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N
"
N
(t
N
(10 s)
N
(t
N
"10 s)
. (1)
Regarding this de"nition, the high liquid holdup at a hlf-
time of 10 s serves as a reference to examine the e!ect of
decreasing hlf-time on the high liquid holdup. A plot of
2608 J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614
Fig. 7. E!ect of the hlf-time on the relative high liquid holdup
(;
J@
"0.0035}0.0077 m s\; ;
JN
"0.0059}0.0128 m s\; ;
E
"0.03}
0.30 ms\; t
@
"20 s).
Fig. 8. Comparison of liquid holdup during high liquid feed rate with
liquid holdup during trickle #ow (;
J
"0.0059}0.0128 m s\; ;
E
"
0.03}0.30 m s\; t
N
"2}10 s; t
@
"20 s).
Fig. 9. Velocity of the moving liquid front (t
@
"20 s; t
N
"1}10 s; pack-
ing material"6.0 mm spheres).
the relative liquid holdup as a response to decreasing
hlf-times is provided in Fig. 7. In this "gure it is noticed
that, except for hlf-times of 1 s and less, no e!ect of the
hlf-time is recognized. The liquid feed is probably not
perfectly square-wave cycled since some delay in the
secondary feed line is inherently present due to the time
needed for the acceleration of the liquid. For very short
hlf-times, the high liquid feed is ended before it is fully
developed. Hence for hlf-times of 1 s and less, the high
liquid holdup which should be reached during cycled
liquid feed is not entirely accomplished.
As seen in the foregoing paragraph, a certain high
liquid holdup is reached as the result of the additional
liquid feed. This high liquid holdup is probably identical
to the liquid holdup during steady-state operation at
a steady liquid #ow rate, equivalent to the high liquid
feed rate. A comparison of the high liquid holdup during
cycled liquid feed with the liquid holdup during constant
liquid feed is made in Fig. 8. Due to cycling the liquid
feed, the liquid holdup varies between two values resem-
bling the liquid holdup obtained during steady-state op-
eration at comparable liquid feed rates.
4.2. Continuity shock waves
By evaluating the time lag between the two signals
from neighboring conductivity probes, it is possible to
evaluate the velocity of the moving liquid front, resulting
from the step-change in liquid feed rate. The experi-
mentally determined linear velocity of the liquid front is
plotted in Fig. 9 as a function of the super"cial gas
velocity for 6.0 mm spheres as packing material. The
velocity of this moving liquid front increases both with
increasing gas #ow rate and with increasing di!erence
between pulse and base liquid #ow rate. The velocities of
the moving liquid front, altering roughly between 0.1 and
0.2 m s\, are much higher than the linear liquid vel-
ocities (super"cial liquid velocity divided by liquid hold-
up) which vary between 0.02 and 0.08 m s\. Hence it can
be concluded that due to cycling the liquid feed some
kind of waves are initiated in the column.
To examine the e!ect of the hlf-time on the velocity of
the moving liquid front, similar to the relative high liquid
holdup, the relative wave velocity can be de"ned as
<
U
"
<
U
(t
N
(10 s)
<
U
(t
N
"10 s)
. (2)
A plot of the relative wave velocity versus the hlf-time is
shown in Fig. 10. Analogous to liquid holdup during high
liquid #ow rate, it is noticed that for hlf-times of 1 s and
less, the velocity of these waves is somewhat less than the
values corresponding to hlf-times above 1 s.
It seems useful to investigate the possibility of the
formation of continuity shock waves resulting from the
step change in liquid #ow rate. Continuity waves occur
whenever the #ow rate of a substance depends on the
amount of that substance which is present. Continuity
waves often emerge in systems where gravity and pres-
sure drop are balanced against drag forces, as is the case
with liquid #ow in packed beds. One steady-state value
simply propagates into another one and there are no
J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614 2609
Fig. 10. E!ect of the hlf-time on the relative shock wave velocity
(;
J@
"0.0035}0.0077 m s\; ;
JN
"0.0059}0.0128 m s\; ;
E
"0.03
}0.30 m s\; t
@
"20 s).
