Chemical Engineering Communications

ISSN: 0098-6445 (Print) 1563-5201 (Online) Journal homepage: https://www.tandfonline.com/loi/gcec20

Probability density functions for bubble size

distribution in air–water systems in stirred tanks

Henrique J. O. Pinho, Dina M. R. Mateus & Sebastião S. Alves

To cite this article: Henrique J. O. Pinho, Dina M. R. Mateus & Sebastião S. Alves (2018)
Probability density functions for bubble size distribution in air–water systems in stirred tanks,
Chemical Engineering Communications, 205:8, 1105-1118, DOI: 10.1080/00986445.2018.1434159

To link to this article: https://doi.org/10.1080/00986445.2018.1434159

Published online: 09 Apr 2018.

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CHEMICAL ENGINEERING COMMUNICATIONS
2018, VOL. 205, NO. 8, 1105–1118
https://doi.org/10.1080/00986445.2018.1434159

none defined

Probability density functions for bubble size distribution in air–water

systems in stirred tanks
Henrique J. O. Pinhoa,b , Dina M. R. Mateusa,c , and Sebastião S. Alvesb
a
Unidade Departamental de Engenharias, Instituto Politécnico de Tomar, Estrada da Serra, Quinta do Contador, Tomar, Portugal; bCERENA,
Centro de Recursos Naturais e Ambiente, Instituto Superior Técnico, Universidade de Lisboa, Lisboa, Portugal; cGEOBIOTEC, GeoBioSciences,
GeoTechnologies and GeoEngineering, Universidade de Aveiro, Campus Universitário de Santiago, Aveiro, Portugal

ABSTRACT KEYWORDS
Bubble size distribution (BSD) is relevant to the design of gas–liquid systems, as it determines the Nukiyama–Tanasawa
interfacial area available in heat and mass transfer processes. Although data on BSD in stirred distribution; particle size
aerated tanks are available, a systematic comparison of alternative modeling functions for these distribution; probability
density function; Rosin–
data is lacking. In this work, BSDs obtained in air–water dispersions in a stirred aerated tank with a
Rammler distribution; Sauter
Rushton turbine and BSDs available in the literature for similar systems were modeled by 14 mean diameter; two-phase
empirical probability density functions (PDFs). It was found that both the distribution of Nukiyama– flow
Tanasawa with three adjustable parameters and the Rosin–Rammler distribution with two
adjustable parameters reasonably fit original and literature BSDs. It is also concluded that it is
possible to correlate the PDF parameters with the power dissipated by the agitator in the liquid
phase, allowing the BSD to be modeled with only two parameters in a range of dissipated power
from 0.5 to 2.3 kW/m3. BSDs thus modeled provide good predictions of average bubble size.
Abbreviations: BE, bi-exponential distribution; BS, Birnbaum–Saunders distribution; BSD, bubble size
distribution; CDF, cumulative distribution function; CFD, computational fluid dynamics; F, Frechet
distribution; G, gamma distribution; G–L, gas–liquid; IG, inverse Gaussian distribution; J, Johnson
distribution; LH4, four parameter log-hyperbolic distribution; LL, log-logistic distribution; LN, log-
normal distribution; N, normal distribution; NT, two-parameter Nukiyama–Tanasawa distribution;
NT3, three-parameter Nukiyama–Tanasawa distribution; PDF, probability density function; PSD,
particle size distribution; RR, Rosin–Rammler distribution; UL3, upper limit distribution

Introduction Sauter mean diameter represented by d32 in

Equation (1), where Ni represents the number of
Particle size is relevant to several unit operations
bubbles with diameter di and M the number of
typically used in chemical, biochemical, energy,
different bubble diameters.
and environmental processes, among other fields
of engineering, particularly for the modeling and PM
Ni di3
scale-up of transport phenomena. Modeling of d32 ¼ Pi¼1
M 2
ð1Þ
mass and heat transfer involving a dispersed phase, i¼1 Ni di

for example, requires knowledge of the interphase
area, which depends upon particle size and
dispersed phase holdup.
One problem in studying these phenomena
derives from the fact that, due to fragmentation
and dispersion dynamics, solid particles, liquid
drops, and gas bubbles are generally found in a
range of sizes instead of a single well-defined
dimension. This usually implies the use of an
appropriate average size. In gas–liquid heat and
mass transfer applications, this average is the
To obtain d32, the bubble size distribution (BSD)
is required. The BSD may also be required in
applications where a single average is not good
enough, such as modeling with computational fluid
dynamics (CFD) (Kálal et al., 2014; Montante et al.,
2008; Petitti et al., 2010; Sajjadi et al., 2012), or
in validation of new experimental methods to
characterize dispersions (Busciglio et al., 2010).
Mathematical description of raw BSD data is
thus important and there are no studies available
on the analysis of alternative BSD models for

