Chemical Engineering Science 210 (2019) 115231

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Chemical Engineering Science

journal homepage: www.elsevier.com/locate/ces

Investigation of the liquid mixing characteristic of an external-loop

hybrid fluidized-bed airlift reactor
Mateusz Prończuk ⇑, Katarzyna Bizon
Department of Chemical and Process Engineering, Cracow University of Technology, ul. Warszawska 24, 31-155 Kraków, Poland

h i g h l i g h t s

The mixing characteristic of a hybrid fluidized-bed airlift loop reactor was analyzed.

Stimulus-response experiments were performed to determine Pe number and mixing time.

The method of moments and axial dispersion model were used to estimate Pe number.

The results obtained are comparable to those concerning classical airlift loop reactors.

Expression for determination of the mixing time in loop apparatuses was proposed.

a r t i c l e i n f o a b s t r a c t

Article history: The paper presents the results of experimental investigation of the mixing characteristics of an external-
Received 15 May 2019 loop hybrid fluidized-bed airlift reactor. Stimulus-response tracer experiments were carried out using KCl
Received in revised form 24 August 2019 solution as a tracer. Based on the obtained tracer residence time distribution (RTD) curves, values of the
Accepted 19 September 2019
Peclet number for the entire apparatus and its selected zones i.e. fluidization, bubbling, bottom and
Available online 19 September 2019
degassing zones were determined. The values of Pe were calculated using three different methods, i.e.
method of moments, optimization method combined with numerical solution of the axial dispersion
Keywords:
model and by fitting the experimental data to a special solution of the axial dispersion model describing
Hybrid airlift reactor
Three-phase reactor
the response of the loop apparatus to the impulse of tracer. The mixing time was determined both from
Dispersion the experimental RTDs and through using the proposed theoretically derived expression that permits an
Mixing time estimation of the values of mixing time based on a single liquid circulation.
Ó 2019 Published by Elsevier Ltd.

1. Introduction
The hybrid fluidized-bed airlift reactor with liquid circulation is a
relatively recent design solution and there are only few reports in
the scientific literature concerning the hydrodynamics of such a
three-phase apparatus (Guo et al., 1997; Olivieri et al., 2010;
Tabiś et al., 2014, Prończuk and Grzywacz, 2016; Prończuk et al.,
2017). The apparatus, also referred to as a novel three-phase airlift
reactor (Guo et al., 1997; Olivieri et al., 2010), is basically a combi-
nation of a liquid-solid fluidized bed located in the lower section of
the riser and an internal- or external-loop airlift reactor (Fig. 1a).
The gas sparged into the upper section of the riser induces liquid
circulation, implemented either via an internal draft tube or by
using an external downcomer, and thus, at sufficient level of the
aeration, enables the fluidization of the solid particles present in
the lower section of the riser. Provided that there is no circulation
⇑ Corresponding author.
E-mail address: mpronczuk@chemia.pk.edu.pl (M. Prończuk).
of the gas bubbles, the main advantage of such a design is elimina-
tion of the shear stress on the solid, particles which in the classical
three-phase fluidized-bed and airlift reactors may be induced by
flowing gas bubbles. This feature is of particular importance in
many biological processes involving sensitive cells or microorgan-
isms immobilized on the solid carrier particles. The lack of direct
contact of the solid particles and gas bubbles in the hybrid
apparatus allows to avoid the risk of damaging a delicate biofilm
that is immobilized on the carrier surface. Moreover, since the
hybrid fluidized-bed airlift reactor combines the advantages of a
fluidized-bed and an airlift reactor, it is characterized by mechan-
ical simplicity, good gas-liquid mixing and excellent liquid-solid
contact of the fluidized bed (Guo et al., 1997).
Knowledge of the type of flow is necessary for the proper
description of the operation of such an apparatus. Depending on
whether the type of the flow approaches a plug flow or an ideal
mixing, or it deviates substantially from ideal flows, different
mathematical models and initial or boundary conditions
should be used in process calculations, thus knowledge of the flow

https://doi.org/10.1016/j.ces.2019.115231
0009-2509/Ó 2019 Published by Elsevier Ltd.
2 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231

Nomenclature

a1, a2, a3, a4 coefficients in Eq. (9) sc circulation time, s

C tracer concentration, kmol m3 u dimensionless inlet tracer distribution
d diameter, m
D dispersion coefficient, m2 s1 Subscripts
FV volumetric flow rate, m3 s1 0 superficial velocity or initial value
G conductance, lS cm1 1, 2, 3, 4, 5 apparatus zone number
H height, m 1 refers to equilibrium value (after complete mixing)
L length, m c refers to circulation
m mass, kg cal calculated value
M number of discrete nodes in the method of lines ex experimental value
Pe Peclet number g gas phase
t time, s in inlet
tmix mixing time, s inhom inhomogenity
u velocity, m s1 l liquid phase
W width, m out outlet
x dimensional coordinate, m s solid phase
z dimensionless coordinate
Abbreviations
Greek letters MOM method of moments
b dimensionless tracer concentration OM optimization method
e gas hold-up PMMA poly methyl methacrylate
l dynamic viscosity coefficient, Pa s REG regression of Eq. (10)
q density, kg m3 RTD residence time distribution
r surface tension, N m1
2
r variance
s residence time, s