Fig. 11. Comparison of the experimentally determined and calculated
shock wave velocity (;
J@
"0.0035}0.0077 m s\; ;
JN
"
0.0059}0.0128 m s\; ;
E
"0.03}0.30 m s\, t
@
"20 s; t
N
"2}15 s).
Fig. 12. Enlargement of the pulsing #ow regime by cycling the liquid
feed (t
@
"20 s; t
N
"0.5}15 s; packing material: 3.0 mm spheres).
dynamic e!ects of inertia or momentum (Wallis, 1969).
Waves can either propagate continuous changes in some
variables or can involve a step change or "nite discon-
tinuity. The later are called shock waves. According to
Wallis (1969), the velocity of a shock wave, derived from
continuity considerations obeys the following equation:
<
U
"
;
JN
!;
J@
N
!
@
. (3)
According to Eq. (3), the shock wave velocity is directly,
related to the di!erence between liquid feed rates and the
di!erence between the resulting values of the liquid hold-
up.
To calculate the shock wave velocity, the experi-
mentally determined liquid holdup data during trickle
#ow are used. This is justi"ed by the fact that the liquid
holdup varies between the values, which are obtained
from steady-state experiments, as shown in Fig. 8. The
solid lines in Fig. 9 depict the calculated velocity of the
moving liquid front conform Eq. (3). A good agreement
exists between experimentally and calculated values, as
well qualitatively as quantitatively. A comparison of all
the experimental data with calculated values is shown in
Fig. 11. Shock wave velocities corresponding to hlf-times
of 1 s and less are not shown here for reasons presented
earlier. The overall agreement is satisfactory for the
whole range of shock wave velocities. The accuracy of the
calculated values increases with increasing di!erence be-
tween high and low liquid holdup. Since this di!erence
varies in a narrow range between 0.03 and 0.1, it is very
important to use very accurate values of the liquid hold-
up, because this has a large e!ect on the calculated shock
wave velocity.
In summary, due to the step-change in liquid feed rate,
continuity shock waves are initiated in the column. As
a result, the column can be split up into two regions of
di!erent liquid holdup, both corresponding to steady-
state conditions. In other words, at the same time two
di!erent steady-state conditions are present in the col-
umn. These steady-state conditions are separated by
a moving boundary of which the velocity can be cal-
culated using accurate liquid holdup data obtained dur-
ing steady-state operation at equivalent liquid feed rates.
5. Liquid-induced pulsing 6ow
5.1. Enlargement of the pulsing yow regime
Fig. 12 provides the results of the enlargement of the
pulsing #ow regime by cycling the liquid feed for 3.0 mm
glass spheres as packing material. Similar results are
found for the 6.0 mm glass spheres as packing material.
The solid line, denoting the transition boundary to self-
generated pulsing #ow, is taken at approximately 0.1 m
from the bottom of the column. In Fig. 12, for each series
of data, the hlf-time increases in the downward direction
2610 J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614
Fig. 13. The for induced pulsing #ow necessary super"cial gas velocity
as a function of the hlf-time (t
@
"20 s; packing material: 3.0 mm
spheres).
Fig. 14. Example of the measured liquid holdup during liquid-induced
pulsing #ow (;
J@
"0.0035 m s\; ;
JN
"0.0077 m s\; ;
E
"
0.29 m s\; t
@
"20 s; t
N
"3 s; packing material"6.0 mm spheres).
denoted by the arrow. This means that with decreasing
hlf-time, higher gas velocities are necessary to obtain
pulsing. It is possible to induce pulses at average liquid
#ow rates, generally associated with trickle #ow during
steady-state operation. Hence, it can be concluded that
although throughputs of liquid are equal, the prevailing
#ow regime is pulsing instead of trickle #ow. The advant-
ages associated with pulsing #ow may be utilized to
enhance mass and heat transfer rates resulting in im-
proved reactor performance. Moreover, with liquid-in-
duced pulsing #ow longer contact times can be achieved
compared to self-generated pulsing #ow, while average
liquid #ow rates are reduced.