CONTACT Henrique J. O. Pinho hpinho@ipt.pt Unidade Departamental de Engenharias, Instituto Politécnico de Tomar, Estrada da Serra, Quinta do
Contador, 2300-313 Tomar, Portugal.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/gcec.
© 2018 Taylor & Francis
1106 H. J. O. PINHO ET AL.
gas–liquid (G–L) contactors. In contrast, the
particle size distribution (PSD) of granulated
solids and gas-dispersed liquids has received
more attention, particularly in the energy and
combustion fields (Babinsky and Sojka, 2002;
Dunbar and Hickey, 2000; González-Tello et al.,
2008; Paloposki, 1994).
In most of the available literature, probability
density functions (PDFs) are used to model
experimentally observed BSD. The use of such an
empirical approach was found to be a practical
and successful alternative to more complex
theoretical models (Macías-García et al., 2004).
The objective of this work was to identify the
best suitable PDFs to model BSD in G–L-stirred
contactors and to evaluate the effects of operating
conditions on the PDFs’ parameters. To achieve
this goal, original data were obtained from experi-
mental work conducted in air–water dispersions
in a lab stirred tank reactor and representative
literature data on gas–liquid systems were gathered
and analyzed.
Probability density functions for bubble
size distributions
The extensive work of Paloposki (1994) identifies
and characterizes 16 examples of PDFs potentially
applicable to model PSDs. In his work, the author
applies six PDFs to experimental drop size distribu-
tions on air-dispersed liquids: the log-normal, upper
limit, Rosin–Rammler and Nukiyama–Tanasawa
distributions, and the four- and three-parameter
forms of the log-hyperbolic distribution.
There is no similar systematic work on BSD data
in aerated stirred tanks. However, a few researchers
attempted to fit PDFs to experimental BSDs: Zhang
et al. (1989) observed that bubbles’ diameters in
air–water system approach normal distribution;
Barigou and Greaves (1992) concluded that the
Weibull distribution may fit the BSD of coalescing
air–water systems, but noncoalescing systems BSD
are better fitted by exponential-type distributions;
Martin (1995) argues that bimodal BSDs in both
coalescent and noncoalescent air–water systems
may be modeled by a set of superimposed log-
normal distributions.
Bubble size distributions are typically non-
normal, positively skewed, and positive only and
with diameters always positive. Several PDFs, with
a variable number of parameters, may be used to
fulfill these criteria. However, there is a trade-off
between fitting quality and parameter determi-
nation difficulties and stability (Paloposki, 1994).
Table 1 includes a selected set of PDFs that meet
BSD basic criteria, most of which are based on
two parameters for the sake of simplicity. Normal
PDF was also included as well as some multipara-
meter PDFs usually successful when applied to
PSDs. To avoid an excessive number of symbols
in Table 1, a and b were used preferentially as
symbols to identify PDF parameters, which may
not correspond to common definitions. For the
most common or the most successful PDFs, the
usual nomenclature was used to avoid misunder-
standing in the following article sections.
Table 1 includes the PDFs’ definition and the
corresponding cumulative distribution function
(CDF). All PDFs used are normalized density
functions according to Equation (2):
Zþ1
pðxÞdx ¼ 1 ð2Þ
1
The CDF is defined accordingly Equation (3):
Zx
P ð xÞ ¼ pð yÞdy ð3Þ
1
In Table 1, erf(t) represents the error function,
Γ(t) represents the gamma function, and Γ(t,z) is
the upper incomplete gamma function. K1(t) repre-
sents the modified Bessel function of the third kind
of order 1.
Among the distributions described by Paloposki
(1994), a few were not tested in the present
work: the square-root normal distribution, the
three-parameter Weibull distribution (the two-
parameter form of which is the Rosin–Rammler
distribution), the Li–Tankin distribution, the
Griffith distribution, and different forms of the
hyperbolic distribution. The decision not to use
these distributions resulted from the observation
that these are minor variants of other distributions,
as confirmed by preliminary fitting tests. On the
other hand, two-parameter distributions not referred
by Paloposki, such as the Birnbaum–Saunders and
the Johnson distributions, were used in this work.
 CHEMICAL ENGINEERING COMMUNICATIONS 1107

Table 1. Selected probability density functions (PDFs). PDFs with more than two parameters are identified with a number in the
abbreviation. It is also represented the cumulative distribution functions (CDFs).
Name Abb. Par. PDF ¼ p(x) CDF ¼ P(x)
Bi-exponential BE a,b ab � ax � 1 � xb
� xa
�
e e bx a 1 e bð1 e Þ
b a a b
Birnbaum–Saunders "� � � �3=2 # ( " rffiffiffi rffiffiffi!#)
BS a,b 1 b 1=2 b 1 x b 1 1 x b
pffiffiffiffiffi þ e½ þð
2a2 b x
2Þ�
1 þ erf pffiffi
2ab 2p x x 2 a 2 b x
Frechet a
F a,b aba x 1 a e ðbÞ
x