Fig. 1. Experimental setup: (a) schematic of the external-loop hybrid fluidized-bed airlift reactor (1 - fluidization zone, 2 – bubbling zone, 3 – downcomer, 4 – degassing zone,
5 – bottom zone, A and B – tracer injection points) and (b) location of probes and measurement devices (PC – personal computer, ADC – analog-to-digital converter,
P – pressure sensor, C – conductivity sensor, MFC – mass flow controller, UFM – ultrasonic flow meter, PP – peristaltic pump).
 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231
character is necessary for correct prediction of the apparatus per-
formance. The degree of mixing in the apparatus can be expressed
by means of a dispersion coefficient, D, or a Peclet number, Pe,
which is a function of the dispersion coefficient.
There are many works devoted to experimental determination
of the flow characteristic of the classic airlift apparatuses
(Verlaan et al., 1989; Gavrilescu and Tudose, 1997, 1999). In the
cited works, the authors determined the values of Peclet number
for the entire apparatus and for its individual zones. However,
for the hybrid fluidized-bed airlift apparatuses, no such studies
have been carried out so far.
Another crucial parameter describing the mixing conditions in
the apparatus is mixing time, tmix. This is defined as the time
required to achieve a certain degree of inhomogeneity of the tracer
concentration after its injection to the apparatus in the form of an
impulse (Dirac d distribution). In other words, the mixing time is
the time when the local tracer concentration in the whole appara-
tus deviates less than 5% (in this work, various authors use differ-
ent values ranging from 1 to 10%) from the final tracer
concentration. One of the first extensive research studies concern-
ing the mixing time in circulating apparatuses was carried out by
Khang and Levenspiel (1976), who assessed the influence of mixing
Reynolds number on the value of tmix in mixers. To determine the
mixing time, they used a function that approximated the envelope
of the residence time distribution curve of the tracer introduced to
the apparatus. The mixing time was then determined as the time
for which this function reaches a certain concentration limit.
A similar approach was used by Verlaan et al. (1989) and by
Gavrilescu and Tudose (1997, 1999) to evaluate the mixing time
in airlift apparatuses. Some attempts to derive mathematical rela-
tionships for determination of the mixing time in airlift appara-
tuses were also made. For instance, Petrović et al. (1995) related
the value of mixing time to gas velocity and volume of the individ-
ual zones of the airlift apparatus, whereas for the hybrid apparatus,
Guo et al. (1997) associated the mixing time with solid loading and
its physical properties.
Experimental determination of the Peclet number and the mix-
ing time is usually based on tracer experiments. They involve the
introduction of a substance called a tracer into the apparatus and
simultaneous measurement of its concentration at a certain point
(or several points) in the apparatus. This procedure leads to obtain-
ing tracer response. The tracer may be an acid or base solution
whose concentration is measured using a pH probe (Verlaan
et al., 1989). However, the most commonly used substance in tra-
cer experiments is a solution of salts characterized by high electri-
cal conductivity, usually NaCl or KCl. The concentration of salts is
normally measured indirectly using conductivity probes
(Gavrilescu and Tudose, 1997, 1999; Behin and Ahmadi, 2010;
Essadki et al., 2011; Moudoud et al., 2018; Lechowska et al.,
2019). An interesting modification of this method was proposed
by Hamood-ur-Rehman et al. (2012), who applied an electrical
resistance tomography (ERT) method to measure the tracer con-
centration in the apparatus cross-section. Recently, Behin and
Farhadian (2013, 2015) employed a colored tracer, whose concen-
tration was determined using digital image processing (DIP)
method. The method was successively compared with the results
obtained from computational fluid dynamics (CFD) (Farhadian
et al., 2018).
Despite the fact that hybrid fluidized-bed airlift reactors are a
very promising three-phase design for handling biological pro-
cesses, there are no reports in the literature dealing with detailed
mixing studies in such devices. The outcomes of the hitherto
hydrodynamic studies concerning both external- (Guo et al.,
1997; Prończuk and Grzywacz, 2016; Prończuk et al., 2017) and
internal-loop hybrid fluidized-bed airlift reactors (Olivieri et al.,
2010) are mainly limited to the experimental evaluation and
3
theoretical prediction of the media velocities and hold up of both
gas and solid phases in the individual sections of such apparatuses.
The only exception is the work of Guo et al. (1997), who also inves-
tigated the mixing time.
For this reason, in the present study, a detailed analysis of the
liquid flow pattern and mixing time in an external-loop hybrid
fluidized-bed airlift reactor was performed. Both the influence of
operating and design parameters on the liquid mixing characteris-
tic of the entire reactor and its individual zones was evaluated
experimentally using the RTD analysis. One of the objectives of
the experiments was to quantify the differences in the flow struc-
ture in selected zones of the apparatus and to evaluate the overall
mixing performance that may facilitate selection of an adequate
reactor design and suitable operating conditions. The extent of
mixing in the individual zones and in the entire apparatus was
expressed in terms of the Peclet number, determined from the
experimental data using different computational methods. Addi-
tionally, the aim of this study was to verify experimentally the pro-
posed theoretical formula for the estimation of the mixing time in
the loop apparatus.
2. Experimental apparatus and procedure
Fig. 1 shows the schematic diagram of an external-loop hybrid
fluidized-bed airlift reactor made of poly methyl methacrylate
(PMMA) in which the RTD of the liquid phase was studied. Due
to different flow characteristics, the apparatus can be subdivided
into five distinct zones (Fig. 1a): fluidization zone ‘‘1”, bubbling
zone ‘‘2”, external downcomer ‘‘3”, bottom ‘‘4” and degassing ‘‘5”
zones. The fluidization zone located in the lower part of the riser
is delimited both from the bottom and from the top by a two-
layer wire mesh with openings of 1 mm and 0.315 mm. The upper
mesh prevents entrainment of the bed particles into the upper part
of the riser, i.e. the bubbling zone. The construction of the appara-
tus permits to use circulation pipes of different diameters. The
dimensions of the apparatus are presented in Table 1.
The fluidized bed contains polyoxymethylene (POM) granules
and the apparatus was operated using ambient air and tap water
(Table 2) in a semi-batch mode, i.e. with the liquid feed and dis-
charge flow rate FVl = 0. However, the peristaltic pump permits to
supply the liquid into the lower part of the bottom zone ‘‘5”, thus
it is also possible to run the process in a continuous mode. The
compressed air was injected into the zone ‘‘2” by means of a
cross-shaped sparger mounted at its bottom and having 25 equally
spaced openings with the diameter of 1 mm. The volumetric gas
flow rate was adjusted by a mass flow controller. The liquid circu-
lation velocity was measured using an ultrasonic flow meter
installed on the outer wall on the downcomer (zone ‘‘3”). The gas
holdup in the bubble zone was determined using a manometric
method from the hydrostatic pressure measurements done with
the aid of pressure sensors mounted along zone ‘‘2”.
The liquid residence time distribution (RTD) in the entire appa-
ratus and its zones was determined using a classical stimulus-
response technique (Levenspiel, 1999; Gavrilescu and Tudose,
1997). To perform RTD measurements, the apparatus was
Table 1
Dimensions of the external-loop hybrid fluidized-bed airlift reactor.
Parameter Value (m) Parameter Value (m)
H1 1 Hl4 0.04
H2 1 L4 0.34
H3 2 W4 0.17
d1 0.08 H5 0.12
d2 0.08 L5 0.17
d3 0.03, 0.05, 0.08 d5 0.08
4 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231