The observation that higher gas #ow rates are required
to induce pulses when hlf-times decrease, is presented
more pronounced in Fig. 13. In this "gure, the necessary
gas velocity is plotted as a function of the pulse feed time
for some of the results presented in Fig. 12. At relative
long hlf-times, the required gas velocity equals the velo-
city needed for transition to self-generated pulsing #ow at
the bottom of the column. However for relatively short
hlf-times, a higher gas velocity is necessary to initiate
pulsing #ow. This gas #ow rate increases with decreasing
hlf-times, although the cycled liquid feed rates remain
constant. These results indicate that not a combination of
gas and liquid #ow rates as such determines whether
pulses are initiated or not, but some other parameter has
to be included.
5.2. The process of liquid-induced pulsing yow
Due to the step-change in liquid feed rate, continuity
shock waves are initiated in the column. This results in
the appearance and downward movement of a liquid-rich
region. In Fig. 14, an example of the liquid holdup during
liquid-induced pulsing #ow at two neighboring conduct-
ivity probes is plotted. In the signal taken at 0.5 m from
the top of the column no pulse is present, while in the
signal taken at 0.7 m from the top evidently a pulse is
visible. Hence it can be concluded that pulses are in-
itiated in the liquid-rich region.
The length of the liquid-rich region can readily be
calculated by
l
U
"<
U
t
N
. (4)
For relatively long hlf-times, the column will eventually
be "lled entirely with the liquid-rich region, as schemati-
cally shown in Fig. 15a. In this case the necessary gas
velocity for pulse formation equals the velocity needed to
obtain self-generated pulsing #ow at the bottom of the
column. For short enough hlf-times, the length of the
liquid-rich region is less than the column height. As
a result the column can now be divided into two zones of
di!erent liquid holdup. With decreasing hlf-time, the
length of the liquid-rich region decreases, as schemati-
cally shown in Fig. 15b}d. With decreasing hlf-times and
hence decreasing length of the liquid-rich region, increas-
ing gas #ow rates are necessary to obtain pulsing #ow.
A similar phenomenon was observed for self-generated
pulsing #ow where the point of pulse inception was found
to move upwards with increasing gas #ow rate. As well
for self-generated pulsing #ow as for liquid-induced
pulsing #ow, there seems to be a relationship between
necessary gas #ow rate and available length for pulse
formation.
It is also noticed in Fig. 14, pulses are initiated at the
front of the liquid-rich region. This is a general observa-
tion during liquid-induced pulsing #ow. In Fig. 15 the
point of pulse inception during liquid-induced pulsing
#ow is visualized. At relative large hlf-times, just as soon
as the column is entirely "lled with the liquid-rich region,
pulses are initiated at the bottom of the column. For
relative short hlf-times, the point of pulse inception
moves upwards in the column with decreasing length of
the liquid-rich region. Pulses are observable just as soon
as the entire liquid-rich region is present in the column.
J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614 2611
Fig. 15. Schematic representation of the in#uence of the hlf-time on the
liquid distribution in the packed bed and the point of pulse inception
during liquid-induced pulsing #ow.
Fig. 16. Example of the measured liquid holdup during liquid-induced
pulsing #ow (;
J@
"0.0035 m s\; ;
JN
"0.0128 m s\; ;
E
"
0.26 m s\; t
@
"20 s; t
N
"2 s; packing material"6.0 mm spheres).
Considering the fact that su$cient length for pulse
formation must be available, pulses are always initiated
in the lower part of the liquid-rich region, at the moment
the entire liquid-rich region is present in the column. This
is also observed visually. Once the liquid-rich region
enters the column disturbances are present in the liquid-
rich region. However these disturbances do not growinto
detectable pulses. This occurs only as the high liquid feed
is ended, when the liquid-rich region is completely pres-
ent in the column.
Because the velocity of the initiated pulses is much
higher than the shock wave velocity, pulses will eventual-
ly move out of the liquid-rich region. Occasionally the
initiated pulses fade away when moving out of the
liquid-rich region, but in most cases the pulses remain
stable. An example of the later case is shown in Fig. 16, in
which the liquid holdup during liquid-induced pulsing
#ow at the two neighboring conductivity probes is plot-
ted. It is clearly seen that the initiated pulses have moved
out of the liquid-rich region, but remain stable. However
while the length of the column is rather short, it cannot
be assured at this moment if pulses remain stable in
columns of longer length.
