56 43.93
PVC 1100 240 1.86 6.78 7.65 17.45 20.84 54.58
PVC 1100 300 2.40 8.96 9.66 20.96 21.04 63.02
PVC 1100 360 2.78 11.32 11.28 23.59 21.29 70.26
PVC 1600 60 0.57 2.62 2.39 3.87 9.34 18.79
PVC 1600 120 0.97 6.14 5.34 8.65 15.07 36.17
PVC 1600 180 1.89 9.89 8.84 14.32 18.44 53.38
PVC 1600 240 2.55 10.86 11.23 21.15 18.68 64.47
PVC 1600 300 3.29 15.02 13.36 22.08 18.25 72.00
PVC 1600 360 4.13 19.16 16.34 21.96 16.11 77.70

In summary, attrition in a rotary valve operating as a
stand-alone device tends to generate product sizes larger than
1.18 mm. This may be linked to the size of the gap between
the vanes and casing wall. Secondly, the amount of attrition
product across all sieve cuts generally increases with increas-
ing rotary valve speed. The specific size distribution depends
on the material characteristics.
Neil and Bridgwater (1994) argued that the size distribution
of attrition product can be represented by

G
d this aspect.
W = WT , (2)
dT
respect to rotary valve speed than PP. This can be seen more
clearly in Fig. 4(c),(d) which show the weight of attrition prod-
uct formed as number of rotations of the rotary valve increases.
It is seen that the attrition data for PP granules (Fig. 4(c)) col-
lapse onto a single line independent of the rotary valve speed
while those for PVC granules (Fig. 4(d)) lie on three differ-
ent lines corresponding to the three rotary valve speeds. This
means attrition of PVC is sensitive to strain rate in its at-
trition. This phenomenon must be due to a material depen-
dent property of PVC and shows that more work is needed on

where d is the particle diameter, dT is the initial particle di-
ameter, G is an exponent characterising the size distribution,
W is the mass of the attrited sample that has a size less than
d and WT is the mass of the attrited sample having a size less
than dT . They argue that Eq. (2) serves to define the amount of
material of every size formed in the process of attrition. Fig. 3
shows the size distribution of attrition products of both PP and
PVC according to Eq. (2); the data show good agreement with
the relation. Furthermore, the plots in each figure correspond-
ing to different times of attrition, other conditions being held
constant, show similar slopes.
Fig. 4(a),(b) shows that the attrition data for both materi-
als in the manner proposed by Gwyn (1969). The plots show
similar slopes irrespective of the speed of rotary valve used;
the Gwyn parameters obtained from the correlation are sum-
marised in Table 3. This is consistent with the observations of
Neil and Bridgwater (1994, 1999) in their work using annu-
lar cell. For both materials, the severity of attrition increases
with increasing rotary valve speed but the rate of attrition, ex-
pressed in this coordinate frame, remains constant with time.
On the other hand, the attrition of PVC is much greater with
3.3. Pneumatic conveying system
Here PVC material was used at three air flow rates
(950 l/min, 1100 l/min and 1600 l/min). A total of 18 tests each
lasting about one hour was conducted. The sieve cuts used
for size distribution analysis were 1.18, 2.00, 2.36, 2.80 and
3.35 mm given and the relevant experimental data are listed
in Table 4.
In the pneumatic conveying system, it has been established
that three different granular flow patterns may be formed (Rao
et al., 2001) depending on the hydrodynamic (solid–fluid in-
teractions) characteristics of the granular material and the air
flow rate (Yao et al., 2004). These flow patterns have similarly
been observed in the present study. When the air flow rate was
about 1600 l/min, granules were transported as a dilute and
homogenous phase. As the airflow rate was decreased to about
1100 l/min, the granular material tended to congregate into
clusters which appeared intermittently in the pipe. When the
air flow rate was decreased further to about 950 l/min, most
granules slid on the pipe wall as a settled layer of granular
material. On the other hand, with increasing attrition taking
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3443

place in the system, solid flow rate increased under constant

gas flow. Based on previous methods (Mathur and Klinzing,
1984; Yao et al., 2004), solid flow rates were measured at
three air flow rates with the total mass of granules used to be 30
1100 g. For intact particles, the solid flow rates measured were

Attrited weight (%)