Table 2 Two methods were used to estimate the value of Pe number for
Physical properties of the media. the individual zones of the apparatus, namely the method of
Parameter Value Unit moments and the axial dispersion model. In the method of moments
Gas (ambient air) qg 1.19 kg/m3 (Levenspiel, 1999), the unknown value of the Peclet number is cal-
lg 1.8 105 Pa s culated from the first two moments of the experimental RTD curve,
Liquid (tap water) ql 999 kg/m3 i.e. the mean residence time, s, and the variance r2.
ll 1.14 103 Pa s If an ideal pulse of tracer is introduced into the fluid entering a
rl 7.32 102 N/m
Bed material (POM) qs 1350 kg/m3
vessel and considering that the concentration curves at the vessel
ds 3.29 103 M outlet are discrete functions of time, C(ti) where i = 1, 2, . . . n, then
ms 0.4 kg the experimental mean residence time and the variance of RTD are
defined, respectively, as:
Pn
t i C i Dti
equipped with five conductivity probes located, respectively, at the s ¼ Pi¼1
n ð3aÞ
downcomer inlet and outlet, under the bottom and the upper mesh i¼1 C i Dti

delimiting the fluidized-bed zone and at the bubbling-zone outlet Pn

(Fig. 1b). The stimulus-response experiments were done using a t 2i C i Dti
r2 ¼ Pi¼1
n  s2 ð3bÞ
20% (by mass) solution of KCl as a tracer. Depending on the exper- i¼1 C i Dti
iment, the tracer was injected at the downcomer inlet or at the
where Ci = C(ti) is the tracer concentration, ti is the discrete time, Dti
bubbling-zone outlet (points marked with A and B, respectively,
is the time distance between successive measurements and n is the
in Fig. 1a). The liquid conductance, which is a function of the tracer
total number of the measurements.
concentration, was then measured at the outlet of each zone using
In the case of the analyzed multi-zone apparatus and an
the conductivity probes. The measurements were carried out for
experimental procedure based on a single injection point, the
the gas superficial velocity in the bubbling zone, u0g2 that varied
moments for the jth zone are determined from the tracer RTD
approximately in the range of 0.005–0.05 m s1. The exact limit
curves at the inlet and at the outlet of the considered zone, namely
values of u0g2 depended on the downcomer diameter (d3 = 0.03,
(Levenspiel, 1999):
0.05 or 0.08 m). In each case, the minimum value of the employed
gas flow rate was higher than the velocity providing the minimum sj ¼ sj;out  sj;in ð4aÞ
fluidization velocity of the solid particles in the fluidization zone,
whereas the highest flow rate was chosen so that the fluidized- r2j ¼ r2j;out  r2j;in ð4bÞ
bed height did not exceeded 90% of the total height of zone ‘‘1”.
Moreover, it was confirmed by visual observations that in the The values of Pe number for each zone of the hybrid apparatus
whole range of the adopted gas velocities, there was no recircula- are then determined using the following analytical expression that
tion of the gas bubbles into the downcomer. is valid for an open-open vessel (Levenspiel and Smith, 1957):