5.3. Necessary gas yow rate
As described previously, as well for self-generated puls-
ing #ow as for liquid-induced pulsing #ow, there is a rela-
tionship between necessary gas #ow rate and available
length for pulse formation. For self-generated pulsing
#ow this results in the upward movement of the point of
pulse inception with increasing gas #ow rate. Neverthe-
less, this point of pulse inception never reaches entirely
the top of the column. The upper part of the column does
not actively participate in the process of pulse formation.
It is likely to expect that this part of the column is needed
to reach the necessary distribution of the phases. How-
ever, to accomplish a relationship between available
length for pulse formation and gas #ow rate, it is required
to know the length of this distribution zone. With liquid-
induced pulsing #ow, the available length for pulse
formation is externally controlled by the hlf-time. This
provides the possibility to determine the length of the
distribution zone. Referring back to Fig. 13, we can
identify a certain critical hlf-time. The critical hlf-time is
de"ned as the hlf-time at which higher gas velocities
compared to those needed to obtain self-generated puls-
ing #ow at the bottom of the column, are required for
pulse induction. The length of the liquid-rich region
corresponding to the critical hlf-time can be readily cal-
culated by multiplying the critical hlf-time with the shock
wave velocity. A plot of this critical length of the liquid-
rich region is given in Fig. 17. The critical lengths are
roughly constant and 0.15 m less compared to the height
of the packed bed for both packing materials. It seems
that the upper 0.15 m of the packed column is not active-
ly participating in the process of pulse formation.
Keeping in mind, that the "rst 0.15 m do not partici-
pate in the process of pulse formation, it is possible to
establish the interdependence between gas #ow rate and
available length for pulse formation for self-generated
pulsing #ow. The data in Fig. 5, simply have to be shifted
0.15 m towards lower distances from the top of the col-
umn. Additionally, the x-coordinate from Fig. 13 can be
transferred from hlf-times to length of liquid-rich regions
by multiplying the hlf-time with the calculated shock
wave velocity. Subsequently, the relationship between the
necessary gas velocity and available length for pulse
formation for both self-generated and liquid-induced
pulsing #ow is established. A comparison of these rela-
tionships for 3.0 mm glass spheres as packing material is
presented in Fig. 18. The data of self-generated and
liquid-induced pulsing #ow coincide. Note that in
the legend of Fig. 18, only high liquid #ow rates are
mentioned because pulses are initiated in the liquid-rich
region. Low liquid #ow rates solely participate in the
resulting shock wave velocity and thus in the length of
the liquid-rich region.
2612 J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614
Fig. 17. Critical length of the liquid-rich region.
Fig. 18. Comparison of the relationships between necessary gas velo-
city and available length for pulse formation for self-generated and
liquid-induced pulsing (solid points: self-generated pulsing #ow; open
points: liquid-induced pulsing #ow).
Fig. 19. Comparison between necessary super"cial gas velocity for
self-generated and liquid-induced pulsing #ow at equivalent available
lengths for pulse formation (;
J@
"0.0035}0.0077 m s\; ;
JN
"
0.0059}0.0128 m s\; t
@
"20 s; t
N
"2}8 s).
Fig. 20. Number of pulses generated during one liquid feed cycle as
a function of the length of the liquid-rich region (packing mater-
ial"3.0 mm spheres).
In Fig. 19 a comparison of the super"cial gas velocities
required for self-generated respectively liquid-induced
pulsing #ow at equal available lengths for pulse forma-
tion is presented for all the performed experiments. The
solid line denoting the necessary gas velocity for self-
generated pulsing #ow is obtained by intrapolation of the
modi"ed results of Fig. 5, considering the fact that the
point of pulse inception during self-generated pulsing
#ow could only be measured at "xed points along the
column axis. From the data of Fig. 19, it is concluded
that the interdependence between necessary length for
pulse formation and super"cial gas velocity is equivalent
for both self-generated and liquid-induced pulsing #ow.