33.63, 50.51, 63.84 g/s when the air flow rates were 950, 1100, 25

1600 l/min, respectively. However, following 6 h of attrition, 20

the solid flow rates were enhanced to 37.74, 53.84, 70.11 g/s,
15
respectively. Attrition thus affects the hydrodynamics of the 6
granular flow. 10 5
4
The size distribution of the attrition product obtained is il- 5 3 )
2 (h
lustrated in Fig. 5, which shows the size distribution obtained m
e
0 1 Ti
with the air flow rates of 950, 1100 and 1600 l/min and a fixed

5
0

0
.1

.8

.3
.3
.0
rotary valve speed of 25.0 rpm. As with the rotary valve alone

<1

-2

-2
-2

-3
18

00

36

80
(Fig. 2(c)), the attrition product shows a higher distribution in

1.

2.

2.

2.
the larger sieve cuts (> 1.18 mm) than in the smaller sieve cuts (a) Sieve aperture (mm)
(< 1.18 mm). This further supports the previous claim that the
minimum size of attrited granules which can be produced by
attrition within the rotary valve is determined by the size of the
gap between the vanes and casing wall (1 mm, Fig. 1). How-
ever, it is also noted that such a trend becomes weaker with
25
increasing air flow rate. For example, when the airflow rate
Attrited weight (%)

was 950 l/min (Fig. 5(a)), attrition products were mostly larger 20
than 2.36 mm in sizes while at 1600 l/min (Fig. 5(c)), the dis-
15
tribution became more uniform over the range 1.18–3.35 mm.
6
Here attrition occurs predominantly in the rotary valve, a high 10 5
air flow rate may lead to more severe attrition in the device. 4
)
5 3 (h
It is because product, being necessarily smaller than the intact 2 m
e
Ti
granules, is transported at higher velocities along the convey- 0
1
ing pipes and so undergoes further attrition subsequently. Thus,
8

35
.1

.3

.8
.0

3.
higher air flow rates would generally result in higher distribu-
<1

-2
-2
2

0-
8-

36
00
1

8
2.

2.
1.

2.
tions in the smaller sieve cut ranges and attrition products in (b) Sieve aperture (mm)
such ranges are more effective at increasing the distributions in
even smaller size ranges.
Fig. 6 shows the attrition product size distribution plotted
according to Eq. (2) for the three different air flow rates. The
data exhibit good agreement with the relation. This further sup-
25
ports the adequacy of Eq. (2) for describing the evolution of
Attrited weight (%)

the particle size distribution as a whole during attrition. 20

Fig. 7 shows that the attrition data obtained in this part of
the study are consistent with the Gwyn correlation for the air 15

flow rates 1100 and 1600 l/min. The parameter m, as presented 10

6
5
in Table 5, is much the same for these two cases. However, 4 )
for the air flow rate 950 l/min, the data are not similar and 5 3 (h
2 e
m
the parameter m is substantially higher. The origin lies in the
0
1 Ti
relation between the hydrodynamic behaviour of the granular
8

35
.1

.0

.3

.8

material and air flow rate in the pneumatic conveying system.

.
<1

-2
-2

-3
-2
36
18

00

80
1.

2.

2.

2.