r2 2 8
3. Computational methodology ¼ þ ð5Þ
s2 Pe Pe2
To assess the possibility of evaluation of the mixing character- The second of the employed methods consists of fitting the the-
istic based on a single injection point, the tracer was injected at oretical RTD curves predicted by the classical axial dispersion
the downcomer entrance (point A in Fig. 1a), just above the first model, to the experimental RTD curves. According to this model,
conductivity probe. The tracer concentration curves, C(t), were the fluid flow has a plug flow character, on top of which some
then determined from the following quadratic relationship degree of backmixing is superimposed (Levenspiel, 1999). The axial
between the concentration of potassium chloride and its electrical dispersion model, expressed in terms of normalized concentration,
conductivity: b, and dimensionless axial coordinate, z, is given by:
!
C ¼ 5:76  1011 G2 þ 7:01  106 G ð1Þ @b 1 1 @ 2 b @b
¼  ð6aÞ
@t s Pe @z2 @z
3
where C denotes the concentration of KCl solution (in mol/dm ) and
G is the conductance of the KCl solution (expressed in lS/cm). Eq. @bð1; tÞ
(1) was obtained by approximation of the measured values of con- bð0; tÞ ¼ uðtÞ; ¼0 ð6bÞ
@z
ductivity of certified standard solutions with various KCl concentra-
tions provided by the conductometer manufacturer, and it is valid bðz; tÞ ¼ 0 for z 2 ½0; 1 ð6cÞ
at the temperature of 25 °C. At different values of the temperature,
a correction factor of 1.9%/oC provided by the manufacturer was where
applied.
CðtÞ  C 0 C in ðtÞ  C 0 x
In order to characterize quantitatively the liquid flow pattern in bðtÞ ¼ ; uðtÞ ¼ ; z¼ ð7Þ
C1  C0 C1  C0 L
each zone and to evaluate the mixing intensity in the entire appa-
ratus, the values of individual (i.e. referred to the zone) and overall with C0, Cin and C1 being, respectively, the initial tracer concentra-
(i.e. referred to the entire apparatus) axial Peclet number were tion inside the vessel, the tracer concentration at the vessel inlet
determined from the RTD curves. The axial Peclet number, Pe, is and the equilibrium concentration (i.e. after complete mixing) of
defined as: the tracer inside the vessel.
While the value of the mean residence time, s, may be deter-
uL
Pe ¼ ð2Þ mined directly from the experimental data using Eq. (4a), the value
D
of Peclet number, Pe, need to be estimated by means of the least
where u is the mean flow velocity, L is the length or height of the squares method. Usually in the fitting procedure, the analytical
analyzed zone and D is the axial mass dispersion coefficient charac- solution of Eq. (6) is used as the model curve to estimate the value
terizing the degree of backmixing. of the Peclet number (Voncken et al., 1964; Verlaan et al., 1989;
 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231
Gavrilescu and Tudose, 1997, 1999). However, when the experi-
mental inlet concentration is different than the Dirac distribution,
such a solution is generally not available. In such a case, the rele-
vant parameter, i.e. Pe, can be determined by combining the least
square fitting with the numerical solution of the partial differential
equation (PDE) (6). For this reason, in the present work, the values
of Peclet number were determined by minimizing the function:
X
n
f ðPeÞ ¼ ½bex ð1; t i Þ  bnum ð1; t i Þ2
i¼1
where bex ð1; t i Þ and bnum ð1; t i Þ denote, respectively, measured and
calculated numerically by solving Eq. (6), values of the tracer con-
centration at the zone outlet at time instant ti, i = 1, 2, . . . n. The
minimum of the function (8) was determined in Matlab using
fminbnd function. The time-dependent outlet concentration
bnum ð1; t i Þ was determined by transformation of PDE (6) into a set
of ordinary differential equations (ODEs) via the method of lines
(Shampine, 1994) with M = 1001 discrete nodes, followed by
numerical integration of the resulting ODEs with the aid of ode15s
Matlab solver.
The advantage of the above method is that the distribution of
the tracer concentration at the zone inlet may be of any shape.
However, due to the employed variable-step ODE solver, there is
a necessity to describe the inlet concentration, using a continuous
function. The function applied for the approximation of the tracer
concentration at the inlet of each zone, adopted as a time-variable
boundary condition at z = 0 (6b) when solving Eq. (6a), is as
follows:
    a4 
t  a2 t  a2
uðtÞ ¼ a1 exp  exp exp 
a3 a3
The methods described above, i.e. the method of moments and
the axial dispersion model, were also utilized to characterize the
overall degree of mixing in the entire apparatus depending on
the diameter of the downcomer and volumetric flow rate of gas
supplied into the bubbling zone. The value of the overall Peclet
number, i.e. Pe referred to the entire apparatus, in both cases
was determined based on the conductivity signal detected by a sin-