5.4. Pulse frequency
Another feature of liquid-induced pulsing #ow is the
possibility to tune the pulse frequency and therefore the
time constant of the pulses. In Fig. 20, the number of
pulses generated during one liquid feed cycle is plotted as
a function of the length of the liquid-rich region for
3.0 mm glass spheres as packing material. Apparently,
only one pulse is generated when the length of the liquid-
rich region is less than approximately 0.5 m. For lengths
of the liquid-rich region above 0.5 m, the number of
pulses increases linearly with increasing length. A compa-
rable plot is encountered for 6.0 mm spheres as packing
material. In this case, the critical length beneath which
only one pulse is generated during a liquid feed cycle is
approximately 0.6 m.
6. Concluding remarks
In this contribution it is made clear that by means of
the periodic operation of a trickle-bed reactor it is pos-
sible to obtain pulsing #ow at throughputs of liquid
associated with trickle #ow during steady-state opera-
tion. Enhanced mass and heat transfer rates are then
considered to be due to the change in #ow regime. More-
over, the fairly high #ow rates required to achieve natural
pulsing #ow are generally considered to be a drawback
since they are associated with rather short contact times
between the phases. Thus applicability of self-generated
pulsing #ow appears to be restricted to chemical
J. G. Boelhouwer et al. / Chemical Engineering Science 56 (2001) 2605}2614 2613
reactions with fast kinetics. By means of liquid-induced
pulsing #ow, longer contact times can be achieved. An
additional advantage of liquid-induced pulsing #ow is
the opportunity to control the pulse frequency. This
tuning of the pulses is an important issue in the optimiza-
tion of selectivity in catalytic reactions. Higher selectiv-
ity's can be achieved when the time constant of pulsing is
comparable to the time constant of important physical
and chemical processes (Wu et al., 1995, 1999).
The formation of detectable pulses is the result of the
growth of convective instabilities, which grow with dis-
tance into pulses. With increasing gas #ow rate, the
necessary length for pulse formation decreases. This phe-
nomenon is responsible for the upward movement of the
point of pulse inception for self-generated pulsing #ow.
This same phenomenon is found to control the process of
liquid-induced pulsing #ow. By cycling the liquid feed,
continuity shock waves are initiated in the column. As
a result, for relatively short hlf-times two regions of
di!erent liquid holdup are present in the column. At high
enough gas #ow rates, pulses are initiated in the liquid-
rich region of which the length is a linear function of
the hlf-time. With decreasing length of the liquid-
rich region, higher gas velocities necessitate the induction
of pulses. For both self-generated and liquid-induced
pulsing #ow, the relationship between the available
length for pulse formation and the required gas #ow rate
is equivalent.
Because the velocity of the initiated pulses is much
higher than the shock wave velocity, pulses will eventual-
ly move out of the liquid-rich region. In most cases the
pulses remain stable and move to the bottom of the
column. However in some cases, the pulses fade away. At
the present, it is not possible to assure that the induced
pulses remain stable in columns of longer length when
they have moved out of the liquid-rich region. Further-
more, the stability of the initiated continuity shock waves
may be a!ected by the distance these waves travel, al-
though no evidence is found these shock waves are unsta-
ble. In conclusion, it will be worth investigating the
process of liquid-induced pulsing #ow in columns of large
lengths. In the near future, experiments in a column of
3 m in height will be performed in our laboratory.
Notation
f
N
pulse frequency, s\
l
U
length of liquid-rich region, m
n
N
number of pulses during one feed cycle, dimen-
sionless
t
@
low-liquid-feed time, s
t
N
high-liquid-feed-time, s
;
E
super"cial gas velocity, m s\
;
J@
super"cial low liquid feed velocity, m s\
;
JN
super"cial high liquid feed velocity, m s\
<
U
shock wave velocity, m s\
<
U
relative shock wave velocity, dimensionless
Greek letters
@
liquid holdup corresponding to low liquid #ow
rate, dimensionless
N
liquid holdup corresponding to high liquid #ow
rate, dimensionless
N
relative liquid holdup during high liquid #ow
rate, dimensionless
References
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