At the low air flow rate, granules are transported relatively
slowly along the conveying pipe as a settled bed resulting in a
low level of attrition. At the same time, due to low flowability,
a fairly large amount of granular material accumulates at the
exit of the rotary valve, giving rise to significant attrition at this
location. The overall effect is an enhanced attrition rate.
In summary, the attrition of material in a rotary valve operat-
ing as part of a pneumatic conveying system can be well char-
acterised by Gwyn function while it is seen differently from
that when it is operated as a stand-alone device. At high air flow
Sieve aperture (mm)
(c)
Fig. 5. Product (pneumatic conveying loop using PVC) size distribution
obtained at an airflow rate: (a) 950 l/min; (b) 1100 l/min; (c) 1600 l/min.
rates (> 1100 l/ min), the attrition data could be well described
by the Gwyn function with a single value for the parameter (m)
while at low air flow rates (950 l/ min), deviations in the pa-
rameter value may be observed. As such, the Gwyn parameter
3444 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451
(a)
(b)
(c)
Fig. 6. Particle size distribution obtained at various times with air flow rate
(PVC): (a) 950 l/min; (b) 1100 l/min; (c) 1600 l/min.
(m) may be important in characterising attrition behaviour un-
der certain operating conditions used in the present pneumatic
conveying study.
It may be noted that, except at low air flow rates, the Gwyn
parameter m for PVC presented in Table 5 shows little differ-
ence to that in Table 3 for cases where the rotary valve is oper-
ated as a stand-alone device. It is suggested that under certain
Fig. 7. Gwyn plots for granules 3.35–4.1 mm as a function of air flow rate,
sample mass 1100 g.
Table 5
Gwyn function parameter of the rotary valve in the pneumatic conveying
system (PVC)
Air flow rate (l/min) Parameter from Gwyn function
m (–) K/10−4 (g s−m )
950 1.06 0.20
1100 0.81 2.41
1600 0.89 1.27
operating conditions, the Gwyn parameter m is approximately
constant for the attrition of PVC in the rotary valve.
3.4. Product shape distribution
Granular attrition arising from mechanical action produces
fragments of different shapes (Meloy, 1988). Watano and
Miyanami (1995) developed a particle image probe compris-
ing a CCD camera and an image processing system for on-line
monitoring for dynamic control of granule size distribution
and shape in a fluidised bed. Bortzmeyer and Goimard (1996)
focused on the attrition properties of calcium carbonate ag-
glomerates obtained by uniaxial compaction and compared the
mechanical and attrition properties of three CaCO3 powders of
different shapes and sizes. However, the relationship between
granular shape and mechanical action has not received proper
attention in the literature. Here, we provide an analysis of the
attrition process and mechanism taking place in the rotary
valve by characterising the shapes of the attrition product.
Attrition of PVC with an original shape of a cylinder (CY)
was conducted in the rotary valve as part of a pneumatic
conveying system and samples of product taken. Each sieve
cut from the attrition product was sampled randomly (about
1 g/sample) and photographed using a particle size/shape an-
alyzer (Analytical Technologies Pte Ltd, Singapore) (Fig. 8).
It was found that the geometry of the attrition product can
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3445

Fig. 8. Microscope image of the attrition product (each group sampled about 1 g, PVC): (a) 1.18–2.00 mm; (b) 2.00–2.36 mm; (c) 2.36–2.80 mm; (d)
2.80–3.35 mm; (e) > 3.35 mm.

be classified conveniently by five basic shapes as defined in
Fig. 9: half-cylinder (HCY), triangular-column (TGC), cone
(CN), trapezoidal-column (TPC) and cube (CU), with each ba-
sic shape being further characterised by a length (L), width (I)
and height (H). This seems reasonable as the HCY and TPC
shapes require only one shearing action on the original granule
for their formation while others such as TGC, CN and CU
require at least 2, 3 and 4 such actions, respectively. It was ob-
served that attrition products with sizes smaller than 2.00 mm
(Fig. 8(a)) were mostly debris with very complex shapes formed
out of cut corners from larger granules. These were scarce and
are not included in the present treatment.
3446 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

(a) (b)

(c) (d)

(e) (f)

Fig. 9. Typical particle shapes formed during granule attrition: (a) half-cylinder (HCY: ns = 1); (b) triangular-column (TGC: ns = 2); (c) cone (CN: ns = 3);
(d) trapezoidal-column (TPC: ns = 1); (e) cube (CU: ns = 4); (f) cylinder (CY: ns = 0).

For large sieve cuts (> 3.35 mm) (Fig. 8(e)), the granules 80

are only minimally damaged with small portions such as cor- HCY
TPC
TGC
CU
CN
CY
ners cut from the original parent granules. For the sieve cut
60
2.80–3.35 mm (Fig. 8 (d)), most of the granules forming the
Attrited shape (%)

half cylinder (HCY) or trapezoidal-column (TPC) shape. In

the sieve cut 2.36–2.80 mm (Fig. 8 (c)), the granules become
40
more irregular and include the cone (CN) and triangular-column
(TGC) in addition to HCY and TPC. Formation of some of
these shapes requires two or more shearing actions on the orig- 20
inal intact granule. For the sieve cut 2.00–2.36 mm (Fig. 8 (b)),
the attrited granules would have suffered several shears and
exhibit various irregular shapes. Fig. 10 shows the shape dis- 0
2.00 - 2.36 2.36 - 2.80 2.80 - 3.35 > 3.35
tribution of a unit weight of sample randomly selected from
Sieve aperture (mm)
the attrition product. The data indicate that for all sieve cuts,
HCY and TPC are the most frequently observed while CU is Fig. 10. Attrition product shape distribution for different size cuts (per unit
the least common. Granules from the lowest sieve cuts have weight, PVC).
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3447

