R. Jafari; R. Sotudeh-Gharebagh; N. Mostoufi -- Modular Simulation of Fluidized Bed Reactors

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Modular Simulation of Fluidized Bed Reactors

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  • Full Papers Modular Simulation of Fluidized Bed Reactors

    By Rouzbeh Jafari, Rahmat Sotudeh-Gharebagh, and Navid Mostoufi*

    Simulation of chemical processes involving nonideal reactors is essential for process design, optimization, control and scale-up.

    Various industrial process simulation programs are available for chemical process simulation. Most of these programs are being

    developed based on the sequential modular approach. They contain only standard ideal reactors but provide no module for

    nonideal reactors, e.g., fluidized bed reactors. In this study, a newmodel is developed for the simulation of fluidized bed reactors

    by sequential modular approach. In the proposed model the bed is divided into several serial sections and the flow of the gas is

    considered as plug flow through the bubbles and perfectly mixed through the emulsion phase. In order to simulate the

    performance of these reactors, the hydrodynamic and reaction submodels should be integrated together in the medium and

    facilities provided by industrial simulators to obtain a simulation model. The performance of the proposed simulation model is

    tested against the experimental data reported in the literature for various gas-solid systems and a wide range of superficial gas

    velocities. It is shown that this model provides acceptable results in predicting the performance of the fluidized bed reactors. The

    results of this study can easily be used by industrial simulators to enhance their abilities to simulate the fluidized bed reactor

    properly.

    1 Introduction

    Fluidized beds have been used as industrial reactors in the

    processes involving catalytic and gas-solid reactions for more

    than 50 years. In spite of the extensive research efforts on

    fluidization during these years, many features of such reactors

    which strongly influence their performance have only recently

    begun to be understood. The uncertainties associated with

    scale-up and modeling of fluidized beds is a significant

    obstacle in the widespread use of fluidized beds in chemical

    industries [1].

    Two types of phenomena, i.e., physical and chemical, coexist

    in the fluidized beds. The physical phenomenon corresponds

    to the bed hydrodynamics, i.e., properties of bubble and

    emulsion phases. The chemical phenomenon corresponds to

    the chemical changes occurring in each phase. In order to

    model a fluidized bed properly, one has to consider two

    submodels describing these two phenomena: the hydrody-

    namic submodel which explains the physical phenomena, and

    the reaction submodel which describes the chemical reactions

    occurring in the bed.

    Fluidized beds are hydrodynamically more complex than

    other gas-solid contactors, mainly fixed and moving bed

    reactors. Thus, it is important to understand and characterize

    the parameters influencing the hydrodynamics of fluidized

    beds [1,2]. Various hydrodynamic models are presented in the

    -

    [*] R. Jafari (MSc), Dr. N. Mostoufi (author to whom correspondence should be addressed, e-mail: [email protected]), Dr. R. Sotudeh-Gharebagh, Process Design and Simulation Research Center, Department of Chemical Engineering, Faculty of Engineering, University of Tehran, P.O. Box 11365-4563, Tehran, Iran.

    literature. Hydrodynamic models are divided into three

    general categories, i.e., single-, two- and three-phase models.

    A large number of these models are developed based on the

    two-phase concept of fluidization. In this category of models,

    the fluidized bed is divided into two sections, i.e., bubble phase

    (rich in gas) and emulsion phase (rich in solids). Early two-

    phase models employed quite simple assumptions, such as the

    existence of solid-free bubbles and the emulsion phase to be at

    minimum fluidization condition [1]. However, the existence of

    solid particles in bubbles has been shown both experimentally

    [3,4] and theoretically [5,6]. The emulsion phase also does not

    remain at the minimum fluidization condition and may

    contain a higher amount of gas at higher gas velocity [4,7]. A

    fluidized bed may operate at several fluidization regimes,

    mainly bubbling, turbulent and fast fluidization regimes. Most

    of the hydrodynamic models available in the literature are

    applicable only to one of these regimes. Recently, there have

    been few attempts to develop hydrodynamic models which

    could be employed at various fluidization regimes [8-10].

    Numerous methods have been introduced in the literature

    for fluidized bed reactor modeling and simulation. Weiss et al.