gle sensor during the first and the second full liquid circulation in
the reactor.
In addition, the results obtained using the methods of moments
and by fitting of the numerically resolved axial dispersion model to
experimental data were compare with the values of Pe derived by
fitting the following particular analytical solution of Eq. (6a) to
experimental RTD:
rffiffiffiffiffiffiffiffiffiffi 1 " #
Pesc X
2
Peðjsc  t Þ
bð1; tÞ ¼ exp 
4pt j¼1 4sc t
where sc denotes the liquid circulation time in the apparatus and j
is the number of liquid circulation loops. Eq. (10) represents the
response of the apparatus with liquid circulation to a Dirac pulse
of the tracer injected at z = 0 = 1 and detected at the same position
(Takao et al., 1982), thus it can be employed when the time duration
of tracer injection is short enough so the inlet signal can be treated
as a Dirac d.
The solution given by Eq. (10) can be further employed for
determination of the mixing time, tmix, in the loop apparatus.
According to Takao et al. (1982), the following extension of Eq.
(10) describes the response to tracer pulse at any point z 2 ð0; 1
of the circulation loop:
rffiffiffiffiffiffiffiffiffiffi 1 " #
Pesc X
2
Peððj þ z  1Þsc  t Þ
bðz; tÞ ¼ exp 
4pt j¼1 4sc t
5
For sufficiently high values of Pe, kth local maximum of the
curve given by Eq. (11) at the measuring point z can be approxi-
mated with very high accuracy by the global maximum of the kth
component of the sum (11):
rffiffiffiffiffiffiffiffiffiffi " 2
#
Pesc Peððk þ z  1Þsc  t Þ
bðz; tÞ ¼ exp  ð12Þ
4pt 4sc t
that is:
ð8Þ
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
sc  sc Pe2 ðk þ z  1Þ2 þ 1
tmax ¼  ð13Þ
Pe
Substitution of the solution (13) into Eq. (11) yields the follow-
ing expression of the so-called envelope curve of the response func-
tion (11):
rffiffiffiffiffiffiffiffiffiffi 1 2 rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi !2 3
Pesc X Pe 2 s
exp4 þ js c  t 5
c
benv ðtÞ ¼ t 1þ ð14Þ
4pt j¼1 4sc t tPe
A theoretical value of the mixing time can be then determined
by finding such a value of time, t 2 Rþ , at which the value of the
function (14) gets lower than 1 þ Dbinhom , where Dbinhom is a certain
degree of inhomogeneity of the final tracer concentration in the
vessel. The degree of inhomogeneity usually adopted in the calcu-
lations is 1% (Bello et al., 1984; Lechowska et al., 2019), 5% (Lin
et al., 1976; Petrović et al., 1995; Behin, 2010) or 10% (Onken
and Weiland, 1980).
4. Results and discussion
ð9Þ
A hydrodynamic study focused on evaluation of the media
velocities in the individual zones of the apparatus was carried
out prior to tracer tests aimed at determination of the Peclet num-
ber and the liquid mixing time. The purpose of this study was to
determine the range of superficial gas velocity in the bubbling
zone, u0g2, at which the apparatus can be operated while ensuring
the fluidization in zone ‘‘1”, and to evaluate its influence on the liq-
uid circulation velocity and gas hold up in zone ‘‘2”.
Fig. 2 presents the dependence of the superficial liquid velocity,
u0l1, and gas hold up, e2, as a function of the superficial gas velocity,
u0g2, in the bubbling zone obtained for the apparatus operated with
the bed made of 0.4 kg of POM particles and with the downcomer
having various diameters, d3. More results that also concerns the
influence of the density and diameter of bed particles on the media
velocities and on the gas and solid holdups, can be found in earlier
works (Prończuk and Grzywacz, 2016; Prończuk et al., 2017).
A typical experimental RTD curve of the tracer obtained from
ð10Þ
the conductivity sensor placed in between degassing ‘‘4” and
downcomer ‘‘3” zone is shown using symbols in Fig. 3a. A special
solution of the axial dispersion model (10) was fitted to the exper-
imental data using the least squares method (solid line in Fig. 3a).
It can be seen that this solution accurately describes changes in the
tracer concentration in an apparatus with liquid circulation, thus it
can be used both for determination of Pe and tmix. The value of cir-
culation time, sc, was determined together with the Peclet number
by approximation of the experimental data by Eq. (10), and it is
roughly equal to the distance between the maxima of two adjacent
peaks (Fig. 3a). In Fig. 3a, the RTD envelope function given by the
Eq. (14) is plotted using a dotted line. The degree of inhomogenity,
Dbinhom, used for determination of tmix in this work was set to 5% of
the final tracer concentration and it is also plotted in Fig. 3a (using
a dashed line).
Fig. 3b shows a comparison of the values of mixing time deter-
ð11Þ
mined experimentally and those calculated theoretically using the
envelope curve (14). As it is indicated in Fig. 3a, the theoretical
6 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231