a
eðx=bÞ
Gamma G a,b a 1 Cða; x=bÞ
x
1
ex=b ba CðaÞ CðaÞ
Inverse Gaussian rffiffiffiffiffiffiffiffiffi � � ( "rffiffiffiffi #) ( "rffiffiffiffi #)
IG a,b b bðx aÞ2 1 b� x� 1 b� x�
e 2xa2 1 erf 1 þ eð2b=aÞ 1 erf 1þ
2px 3 2 2x a 2 2x a
Johnson � � ��
J a,b b 1 2 1 a þ b ln x
pffiffiffiffiffi e 2ðaþb ln xÞ 1 þ erf pffiffi
x 2p 2 2
Log-hyperbolic pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi �pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi2ffi � pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi Z �p ffiffi2ffiffiffiffiffiffiffiffiffiffiffiffiffi2ffi �
LH4 a,b,δ,µ a2 b2 2 a2 b 2 x
� pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi� e d þðx lÞ þbðx lÞ
� pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi� e d þðy lÞ þbðy lÞ
dy
2
2adK1 d a 2 b 2adK1 d a2 b2 0
Log-logistic
LL a,b axa 1 xa
ðb þ a
x a Þ2 ba xa
Log-normal � � � � ��
LN μ,σ 1 ðln x lÞ2 1 ln x l
pffiffiffiffiffi e 2r2 1 þ erf pffiffi
xr 2p 2 r 2
Normal � � � � ��
N μ,σ 1 ðx lÞ2 1 x l
pffiffiffiffiffi e 2r2 1 þ erf pffiffi
r 2p 2 r 2
Nukiyama–Tanasawa 3
� �
NT b,q qbq 2 bxq C q3 ; bx 2
� �x e ��
1
C q3 C q3
Nukiyama–Tanasawa
pþ1
� �
NT3 b,p,q qb q C pþ1 p
� � xp e bx q q ; bx
1 � �
C pþ1
q C pþ1
q
Rosin–Rammler
RR m,n n � x �n 1 ðx=mÞn 1 e ðx=mÞn
e
m m � � � � � ���
Upper limit UL3 a,δ,xmax dxmax 2 2
1 ax
pffiffiffi e d ½lnðxmax xÞ�
ax
1 þ erf d ln
x ðxmax x Þ p 2 xmax x

Materials and methods Filtered air was introduced through a 0.088-m-

diameter ring distributor with 14, 0.6-mm-
Experimental setup
diameter holes, placed 0.103 m below the turbine.
This work A rotameter measured the airflow rate. The
Bubble size distributions were obtained by photo- operative conditions combined three agitation
graphing air–water gas dispersions in a stirred tank speeds of 300, 400, and 500 rpm (respectively,
reactor. The experiments were performed with tap 5.00, 6.67, and 8.33 revolutions/s) with three gas
water (surface tension of 71.8 mN/m) for various flow rates of 0.265, 0.529, and 0.968 vvm (vessel
combinations of agitator speeds and air flow volumes/minute; corresponding to superficial gas
rates. The lab-scale reactor consisted of a 0.232 m velocities of 1.03, 2.03, and 3.74 � 10−3 m/s,
diameter, flat-bottomed, and fully baffled glass respectively).
vessel with steel bottom, described in Figure 1. Photographs of gas dispersions were obtained
The liquid level was kept equal to the tank diameter using a digital camera (Pentax, Model *istD), with
resulting in a working volume of 9.8 L. Agitation a Pentax SMCDA 18–55 mm f/3.5–5.6 AL lens.
was provided by a 0.090-m-diameter Rushton The focal plane was set at 20 mm from the tank
turbine placed 0.118 m above the tank bottom. wall. A small Perspex box full of water attached
1108 H. J. O. PINHO ET AL.
Figure 1. Details of the experimental setup (not to scale). Dimensions (mm): B ¼ 28; C ¼ 118; D ¼ 90; Dd ¼ 60; De ¼ 17; Ds ¼ 28;
h ¼ 32; H ¼ 232; L ¼ 20; T ¼ 232; W ¼ 30; x1 ¼ 2; x2 ¼ 3.
to the tank wall eliminated the curvature effect.
The images have 49 mm height and 77 mm width
and half height point 70 mm below the liquid level.
The photographs were analyzed using the Scion
Image for Windows software, version 4.0.3.2
(Scion, USA). Equivalent diameter db for ellipsoid
bubbles was calculated through Equation (4):
�13
2 P
db ¼ d M dm
where dM is the length of the major axis and dm the
length of the minor axis. Approximately 1000
bubbles were measured for each of the nine combi-
nations of agitator speed and gas flow rate used.
The power transferred to the liquid was
estimated from a corrected power number in
accordance with Brauer’s work (1985), to include
the effect of tank and stirrer geometric details,
and with Hughmark’s (1980) model, to account
for the gas holdup effect on power. The power
number (P0) calculated from Brauer’s (1985) set
of equations depends on the Reynolds number
but is near 8 for the three agitations speeds used
in the present work. The power dissipated by the
impeller was then calculated using Equation (5)
and corrected to gassed conditions with Hughmark’s
correlation [Equation (6)], where ρ is the specific
weight of the liquid phase (kg/m3), ND is the impel-
ler rotational speed (/s), D is the diameter of the
impeller (m), QG is the gas flow rate (m3/s), V is
the tank volume (m3), g is the gravitational acceler-
ation (m/s2), and W the width of the impeller
blades (m). The estimated power ranges from 371
to 2281 W/m3.
P ¼ P0 qND3 D5 ð5Þ
� � ! 0:2
0:25
PG QG ND2 D4
¼ 0:10 2 ð6Þ
ND V gWV 3
ð4Þ
Data from the literature
Bubble size distributions from three published
works were analyzed for comparison with the
present work, covering a range of stirred tank sizes,
operating conditions, and bubble sizing methods.
Samaras et al. (2014) obtained bubble size
distributions in a 5-L stirred tank reactor, a fully
baffled Plexiglas cylindrical tank of 0.190 m diam-
eter with a curved bottom. Agitation was provided
by a 0.063-m-diameter Rushton turbine, placed
0.063 m above the tank bottom. The liquid level
was kept equal to the tank diameter. A nozzle with
2 mm internal diameter placed at the bottom’s
center was used to introduce the gas. The article
provides graphical results for the arithmetic and
Sauter mean bubble diameters and experimental
PDFs, for experiments with 4.3 mM sodium chlor-
ide aqueous solutions, which the authors claim to
be similar to tap water (conductivity 0.5 mS/cm,