    [11] simulated a fluidized reactor by dividing it into 11 serial

    blocks, each of them being a continuously stirred tank reactor

    (CSTR) for both gas and solid phases. Basu et al. [12]

    developed a model in which a plug flow regime for both the gas

    and solids is assumed. Lee and Hyppanen [13] presented a

    model which considers the CSTR and plug flow reactor (PFR)

    for gas phase and solid phase in the reactor riser, respectively.

    Soutudeh-Gharebagh et al. [14] simulated the circulating

    fluidized bed combustor by ASPEN PLUS by combining

    some standard blocks and user-written kinetic subroutine.

    Alizadeh et al. [15] simulate the polymerization fluidized bed

    Chem. Eng. Technol. 2004, 27, 2 DOI: 10.1002/ceat.200401908 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 123

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    124 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.de Chem. Eng. Technol. 2004, 27, 2

    reactor using CSTRs in series. El-Halwagi et al. [16] also

    presented the three-phase model for fluidized bed reactor

    simulation by PFRs and CSTRs for bubble, cloud and

    emulsion phases. These models either have not yet been

    implemented in the industrial process simulation programs or

    have used simplified hydrodynamic assumptions. The hydro-

    dynamics of such reactors become very important when highly

    exothermic reactions take place in the reactor.

    Various process simulation programs, such as ASPEN

    PLUS, PRO/II, HYSYS, CHEMCAD, DESIGN II and

    INDISS, are available and are employed for process simula-

    tion purposes by industrial entities. All these programs have

    been developed based on the sequential modular approach,

    i.e., they consist of different standard modules which could be

    combined together to represent the whole process. These

    process simulators are generally not strong in reactor modules

    and only contain standard, ideal reactors, such as PFR and

    CSTR. In spite of their vast use in the chemical industries, a

    fluidized bed reactor module is not offered in these programs.

    In this work, a fluidized bed reactor model is presented by

    combining the standard reactor modules available in the

    process simulation programs. These standard modules have to

    be combined in a logical way to represent the reality in the

    fluidized bed reactors. Furthermore, the model has to be easily

    applicable in all process simulation programs.

    2 Model Implementation

    A fluidized bed reactor is a nonideal reactor, i.e., it cannot

    be considered as either a PFR or a CSTR. It has been tried by

    some researchers to model such nonideality by the tanks-in-

    series model (e.g., [11,15,16]). However, these models ignore

    the main aspect of gas-solid fluidization, i.e., coexistence of

    bubble and emulsion phases in the reactor. The movement of

    gas through the bubbles in the fluidized bed could be

    considered as plug flow while it could be considered as

    completely mixed in the emulsion phase. Therefore, while the

    whole reactor could be axially divided into several sections,

    each section itself may be considered to be consisting of two

    ideal reactors: a PFR to represent the gas flow through the

    bubbles and a CSTR to represent the gas flow through the

    emulsion. Such an approach is closer to the reality than the

    previous models which consider each section as a CSTR. A

    schematic diagram of the ith stage of the proposed model is

    Figure 1. The schematic diagram of the ith stage.

    parameters of the fluidized bed properly, compared to other

    hydrodynamic models [17-19].

    - The reactor operates at isothermal conditions. As a result,

    the hydrodynamic parameters of the bed, physical proper-

    ties of components and reaction rate constants are

    considered to be constant throughout the bed.

    - Radial gradients within the bed are neglected.

    As mentioned before, the bed is divided into a number of

    equal-volume stages, each consisting of two phases, i.e.,

    bubble and emulsion. The generalized steady-state mass

    balance equation for either bubble or emulsion phases in a

    reacting stage is:

    illustrated in Fig. 1. It is assumed that first the reaction takes

    place in each reactor of each stage and then the mass transfer

    occurs at the exit of the reactors between the effluents.

    ( bulk flow

    \

    in

    ( bulk flow

    \

    out

    ( dissapearance by

    \

    chemical reaction

    Additional assumptions considered in developing the

    model are:

    ( mass

    \

    transfer

    = 0 (1)

    - The bubbles reach their equilibrium size quickly above the

    distributor. Therefore, the bubble diameter is assumed to be

    constant along the bed height.