Fig. 2. Superficial liquid velocity in the fluidization zone, u0l1 (a) and gas holdup in the bubble zone, e2 (b) versus superficial gas velocity in the bubbling zone, u0g2.

Fig. 3. Dimensionless tracer concentration, b, versus time, t (a) and comparison of the experimental, tmix,ex, and calculated values of mixing time, tmix,cal, for different values of
the downcomer diameter (b).

mixing time is the time in which the envelope of the tracer RTD
becomes lower than the limit tracer concentration (1 + Dbinhom).
The mixing characteristic was determined based on the series of
13 tracer experiments performed at the superficial gas velocity in
the bubbling zone, u0g2, equal, respectively, to 0.0083, 0.0132,
0.0199, 0.0265, 0.0332 m/s for d3 = 0.03 m; 0.0083, 0.0099,
0.0116, 0.0133, 0.0149 m/s for d3 = 0.05 m and 0.0099, 0.012,
0.013 m/s for d3 = 0.08 m, and selected based on the previous
hydrodynamic tests. It can be observed in Fig. 3b that the devia-
tions of the experimental values of tmix,cal from the theoretical
results do not exceed 10%. Moreover, the values of mixing time
determined empirically, tmix,ex, are larger than the calculated val-
ues, tmix,cal. The experimental results contain large amounts of
noise, so determination of the maxima of subsequent peaks from
the measurement data is rather difficult. This in turn may lead to
undervaluation of the mixing time, especially when it is placed
between two adjacent peaks (Fig. 3a).
The dependence of experimentally determined mixing time,
tmix,ex, on the superficial gas velocity, u0g2, for the apparatus
equipped with the downcomer having various diameters, d3, is pre-
sented in Fig. 4a. It can be seen that for the largest downcomer
diameter, i.e. d3 = 0.08 m, the values of the mixing time are much
higher than those obtained for the smaller diameters. The reason
for this is the flow structure in the downcomer, which in this case
is a large fraction of the entire volume of the apparatus. Since there
was no recirculation of the bubbles that might influence the flow
pattern, the downcomer zone was characterized by virtually unin-
terrupted flow through the circular channel approaching the plug
flow, i.e. characterized by high values of Pe. Thus, the liquid mixing
in this zone was rather limited. In consequence, the apparatus
equipped with the downcomer of this diameter is also character-
ized by very large values of the overall Pe number (see Fig. 5),
because as follows from the formula (Verlaan et al., 1989):
s2c X s2j
¼ ð15Þ
Pe j
Pej
the longer the residence time is in the analyzed zone sj (or its vol-
ume), the greater is the influence of its individual Peclet number,
Pej, on the entire apparatus Peclet number, Pe. The apparatus with
the largest downcomer diameter (d3 = 0.08 m) has the largest
volume, hence the liquid circulation time, sc (Fig. 4b), for the same
liquid circulation velocity, u0l2, is higher than in case of d3 = 0.03 m
and d3 = 0.05 m.
Fig. 4c presents the relationship of the experimental mixing
time, tmix,ex, and the product of the liquid circulation time and
the overall Peclet number, scPe. The values of Pe for the entire
apparatus were derived here by fitting Eq. (10). The experimental
mixing time is practically directly proportional to scPe. The contin-
uous line plotted in Fig. 4c represents the theoretical values of the
mixing time in the loop-apparatus predicted based on the envelope
curve given by Eq. (14). To determine the proportionality coeffi-
cient a in equation:
tmix ¼ a  sc Pe ð16Þ
 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231
Fig. 4. Experimentally determined values of mixing time, tmix,ex, versus superficial gas velocity, u0g2 (a), circulation time, sc, versus superficial liquid velocity, u0l2 (b) and
mixing time, tmix,ex, versus the product of scPe (c).
certain ranges of Pe and sc were adopted based on the minimal and
maximal experimental values. The pairs of the parameters Pe and sc
from these ranges were substituted into Eq. (14) and the equation
was resolved for tmix under the assumption that benv ¼ 1 þ Dbinhom
and binhom ¼ 0:05. Then the linear regression was performed to cal-
culate the proportionality coefficient between the product scPe and
the corresponding tmix. It can be seen (Fig. 4c) that the experimental
data is well represented by the theoretical model. Moreover, the
determined value of a, i.e. a = 0.0934, is in a very good agreement
with the results concerning the relation of Pe, sc and tmix for the loop
apparatus reported in (Verlaan et al., 1989).
The values of the Pe number for the whole apparatus (referred
also as to the overall Peclet number) as a function of superficial gas
velocity u0g2 obtained for various downcomer diameters are shown
in Fig. 5. These were determined by three different methods:
regression of a special solution (10) of the dispersion model
(REG), method of moments (MOM) and optimization method
(OM). Some discrepancies between the results obtained using dif-
ferent methods can be observed in Fig. 5, especially in case of
d3 = 0.03 m (Fig. 5a) and d3 = 0.05 m (Fig. 5b). This can be explained
by the fact the subsequent residence time distribution curves of
the loop apparatus may overlap, which introduces a certain error
to the calculated values of Pe when using MOM or OM. The effect
of overlapping is taken into account when determining Pe from the
solution of the dispersion model for the circulating flow (REG, Eq.
(10)). Therefore, the REG method can be considered as the most
accurate, assuming that the time duration of tracer injection is very
short so the inlet signal can be treated as a Dirac d.
A general tendency for the overall Peclet number to increase as
the downcomer zone diameter, d3, increases, emerges from the
obtained results (Fig. 5). The increase in the diameter d3 results
7
in the larger volume of this zone and thus a larger volume of the
liquid in zone ‘‘3”. As already mentioned, the value of the Pe num-
ber for the whole apparatus depends on the Pe numbers for each
zone and on their volumes (Eq. (15)). Therefore, the increase of
the contribution of the volume of this zone to the entire apparatus
volume arising from its greater diameter results in higher value of
the overall Pe number.
Fig. 6 shows the values of the Pe number determined for the
fluidization zone ‘‘1” (Fig. 6a) and the bubbling zone ‘‘2” (Fig. 6b)
versus the superficial gas velocity, u0g2. These were obtained via
the optimization method and the method of moments. Since the
general trend of the results practically do not depend on the diam-
eter of the downcomer, only the values for one intermediate diam-
eter, i.e. d3 = 0.05 m, are presented. Despite some quantitative
discrepancies, a qualitative conformity of the results obtained by
two different methods is observed in Fig. 6. For the fluidization zone
‘‘1” (Fig. 6a), the value of Pe number decreases with the increase of
the gas superficial velocity in zone, u0g2, which is the driving force of
the liquid circulation in the apparatus and thus it affects the flu-
idization conditions in zone ‘‘1”. It should be noted that the fluidiza-
tion zone itself consists of two parts: a fluidized bed and a liquid
above the bed. The liquid flow through the fluidized bed approaches
the ideal mixing, so when its height increases with the increase of
the superficial gas velocity in zone ‘‘2”, the contribution of the flu-
idized bed to the value of the Pe number for this zone also increases.
Similar values of the Pe number were obtained for the bubbling
zone ‘‘2” (Fig. 6b). The relatively good mixing of the liquid in this
zone is due to the presence of gas bubbles. The rise velocity of bub-
bles is much higher than the liquid velocity, thus the fluid flow
structure is significantly disturbed by the differences of these veloc-
ities, which results in increased axial mixing.
8 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231