Fig. 11. Product (PVC) shape distribution displayed as (a) length–height; (b) length–width; (c) length–size; (d) length–length ratio. Original: particle size
3.35–4.1 mm.

necessarily undergone multiple attrition processes and so would
exhibit complex geometries and shapes. As such, with respect
to the present system, it seems that such granules have almost
equal likelihood of possessing any one of the five basic shapes,
as depicted in Fig. 10.
Fig. 11 shows the length (L), width (I) and height (H) of
product randomly chosen from each sieve cut. In these measure-
ments, granules were placed on a flat surface with the largest
face as the base; the length and width were then taken to be
the longer and shorter sides of the base, respectively, while the
height was defined by the vertical distance from the base to the
highest tip. As attrition progresses, granules become smaller
in height and width. These in turn lead to an overall decrease
in the general size scale defined as L × I × H. Further, by
comparing the ratio of length-to-height and length-to-width, it
is proposed that attrition occurs anisotropically and preferen-
tially along the directions defined by the height and width of
the granules. A parameter termed length-ratio was thus defined
to represent this idea
length
Length-ratio = . (3)
min(height, width)
Fig. 11(d) shows the length-ratio of attrited granules shows
that attrition tends to form products with higher length-ratios.
In other words, the attrition products formed in a rotary valve
develop a narrow and elongated morphology. Furthermore, the
data are more scattered for smaller products.
3448 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451

Watano and Miyanami (1995) studied granular shapes using
a “shape factor” defined by
 = P 2 /4 · S,
where S is the projected area and P is the perimeter of this
projected area. Several geometrical shape factors  is 1.00 if
a circle, 1.27 if a square and 1.65 if an equilateral triangle.
The shape factors for the samples shown in Fig. 8 were calcu-
lated automatically from the particle size/shape analyzer and
are plotted in Fig. 12. It is seen that the points on Fig. 12 are
significantly more scattered for products from the lower-sized
range and this implies that the shapes of these smaller granules
are made up of complex combinations of different geometries.
To characterise products shape, the concepts of shear fre-
quency, fs and attrition frequency, f as defined in Eqs. (5) and
(6), respectively, are proposed.
number of shearing actions required to form the ith geometry
(Fig. 9) and M is the total number of basic shapes. For exam-
ple, attrited granules with sizes in the range 2.80–3.35 mm are
(4) composed of 6 (M = 6) kinds of geometry with corresponding
shape frequency (per unit weight) fp(i) (i =1, 2, . . . , M) listed
in Table 6. The granular shear frequency (per unit weight) may
be calculated as
fs(2.8–3.35) = 40.03% · 1 + 13.33% · 2 + 4.41% · 3
+ 31.12% · 1 + 4.44% · 4 + 6.67% · 0 = 1.29.
For other size cuts (> 2.00 mm), the shear frequencies per unit
weight were calculated in a similar fashion and summarised in
Table 6.

N
f= fw(i) · fs(i) , (6)
i=1


M fw(i) (i = 1, 2, . . . , N ) is the percentage by weight of attrited
fs = fp(i) · ns(i) , (5) granules in the ith sieve cut, fs(i) (i = 1, 2, . . . , N ) is the shear
i=1 frequency of the ith sieve cut calculated from Eq. (5) and N is
where fs the shear frequency per unit weight, fp(i) (i = the number of sieve cuts used to analyse the attrition product.
1, 2, . . . , M) is the shape frequency of the attrited granules For example, when the air flow in the pneumatic conveying
having the ith geometry, ns(i) (i =1, 2, . . . , M) is the minimum system was 950 l/min and the attrition product obtained after
the first hour was sieved into five cuts as listed in Table 4, the
attrition frequency for attrited granules with sizes larger than
2.00 mm (N = 4) could be calculated using the shear frequency
20 >3.35 mm
2.8-3.35 mm
2.36-2.80 mm
2.00-2.36 mm
1.5
15 950 L/min
1100 L/min
1600 L/min
Shape factor

Attrition frequency (f )

1
10

5 0.5

0 0
1 2 3 4 5 6
2 4 6
Length (mm) Time (h)

Fig. 12. Shape factors for various sieve cuts (each group sampled about 1 g, Fig. 13. Attrition frequency per unit weight of granules with sizes larger than
PVC). 2.00 mm (pneumatic conveying loop using PVC).