    - The hydrodynamics of both phases could be characterized

    by the dynamic two-phase (DTP) model [9]. It has been

    shown that this model could estimate the hydrodynamic

    By applying Eq. (1) to the system shown in Fig. 1 for the

    reactant A, the mass balances in the ith stage for bubble and

    emulsion phases are given by the following equations1):

    -

    1) List of symbols at the end of the paper.

    CAbi CAei

    CAb(i-1) CAe(i-1)

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    (A U U

    D u Ee

    (i)

    N

    Bubble phase: zi

    The hydrodynamics and mass transfer coefficients needed

    to solve these equations are given in Tab. 1. Number of CAb(i 1) Ub Ab Ab Eb

    {

    zi 1

    rA(i) dz Kbe (CAb(i) divisions, n, in these equations is the parameter of the model

    that has to be determined from the experimental data. CAe(i) )Vb(i) CAb(i) Ub Ab = 0 (2)

    Emulsion phase:

    CAe(i 1) Ue Ae rA(i) VCSTR(i) + Kbe (CAb(i)

    3 Results and Discussion

    As has been mentioned in the previous section, the bed

    ( o \

    CAe(i) )Ve(i) 1 o CAe(i) Ue Ae = 0 (3) height is divided into a number of divisions with equal

    Table 1. Hydrodynamic and mass transfer equations of the model.

    Bubble diameter [25] Db = Dbm (Dbm Dbo ) exp

    ( 0.15hmf

    \

    D r

    0.4

    ( o mf )\

    Dbo = 0.8713 D

    Dbm = 1.6377(

    A(Uo Umf )

    0.4

    Bubble velocity [26] Ub = Uo Ue + ubr

    ubr = 0.711/

    gDb

    Bubble to emulsion mass transfer coefficient [1] 1

    Kbe

    1 =

    Kce

    1 +

    bc

    ( \ AB br

    Kce = 6.77 D3

    b (

    Ue

    \ (

    D g \

    Kbc = 4.5 D + 5.85

    0.5 AB D

    0.25

    5/4

    b b

    Bubble phase fraction [9] o = 1 Af (1) Af (2) exp

    ( (Uo Umf )

    \

    A f (3) (

    (Uo Umf )\

    Bubble phase voidage [9] Eb = Avoid b(1) + Avoid b(2) exp

    Avoid b(3)

    Emulsion phase voidage [9] Ee = Avoid e(1) + Avoid e(2) exp

    ( (Uo Umf )

    \

    A

    Volume of the ith stage V

    Vt

    (i) = n

    void e(3)

    Volume of bubble phase in each stage Vb(i) = V o

    Volume of emulsion phase in each stage Ve(i) = V(i) (1 o)

    Volume of PFR in each stage VPFR(i) = Vb(i) Eb

    Volume of CSTR in each stage VCSTR(i) = Ve(i) Ee

    K

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    =

    volumes. This number is a parameter of the model developed

    in this work and has to be determined from the experimental

    data. Several sets of the experimental reaction data carried out

    in fluidized bed reactors are available in the literature. Five

    series of experimental data sets are employed in this work.

    These data are as follows:

    - Grace and Sun [20] carried out ozone decomposition

    reaction in a fluidized bed. Air was used as the fluidizing

    gas and the reaction is first order with respect to ozone.

    - Fryer and Potter [21] carried out ozone decomposition

    reaction in a fluidized bed. Air was used as the fluidizing gas

    and the reaction is first order with respect to ozone.

    - Shen and Johnstone [22] carried out catalytic oxidation of

    nitrous oxide in excess of oxygen. Oxygen was the fluidizing

    gas and the reaction is first order with respect to nitrous

    divisions which would best fit the experimental data was

    chosen to be the total number of stages in that case. It was

    found that in the case of slower reactions and higher gas

    velocities a larger number of stages are required to simulate

    the fluidized bed reactor accurately as compared to the faster

    reactions and lower gas velocities for which the reactor could

    be simulated even with a single stage. In fact, a higher gas

    velocity enhances the solids mixing and also makes the gas

    pass faster through the bed, thus, the whole bed could be

    simulated as a smaller number of stages shown in Fig. 1.

    Similarly, a smaller number of stages would be needed if a

    faster reaction is to be carried out in the reactor. Based on this

    discussion, it is proposed that the number of stages is a

    function of the following dimensionless number:

    U oxide.