surface tension 71.7 mN/m). Agitation speeds
ranged from 500 to 800 rpm, with gas flow rates
of 7.05 and 12.9 � 10−3 m/s. Bubble size was
obtained by photography. The average sample size
was 500 bubbles. The authors did not provide
power data. Using a power number of 5 and
Hughmark’s correlation (1980), gassed power was
estimated to range from 289 to 1282 W/m3.
Martin’s (1995) experimental setup consisted
of a fully baffled Perspex cylindrical stirred tank
reactor with 138 L liquid capacity and 0.56 m
diameter. A Rushton turbine with 0.168 m in
diameter was placed 0.14 m above the tank bottom.
Oil-free air was introduced through a 0.10-m-
diameter ring with 16 2.5-mm-diameter holes
placed at the center of the tank below the impeller.
The liquid media consisted of deionized water
(surface tension 71.79 mN/m). Agitation speeds
ranged from 200 to 500 rpm, with gas flow rates
between 3.74 and 18.7 � 10−3 m/s. Bubble size
was obtained by a video technique. The average
sample size was 500 bubbles. The author obtained
the gassed power experimentally by measuring
the torque in the agitator shaft. Gassed power
ranges from 167 to 2415 W/m3, estimated from
graphical data given by the author.
Barigou (1987) made an extensive work in a
800-L stirred tank consisted in a cylindrical tank
made of Perspex, with 1.0-m-diameter, fully
baffled, and a 0.33-m-diameter Rushton turbine.
The turbine was placed 0.25 m above the tank
bottom. Filtered air was introduced through a
19-mm-diameter nozzle placed at the center of
the tank and below the impeller. The liquid media
consisted in softened tap water (surface tension
70.99 mN/m). Agitation speeds range from 100
to 300 rpm, with gas flow rates of 2.09 and
5.58 � 10−3 m/s. Bubble size was obtained by the
capillary suction probe technique. The average
sample size was 500 bubbles. The author obtained
the gassed power experimentally by measuring
the torque in the agitator shaft. Gassed power
ranges from 106 to 2026 W/m3, as calculated from
a correlation obtained by the author.
Fitting procedure and criteria
Parameter optimization for PDF fitting of bubble
size distributions followed the procedures of
Paloposki (1994). Experimentally measured bubble
CHEMICAL ENGINEERING COMMUNICATIONS 1109
sizes were organized into discrete classes (bins)
with identical width. For the literature data, the
original bins were used, except when a minimum
number of five bubbles were not guaranteed, in
which case bins were modified or grouped to
ensure statistical significance. The best set of
parameters for each combination of operative
conditions and for each of the 14 tested PDFs
was the one which minimized the chi-square stat-
istics [Equation (7)], where (Nhyp,i) and (Nexp,i)
are the theoretical and experimental numbers of
bubbles within each bin and M represents the
number of bins.
�2
XM
Nhyp;i Nexp;i
2
v0 ¼ ð7Þ
i¼1
Nhyp;i
The theoretical number of bubbles within each
bin was calculated for each PDF using the hypo-
thetical parameter values and the corresponding
CDF (P(x)) by Equation (8), where N is the total
number of bubbles, xi is the upper end, and xi−1
the lower end of the ith bin.
Nhyp;i ¼ N ½Pðxi Þ Pðxi 1 Þ� ð8Þ
All calculations were performed with Microsoft
Excel® 2016 (Microsoft, USA), using the solver
functionality to minimize the value of the chi-
square statistics [Equation (7)]. Test computations
of the chi-square statistics were performed with
IBM’s SPSS® package version 21 (IBM, USA),
which validated the Excel results.
The chi-square statistics in Equation (7) may be
used to test if a sample of data came from a popu-
lation with a specific distribution (Snedecor and
Cochran, 1989). A sample of bubbles comes from
a population with a specific distribution if
Equation (9) holds, where the right-hand side is
the chi-square critical value with DF degrees of
freedom and significance level a, DF being the dif-
ference between the number of data bins, M, minus
one, and the number of the adjusted parameters, k
(DF ¼M − 1 − k). In general, the significance level
is chosen at 5% (a ¼ 0.05). When the chi-square
statistics does not exceed the critical value, the true
hypothesis that the data follow a specified distri-
bution cannot be rejected at the stated statistical
significance level (Paloposki, 1994).
v20 < v21 a;DF ð9Þ
1110 H. J. O. PINHO ET AL.