Table 6
Attrition product shape distribution for different size cuts (PVC)

Size interval (mm) Shape frequency (%) fs

HCY TGC CN TPC CU CY

> 3.35 7.69 – – 34.62 – 57.69 0.42

2.80–3.35 40.03 13.33 4.41 31.12 4.44 6.67 1.29
2.36–2.80 38.81 13.45 22.36 22.39 2.99 – 1.67
2.00–2.36 21.45 18.73 19.64 29.46 10.72 – 1.90
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451 3449

60 0.8 60 0.8
Attrition weight Attrition weight
Attrition frequency Attrition frequency
Attrition weight (%)

Attrition frequency (f)

Attrition weight (%)

15.8 rpm

Attrition frequency (f)

25.0 rpm
40 0.6 40 0.6

20 0.4 20 0.4

0 0.2 0 0.2
60 90 120 150 180 210 240 40 80 120 150 200
(a) Time (minutes) (b) Time (minutes)

60 0.8 120 1.2

Attrition weight Attrition weight
Attrition frequency Attrition frequency
950 L /min

Attrition weight (%)

30.4 rpm
Attrition weight (%)

Attrition frequency (f)

Attrition frequency (f)
90 0.9
40 0.6

60 0.6

20 0.4
30 0.3

0 0.2 0 0
93 06 09 01 20 150 60 120 180 240 300 360
(c) Time (minutes) (d) Time (minutes)

120 1.2 120 1. 2

Attrition weight Attrition weight
Attrition frequency Attrition frequency
1600 L/min
Attrition frequency (f)

1100 L/min
Attrition weight (%)

Attrition frequency (f)

90 0.9 90 0. 9
Attrition weight (%)

60 0.6 60 0. 6

30 0.3 30 0. 3

0 0 0 0
60 120 180 240 300 360 60 120 180 240 300 360
(e) Time (minutes) (f) Time (minutes)

Fig. 14. Comparison of time evolution of attrition frequency and attrition product weight (PVC): for single rotary valve at three speeds: (a) 15.8 rpm;
(b) 25.0 rpm; (c) 30.4 rpm; in a pneumatic conveying system at three airflow rates: (d) 950 l/min; (e) 1100 l/min; (f) 1600 l/min.

as listed in Table 6 of granules which have undergone attrition. It shows that, in