Fig. 5. Overall Peclet number versus superficial gas velocity in the bubbling zone, u0g2, for apparatus with the downcomer diameter, d3, equal to 0.03 m (a), 0.05 m (b) and
0.08 m (c) obtained for the tracer injection point ‘‘A”.

Fig. 6. Peclet number for the fluidization zone ‘‘1” (a) and bubbling zone ‘‘2” (b) versus superficial gas velocity in the bubbling zone, u0g2, for an apparatus with the
downcomer diameter d3 = 0.05 m and a tracer injection point ‘‘A”.

Fig. 7 shows the values of the Pe number determined for the
degassing zone ‘‘4” and for the bottom ‘‘5” zone. Both zones are
characterized by relatively small Peclet number, which, as
expected, indicates that the liquid flow through these zones is
close to perfect mixing. However, for zone ‘‘4”, a significant dis-
agreement between the results obtained by two different methods,
i.e. MOM and OM, can be observed. These discrepancies result from
the construction of this zone and the methodology of the per-
formed tracer experiments. The degassing zone ‘‘4” is character-
ized by a small volume compared to the volume of the whole
apparatus, therefore, the residence time, s, in this zone was very
short - about 1–2 s. The point of tracer injection ‘‘A” was positioned
(Fig. 1a) practically at the outflow from this zone, hence, to reach
this zone, the tracer had to flow almost through the entire volume
of the apparatus. Thus, the time span of the RTD of the tracer both
at the inlet and at the outlet of zone ‘‘4” was much greater than the
residence time in this zone. Beyond the discrepancy of the results,
the very short residence time, coupled with the wide times span of
 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231 9

Fig. 7. Peclet number for the degassing zone ‘‘4” (a) and bottom zone ‘‘5” (b) versus superficial gas velocity in the bubbling zone, u0g2, for an apparatus with the downcomer
diameter d3 = 0.05 m and a tracer injection point ‘‘A”.