p-Values for the chi-square test, which represent
the probability that the critical value of the chi-
statistics exceeds the value obtained in the fitting
procedure, were used to compare different PDFs
taking into account the different numbers of
parameters. Higher p-values mean greater agree-
ment between experimental and fitted results.
Coefficient of determination (R-squared, or
simply R2) is widely used to measure the goodness
of fit for linear models. Despite being deemed a
poor evaluator of the goodness of fit of nonlinear
models (Spiess and Neumeyer, 2010), R-squared
was used here due to its universality and simplicity
of reading in comparing the goodness of fit. How-
ever, it was not the main criterion to distinguish
the fittings.
Sauter mean diameter calculations
Sauter mean diameter (d32) is the most important
parameter obtained from a BSD, since it is directly
used in the calculation of heat and mass transfer
area. Agreement between d32 directly calculated
from experimental BSD and calculated from BSD
modeled through PDF is therefore an alternative
valuable criterion for goodness of PDF fitting.
Equation (10) is a measure of the Sauter mean
diameter relative deviation, d32,dev
K �
� �
1X d32;hyp;j d32;exp;j �
d32;dev ¼ ð10Þ
K j¼1 d32;exp;j
where d32,hyp,j represents the Sauter mean diameter
calculated with the number of bubbles within each
bin, Nhyp,i, estimated using a PDF, while d32,exp,j
represents the Sauter mean diameter calculated
with the number of experimental bin-grouped bub-
bles, Nexp,i. K represents the number of evaluated
data sets. d32,hyp,j and d32,exp,j were calculated by
Equation (1), where di represents the mean
diameter for each bin (di ¼ (xi þxi−1)/2), and Ni
either Nhyp,i or Nexp,i.
To evaluate the bin processing effects, d32,pop
was also estimated using the complete bubble
population in the present work, replacing the total
number of bubbles, N, for the number of bins, M,
and the real measured individual bubble diameters
for the mean bin diameter, di, in Equation (1). This
calculation was not possible to perform for the
literature data.
Results and discussion
PDF assessment
Data from this work
Table 2 contains the experimental conditions of
the present work, the number of bubbles measured
for each set of experimental conditions, and the
calculated arithmetic (d10) and Sauter mean
diameters.
Figure 2 presents the average goodness of fit
criteria evaluated for the 14 PDFs tested. The
values presented represent the average of the nine
experimental data sets. The vertical intervals in
the figure represent the spread of the chi-square
statistics for the experimental data sets for each
fitted PDF.
Since the number of bins was equal to nine for
all data sets, the critical chi-square value is 12.6
for the two-parameter PDFs, 11.1 for the three-
parameter PDFs (NT3 and UL3), and 9.5 for the
four-parameter LH4 PDF. p-Values may be directly
comparable because they account for the number
of adjustable parameters. Average p-values showed
significance for the NT3, RR, and UL3 PDFs
(higher than 0.05).
For individual data sets (Figure 3), NT3 PDF
shows statistical significance for eight of the nine

Table 2. Experimental conditions and observed representative bubble diameters.

Agitator speed Gas flow rate Estimated Number Minimum Maximum
Data set (rps) (rpm) (�10−3 m/s) (vvm) power (W/m3) of bubbles diameter (mm) diameter (mm) d10 (mm) d32 (mm)
1 5.00 (300) 1.03 (0.265) 513 926 0.10 5.01 1.31 2.54
2 2.04 (0.529) 432 940 0.05 4.67 1.41 2.59
3 3.74 (0.968) 371 1015 0.08 5.58 1.71 3.00
4 6.67 (400) 1.03 (0.265) 1189 1095 0.14 5.09 1.32 2.23
5 2.04 (0.529) 1001 1191 0.09 4.98 1.43 2.31
6 3.74 (0.968) 861 997 0.10 5.29 1.51 2.58
7 8.33 (500) 1.03 (0.265) 2281 1129 0.13 5.23 1.30 2.05
8 2.04 (0.529) 1920 1264 0.13 4.83 1.32 2.25
9 3.74 (0.968) 1651 1135 0.10 5.99 1.32 2.32
 CHEMICAL ENGINEERING COMMUNICATIONS 1111