f(950–1h) = 1.43% · 1.90 + 2.85% · 1.67 + 5.95% · 1.29 all cases both for a single rotary valve and the pneumatic con-
veying system, attrition frequency increases with time and the
+ 88.17% · 0.42 = 0.52.
evolution exhibits good agreement with that of attrition weight
The attrition frequencies were calculated and are presented (percentage).
in Fig. 13. It shows that for all cases in the pneumatic convey- To evaluate the attrition progress, attrition frequency is cal-
ing system the attrition frequencies increase with time. Further- culated by the cumulative of each sieve cut. As a result, for
more, for low air flow rate (e.g. 950 l/min) the ratio is seen to be all cases conducted in a rotary valve (operating both as a
higher than the other cases. This is consistent with the trend in stand-alone device and as part of a pneumatic conveying sys-
Gwyn parameter values obtained by correlating the experimen- tem), the calculation of attrition frequency agrees well with
tal data with the Gwyn function (Fig. 7). Attrition processes experimental data as shown in Fig. 14. As both experimental
are quantitatively described by attrition frequency in Fig. 14 data and the calculated attrition frequencies in the figure are
and the results are compared with the percentage by weight cumulative quantities, both are expected to show monotonic,
3450 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451
non-decreasing variations with respect to time. However, we
would like to emphasise the close similarities in trends and
shapes between the two curves in each panel of Fig. 14 which
do not arise naturally out of any monotonic functions. The pro-
posed concept of attrition frequency is a macroscopic quantity
and, as shown in the present study, may be compared directly
with experimentally measured attrition weight values. This con-
cept is in turn built on that of shear frequency which is related
to the shapes of particles and so may be viewed upon as a mi-
croscopic quantity.
Physically, the process of attrition arises as a result of me-
chanical action on solid granules. The larger the amount of
such mechanical action, the larger the amount of attrition prod-
ucts formed. In the present work, such mechanical action has
been quantified and expressed as a function of shear and at-
trition frequency as defined in Eqs. (5) and (6). These quan-
tities have in turn been defined such as to be closely related
to important physical attributes of the granules which undergo
the attrition process, such as their size and shape. The ob-
served close similarity in the time evolution of attrition fre-
quency and the experimentally measured extent of attrition
shows that the concepts proposed here are sound and useful
for characterisation of attrition processes in generally complex
systems.
4. Conclusions
The attrition processes occurring in a rotary valve operating
either as a stand-alone device or as part of a pneumatic con-
veying system were investigated.
The attrition product generated from the rotary valve oper-
ating as a stand-alone device was mainly of the large size than
the smaller ones. The amount of product increased with in-
creasing speed of the rotary valve. The attrition data obtained
were found to be in good agreement with the Gwyn correlation,
the values of the Gwyn parameter remained substantially con-
stant irrespective of the speed of the rotary valve. The weight
of attrition product formed increases as number of rotations
of the rotary valve increases. The attrition data for PP gran-
ules were independent of the rotary valve speed while those
for PVC granules depended on the rotary valve speeds used in
this study.
When the rotary valve was operated as part of a pneumatic
conveying system, the product similarly showed higher distri-
butions in the larger sieve cuts. However, smaller attrited prod-
ucts would be transported at higher velocities along the con-
veying pipes and so undergo further attrition in the rotary valve
due to increasing solid flow rates. As a result, higher distribu-
tions in the smaller sieve cuts were observed in this mode of
operation than in the previous mode. The attrition data were
in good agreement with the Gwyn correlation while at low air
flow rate the Gwyn parameter value was found to be higher
than those for higher air flow rates. The reason for this phe-
nomenon can be explained in terms of the relation between the
hydrodynamic behaviour of the granular material and air flow
rate in the pneumatic conveying system. At a low air flow rate,
due to low flowability, a fairly large amount of granular mate-
rial accumulates at the exit of the rotary valve, giving rise to
significant attrition at this location.
The attrition product tended to assume a narrow and elon-
gated morphology. As attrition progresses, the granular mate-
rial becomes more complex in shape and may eventually show
equal likelihood of exhibiting any of several basic shapes de-
fined in this study. The quantitative confirmation of this point
may be the focus of a subsequent study. The concepts of shear
frequency and attrition frequency were proposed and used for
the characterisation of the attrition process. In this fashion, the
variation of attrition frequency with respect to time exhibited
a parallel correspondence with the percentage by weight of
granules which had undergone attrition both for single rotary
valve and in the pneumatic conveying system. Thus, the pro-
posed concepts of shear and attrition frequencies seemed useful
for characterisation of attrition processes in generally complex
systems.
These studies demonstrate that the principles of attrition in
the rotary valve, when evaluated over a wide range of attrition
product sizes and shapes, are unified in a remarkably simple
manner. It is also proposed that the novel concepts and approach
used to account for shapes of attrition products introduced in
the present study may be further developed into a more general
and widely applicable granular attrition theory.
Notation
CN attrition product shaped as cone
CU attrition product shaped as cube
CY original particle shape cylinder
HCY attrition product shaped as half-cylinder
TGC attrition product shaped as triangular-column
TPC attrition product shaped as trapezoidal-column
d diameter of sample, mm
dT largest sized particle, mm
f attrition frequency, dimensionless
fp shape frequency, dimensionless
fs shear frequency, dimensionless
fw attrition product weight percentage, dimensionless
G Schuhmann size distribution modulus, dimension-
less
H attrition product height, mm
I attrition product width, mm
K proportionality constant in the Gwyn formulation,
s−m
L attrition product length, mm
m exponent in the Gwyn formulation, dimensionless
M total number of attrition product basic shapes, di-
mensionless
ns minimum number of shearing actions required to
form product into a specific shape, dimensionless
N number of sieved cut used, dimensionless
P projected area perimeter, m
S projected area, m2
t attrition time, s
 J. Yao et al. / Chemical Engineering Science 61 (2006) 3435 – 3451
W mass degradation, g
WT estimated overall mass degradation, g
Greek letter
 shape factor, dimensionless
Acknowledgements
This project is supported by the National University of Sin-
gapore and Singapore-MIT Alliance under the grant numbers
R279-000-095-112 and MEBCS project-003, respectively.
CHW thanks the Chemical Engineering Department, Cam-
bridge University for a visiting appointment during the period
April–July 2004.
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