the inlet tracer RTD resulted in the need to repeat part of the tracer
experiments because, in some cases, the value of the second RTD
moment, r24 , determined from equation (4b) and required for cal-
culating Pe using MOM, was negative.
Nevertheless, the design and the nature of the flow in the
degassing zone ‘‘4” suggest that the results obtained from the
MOM are more reliable than those derived using OM. Short resi-
dence time, low mean liquid velocity and sudden change of flow
direction in zone ‘‘4” (see Fig. 1a) should result in intense mixing,
so Pe should have low values. Therefore, to understand better the
impact of the tracer distribution at the inlet of the zone character-
ized by a very short residence time onto the optimization method
results, a numerical simulation of the apparatus response was per-
formed using model (6). Two different inlet RTDs characterized,
respectively, by a short (Fig. 8a) and long (Fig. 8b) time span were
used in the computations. In both cases, the residence time was set
to s = 1 s. Simulations of dynamic responses to the presented inlet
RTD for three different values of the Peclet number were then con-
ducted. For RTD with a smaller time span (Fig. 8a), significantly dif-
ferent response curves were obtained for the assumed values of Pe
(Fig. 8c). In the case of a longer time span of inlet tracer RTD
(Fig. 8b) and short residence time, i.e. the conditions prevailing
in zone ‘‘4” when the tracer is injected in point ‘‘A”, very similar
RTDs curves were obtained, even for significantly different Peclet

Fig. 8. Distribution of the injected tracer u(t): (a) variant I and (b) variant II. Corresponding simulated RTDs: (c) variant I and (d) variant II for the mean residence time s = 1 s
and different values of Pe number.
10 M. Prończuk, K. Bizon / Chemical Engineering Science 210 (2019) 115231
Fig. 9. Peclet number for the degassing zone ‘‘4” versus superficial gas velocity in
the bubbling zone, u0g2, for an apparatus with the downcomer diameter d3 = 0.05 m
and for the tracer injection point ‘‘B”.
number values, i.e. 1, 10 and 100 (Fig. 8d). Therefore, the reason for
discrepancies in the results obtained by various methods, i.e. OM
and MOM, is the too long RTD time span in relation to the resi-
dence time in the degassing zone ‘‘4”, which makes that the opti-
mization problem (8) has many local extrema.
In order to confirm the proposed thesis, the tracer experiments
were repeated, changing the tracer injection point to the position
marked with ‘‘B” in Fig. 1a. The results are presented in Fig. 9. It
can be observed that after moving the injection point closer to zone
‘‘4”, the discrepancies between the results obtained by different
methods are smaller. For the remaining zones, no major discrepan-
cies were found in the results irrespective of the tracer injection
point used in the experiments.
5. Conclusions
The hybrid fluidized-bed airlift apparatus analyzed in this work,
is basically a modification of a two-phase airlift apparatus with
external circulation, with the main difference consisting in the
presence of three-phases and a division of the riser into fluidization
and bubbling zones. Both in the hybrid and classical external-loop
airlift apparatus one can distinguish the bubbling zone, down-
comer, degassing and bottom zones, therefore as expected the val-
ues of Peclet number for individual zones of the hybrid apparatus
are quantitatively and qualitatively comparable to those obtained
by Verlaan et al. (1989) or Gavrilescu and Tudose (1997) who ana-
lyzed the liquid flow structure in the two-phase airlift reactor.
The values of Pe for individual zone were determined using two
methods, i.e. method of moments (MOM) and optimization
method (OM). The MOM is a commonly used and well-known
method for determining the Peclet number based on experimental
tracer RTDs. Its main advantage is a simple analysis of the results
when dealing with the inlet tracer RTDs approaching Dirac d distri-
bution. In contrast, the OM allows a very easily determination of
the Pe value number for virtually any kind of tracer RTD at the zone
(vessel) entrance. However, as demonstrated in this study when
analyzing the values of Pe for individual zones of the hybrid loop
reactor, for a short residence time in a given zone, the time span
of the inlet tracer RTD cannot be too wide since it may lead to erro-
neous results.
Both MOM and OM may lead to overestimation of the entire
apparatus Pe when dealing with a hybrid apparatus equipped with
a narrower downcomer and thus characterized by more efficient
mixing, since in this case, the subsequent RTDs used in the calcu-
lations may overlap. The effect of overlapping is taken into account
in the third method employed for the determination of the overall
Peclet number, i.e. regression of a special solution of the dispersion
model for loop apparatus (REG). The smallest differences between
the results obtained by MOM and OM, and by REG were in fact
obtained for the case with the highest overall Pe, i.e. for the appa-
ratus operated with the largest diameter of the downcomer. When
the flow character in the loop apparatus deviates significantly from
the mixed flow, the first two RTD peaks do not overlap signifi-
cantly, thus similar results can be obtained using all three
methods.
It was confirmed that in the examined range of superficial gas
velocities, the values of mixing time strongly depended upon the
downcomer diameter. The longest mixing time was obtained for
an apparatus with the largest downcomer diameter. Moreover, in
depth analysis of the obtained results showed that the mixing
time, tmix, is proportional to the product of the liquid circulation
time, sc, and the overall Pe number. Moreover, theoretical analysis
allowed determination of the proportionality coefficient between
scPe and the corresponding tmix. An advantage of the proposed
equation is that there is no need to carry out long RTD experiments
until nearly complete mixing since the value of Pe and the circula-
tion time can be determined from the first peak of the tracer RTD.
This may be especially useful in case of apparatuses characterized
by high values of both Pe and circulation time.
Declaration of Competing Interest
None.
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