Figure 2 Goodness of fit indicators. Bars represent average reduced chi-square for tested PDFs fitted to experimental data. Vertical
lines represent minimum and maximum values of reduced chi-square. Circles represent average p-value and squares represent
average R-squared.

data sets, RR PDF shows significance for four data
sets, LH4 PDF for three data sets, and UL3 PDF for
one data set. NT PDF and G PDF also show
significance for one data set.
The R-squared was higher for the same four
PDFs (Figure 2). The G, BE, and NT PDFs also
showed an average R-squared greater than 0.95.
Figure 4 shows the average d32 deviation with
d32 calculated from experimental data after bin
grouping. Five PDFs showed an average relative
deviation lower than 5%. NT3 PDF has an average
relative deviation of 0.4%, and a maximum devi-
ation of 0.8%. The N, RR, LH4, and UL3 PDFs
have average relative deviations of 3.3, 3.7, 3.8,
and 4.1%, respectively. The N PDF was surprisingly
good at predicting d32 after data fitting. d32 calcu-
lated with the NT3 PDF was very close to the
experimental results for all tested operating
conditions (Figure 5). The other PDFs showed high
relative d32 deviations for some operating con-
ditions. RR shows higher deviations for lower input
power conditions with a maximum deviation of
6.9% for data set 7. N PDF does not show a regular
trend on the d32 relative deviation. LH4 PDF shows
very high deviations for data sets 1 and 4, two of
the three lower power input conditions. UL3 PDF

Figure 3. Individual data set p-values for three-parameter Nukiyama–Tanasawa (NT3), Rosin–Rammler (RR), four-parameter
log-hyperbolic (LH4), and three-parameter upper limit (UL3) PDFs. Data set operating conditions according to Table 2.
1112 H. J. O. PINHO ET AL.

Figure 4. Average relative deviation between d32 calculated from PDF fitting results and d32 calculated from experimental
bin-grouped data. Intervals represent minimum and maximum values. Maximum values higher than 40% are not showed.

ranks the fifth best average relative deviation but
with low dispersion from that value.
In general, the PDFs with the best fitting to
experimental data were the NT3, RR, LH4, and
UL3, in that order. The N PDF was revealed to
be an acceptable alternative to estimate the d32
after data fitting. RR and N have the advantage
of requiring only two fitting parameters.
Literature data
Six data sets were extracted from Samaras et al.
(2014) work. The BSDs were estimated from the
author’s figures presenting bubble size probability
against bubble diameter. Due to the smaller tank
volume used by Samaras et al., agitation speed
and superficial gas velocity ranges exceed that of
the present work. With the exception of one data
set, however, the gassed power was within the
range of this work. Samaras et al. data were orga-
nized in nine bins for direct comparison with data
from this work.
Figure 6 presents the results from the fitting
of the 14 tested PDFs. The critical values of the
chi-square statistics are the same as referred
for the present work data. Although all fittings
show chi-square values higher than the critical
ones, the UL3 and NT3 PDFs have the
best behavior, followed by the NT and G PDFs.

Figure 5. Relative deviation for d32 calculated from PDF fitting results and d32 calculated from experimental bin-grouped data.
Three-parameter Nukiyama–Tanasawa (NT3), Rosin–Rammler (RR), Normal (N), four-parameter log-hyperbolic (LH4), and three-para-
meter upper limit (UL3) PDFs.
 CHEMICAL ENGINEERING COMMUNICATIONS 1113

Figure 6. Goodness of fit indicators for Samaras et al. (2014) data sets. Bars represent average reduced chi-square for tested PDFs
fitted to experimental data. Vertical lines represent minimum and maximum values of reduced chi-square. Triangles represent average
d32 deviation and squares represent average R-squared.

For these data sets, the RR PDF only obtains the
11th position but gives the best estimation of the
d32, showing a d32 average deviation of 0.7%.
From Martin’s data (1995), eight data sets were
extracted. The operating conditions for three data
sets are slightly below the ranges covered in the
present work. Gassed power of four data sets is
outside the present work’s range of values.
Bubble size distributions were estimated from
the author’s figures presenting bubble number fre-
quency against bubble diameter. Martin’s data are
bimodal, with a high frequency peak very close to
zero diameters, the maximum contribution of
which to d32 is only about 0.5%. As all the tested
PDFs are unimodal, these very small bubbles were
neglected in the calculations.
Bubble size distribution data were organized in
nine bins to allow a direct comparison with the
present work’s results. Maximum bubble sizes
interpreted from the author’s work was 6 mm.
The average d32 deviation between the bin-grouped
diameters and the d32 given by the author
was 2.0%.
Figure 7 presents the results from the fitting of
all the tested PDFs except for LH4 PDF, which
does not converge for two data sets. The critical

Figure 7. Goodness of fit indicators for Martin’s (1995) data sets. Bars represent average reduced chi-square for tested PDFs fitted to
experimental data. Vertical lines represent minimum and maximum values of reduced chi-square. Triangles represent average d32
deviation and squares represent average R-squared.
1114 H. J. O. PINHO ET AL.

values of the chi-square statistics are the same as Table 3. Nukiyama–Tanasawa and Rosin–Rammler parameter
those for the present work’s data, as already correlations with the input gassed power.
mentioned. All fittings present chi-square values PDF parameter correlations R2 F-value
�
1:48 (12)
b ¼ 6:43 � 10 6 PVG 0.876 0.016
higher than the critical ones, and higher than the �
p ¼ 9:43 � 10 15 PVG
4:29 (13) 0.852 <0.001
values obtained with Samaras et al.’s (2014) data. �
q ¼ 14:8 PVG
0:279 (14) 0.838 0.038
The lower chi-square values were obtained for � 0:0892 (15)
m ¼ 2:89 PVG 0.669 0.024
the NT3, N, RR, and UL3 PDFs by that order. �0:171 (16) 0.713 0.004
n ¼ 0:475 PVG
d32 deviations follow the same order: 0.6% for the
NT3 and N PDFs, and 14 and 20%, respectively,
for the RR and UL3 PDFs. There is not a single PDF that accurately
From Barigou’s data (1987), three data sets were describes all the literature data analyzed. The LN
extracted. BSDs were estimated from the author’s PDF, sometimes mentioned as appropriate for
figures presenting bubble number frequency BSD description, is not among the best ranked
against bubble diameter. Maximum bubble size PDFs.
was 5.65 mm. The NT3 and RR PDFs, which best described the
The average d32 deviation between the present authors’ original data, showed to be a
bin-grouped diameters and the d32 given by the reasonable descriptor of BSD in the case of NT3
author was 1.8%. Figure 8 presents the results from PDF, and a reasonable estimator of d32 in the case
fitting the 14 tested PDFs to the experimental data. of RR PDF.
The critical value of the chi-square statistics is the
same as the value found for the present work’s
data. The lower chi-square value was obtained Correlation of PDF parameters with
for LH4 PDF, but all values were higher than the experimental conditions
critical ones except for the G and UL3 fittings to Data from this work
one data set. All fitted PDFs give very low d32 The dependency of the adjusted PDF parameters
deviations, less than 2% except for N, F, and BE, on the operative conditions was tested for the four
the PDFs with the worst fittings. RR PDF does PDFs which best fitted the original experimental
not rank well, but the fitting quality indicators data and for the normal PDF. The latter was stud-
are similar to the best ranked PDF. ied because of its simplicity and universality and its

Figure 8. Goodness of fit indicators for Barigou’s (1987) data sets. Bars represent average reduced chi-square for tested PDFs
fitted to experimental data. Vertical lines represent minimum and maximum values of reduced chi-square. Triangles represent average
d32 deviation and squares represent average R-squared.
 CHEMICAL ENGINEERING COMMUNICATIONS 1115

PDF parameter, ϕk and ψk are the corresponding

correlation parameters.
� �wk
PG
ck ¼ /k ð11Þ
V
Equation (11) is used since it has been shown
that in aerated stirred tanks, bubble size correlates
well with PG/V for both coalescing and noncoales-
cing systems, both at impeller discharge and in the
bulk of the tank (Alves et al., 2002).

Figure 9. Parity plots for PDF parameters from gassed power
correlations vs. Parameters directly from experimental data. (a)
RR: ▪ parameter m; ● parameter n; (b) NT3: Δ parameter b;
� parameter p; & parameter q. Dashed line represents identity.
accuracy in predicting d32. A simple correlation
with gassed power (PG) per liquid volume (V)
was tested [Equation (11)]. γk represents each
Nukiyama–Tanasawa and Rosin–Rammler PDFs
Table 3 presents the resulting expressions after ϕk
and ψk optimization of the three-parameter
Nukiyama–Tanasawa and Rosin–Rammler PDFs.
Probability density function parameter regres-
sions are significant for both correlations: b, p, q
for NT3 PDF and m, n for RR PDF (all with
F-value <0.05, which represents the Fisher test

Figure 10. Comparison of fitted NT3 PDF to the experimental data sets, identified inside brackets from 1 to 9. X-axis is the average
bubble diameter for each bin (mm) and Y-axis is the number frequency (/mm). ▪ Experimental data; — NT3 PDF directly from
experimental data; ···· NT3 PDF with parameters calculated from correlation.
1116 H. J. O. PINHO ET AL.

p-value). The corresponding correlation para-
meters are also significant (ϕk and ψk always with
P < 0.05, for both correlations). Figure 9 presents
parity plots for both correlations: parameters
correlated with gassed power against the original
parameters fitted directly to the experimental data.
Figures 10 and 11 present the comparisons
between the experimental BSDs for the nine
experimental data sets and the fitted three-
parameter Nukiyama–Tanasawa and Rosin–
Rammler PDFs, respectively. The figures also
include the BSDs calculated using the same
distributions but with PDF parameters computed
from the correlation with gassed power. The
experimental data show a pronounced effect of
the operative conditions on the BSD shape, which
can be satisfactory modeled by both the NT3 and
RR PDFs. High power input to the dispersion
causes a pronounced number frequency peak at
lower bubble diameters and a decrease in number
frequencies at higher bubble diameter sizes,
decreasing the BSDs tails. Both the NT3 and RR
PDFs correctly follow these BSD profiles.
Three-parameter Nukiyama–Tanasawa distri-
bution PDF with parameters calculated from the
power correlation [Equations (13)–(15) of
Table 3)] has the biggest deviation from the experi-
mental data on the data set 7, which corresponds to
the higher input power. RR PDF, with only two
parameters [from the power correlations of
Equations (16) and 17) of Table 3], presents a more
stable description of power effects.
No expressions for the normal, log-hyperbolic,
and upper limit PDFs parameters are presented,

Figure 11. Comparison of fitted RR PDF to the experimental data sets, identified inside brackets from 1 to 9. X-axis is the average
bubble diameter for each bin (mm) and Y-axis is the number frequency (/mm). ▪ Experimental data; — RR PDF directly from
experimental data; ···· RR PDF with parameters calculated from correlation.
 CHEMICAL ENGINEERING COMMUNICATIONS 1117

since they do not correlate significantly well as a Conclusion

function of PG/V.
Bubble size distributions in aerated stirred tanks
have been successfully modeled by PDFs. However,
Literature data
the literature is lacking in:
Three-parameter Nukiyama–Tanasawa and Rosin–
i. A systematic comparison of alternative
Rammler PDFs’ parameters correlated in the
modeling functions and
previous section [Equations (12)–(16) in Table 3]
ii. correlations between modeling function
were used to estimate the BSDs for Samaras et al.
parameters and operating conditions.
(2014), Martin (1995), and Barigou (1987), from
To systematically evaluate the modeling of
experimental or calculated gassed power in these
bubble size distribution in air-sparged vessels
authors’ experiments. The resulting BSDs were
agitated by Rushton turbines, 14 different PDFs
then used to calculate d32 using the procedure
were studied and fitted to bubble size distributions,
described in the “Sauter mean diameter calcula-
both original and retrieved from the literature. The
tions” section.
results obtained indicate that:
Figure 12 compares d32 thus calculated with the
i. Bubble size distributions in air-sparged
d32 obtained after bin grouping of experimental data.
vessels agitated by Rushton turbines may be
For Samaras’ data, d32 deviation was 5.6 and 6.3%
reasonably modeled by the three-parameter
for the NT3 and RR PDFs, it was 4.8 and 7.5% for
Nukiyama–Tanasawa PDF, and acceptably by
Martin’s data and 20.9 and 24.5% for Barigou’s data,
the two-parameter Rosin–Rammler PDF;
respectively. Globally, considering the data from all
ii. the parameters of these two PDFs can be
authors, including the present work, d32 deviation
correlated with the experimental power of
was 7.5 � 3.2% for the NT3 PDF (P ¼ 0.33;
the impeller; and
r ¼ 0.525) and 8.4 � 3.5% for the RR PDF (P ¼ 0.53;
iii. both PDFs, with parameters correlated with
r ¼ 0.491). Results show that the BSDs in aerated
power data, provide good predictions of
agitated tanks may be reasonably represented by
bubble size distribution and Sauter mean
two-parameter correlations on dissipated power,
diameter.
resulting in good approximations for the Sauter
The correlations obtained may be useful in
mean diameter. It should be recognized that the data
improving the application of CFD to air–water
were retrieved from the literature and used in this
systems in stirred tanks, and set an example
work for comparison results from a smaller number
for similar correlations in other multiphase
of measured bubbles, which may significantly
systems.
contribute to the poorer fittings.

Nomenclature
a upper limit distribution parameter
b Nukiyama–Tanasawa distribution parameter
D impeller diameter, m
d10 arithmetic mean diameter, m
d32 Sauter mean diameter, m
d32,dev Sauter mean diameter relative deviation
d32,exp,j Sauter mean diameter calculated with
the experimental number of bin-grouped
bubbles, m
d32,hyp,j Sauter mean diameter calculated with
the theoretical number of bin-grouped
bubbles, m
Figure 12. Parity plot of d32 calculated with correlated
parameters against bin-grouped experimental data d32, for all d32,pop Sauter mean diameter calculated with the
analyzed data sets: ● Present author’s data; Δ Samaras et al. whole bubble population, m
(2014) data; � Martin’s (1995) data; & Barigou’s (1987) db bubble equivalent diameter, m
data. (a) Three-parameter Nukiyama–Tanasawa PDF; (b) Rosin– di bubble diameter, m
Rammler PDF. DF degrees of freedom
1118 H. J. O. PINHO ET AL.

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