    - Massimilla and Johnstone [23] carried out oxidation of

    J Ha 0 U

    mf

    (5)

    ammonia in excess of oxygen. Oxygen was the fluidizing gas

    and the reaction is first order with respect to ammonia.

    - Heidel et al. [24] carried out ethylene hydrogenation in

    excess of hydrogen. Hydrogen was the fluidizing gas and the

    reaction is first order with respect to ethylene.

    All reactions considered in this work are first order with

    respect to one of the reactants. Thus, the kinetics used in this

    work can be described by:

    rA = KCA (4)

    The properties and operating conditions of these data is

    given in Tab. 2. These data sets are employed in this work to

    estimate the number of divisions of the fluidized reactor at

    different operating conditions.

    In each case, the bed height is initially divided into a number

    of equal zones. The model equations (Eqs. (2) and (3)) are

    then solved and the results of such solution were compared

    with the corresponding experimental data. The number of

    A faster reaction (higher Ha) and/or higher superficial gas

    velocity (higher U0) both have the same effect on the newly

    defined dimensionless number (higher J) and would result in a

    smaller number of stages to be employed in the simulation

    (smaller n). The minimum fluidization velocity is added to

    Eq. (5) to represent the effect of the properties of the solids in

    the number of stages in the proposed model. The values of the

    number of stages obtained at different operating conditions

    are summarized in Tab. 3 as a function of the dimensionless

    number J.

    Table 3. Number of stages.

    J N

    J < 11.1 1

    11.1 J < < 5.62 2

    5.62 < < J 0.63 3

    0.63 < J 4

    Table 2. The experimental data sets information. In order to determine the valid-

    ity of a hydrodynamic model, it is Parameter Unit Grace and Sun

    [20] Fryer and Potter [21]

    Shen and Johnstone [22]

    Massimilla and Johnstone [23]

    Heidel et al. [24] necessary to check it at the cir-

    cumstances that the hydrody- Dr m 0.1 0.229 0.114 0.114 0.075

    H m 2 2 0.54 0.58 0.26

    dp m 60 117 - - -

    ps kg/m3 1580 2650 - - -

    Umf m/s 0.0026 0.017 0.005 0.014 0.011

    U a m/s 0.6502 1.4182 0.52 1.01 0.75 C

    Emf - 0.475 0.48 0.5 0.5 0.5

    T oC 25 25 427 250 150

    P kPa 101.3 101.3 101.3 101.3 101.3

    K s-1 2.41, 8.95 0.05-0.085 0.003-0.008 0.0446 0.16, 0.27

    U0 m/s Umf-1.2 0.024-0.058 Umf-0.06 Umf-0.06 0.005-0.075

    Geldart - A B A A A

    a) calculated by the correlatoin of Bi and Grace [27]

    namics would be predominant.

    The reactions considered in this

    work could be considered as fast

    reactions. In such a condition, the

    performance of the reactor is

    more influenced by the hydrody-

    namics than the kinetics. In fact,

    since the extent of the mixing in

    the reactor is represented by its

    hydrodynamics, the hydrody-

    namics of the bed becomes the

    limiting step in the conversion of

    the reactant(s) in the case of fast

    reaction rate. Therefore, the per-

    formance of the reactor would be

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    127 Chem. Eng. Technol. 2004, 27, 2 http://www.cet-journal.de 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

    E: K=2.41(1/s)

    E: K=8.95 (1/s)

    C: K=2.41 (1/s)

    C: K=8.95 (1/s)

    K=2.41 (1/s)

    K=8.95 (1/s)

    Ca

    cula

    ted

    Co

    nv

    ersi

    on

    (%

    )

    mainly characterized by its hydrodynamics at the conditions of

    the experimental data employed in this work.

    Results of the model presented in this work are compared

    with the experimental conversion of ozone in the fluidized bed

    reactor reported by Grace and Sun [20] at different superficial

    gas velocities and various reaction rate constants in Fig. 2. The

    parity plot of calculated against experimental conversions is

    also given in Fig. 3. It could be seen in these figures that the

    proposed model is in good agreement with the experimental

    results in predicting the fluidized bed reactor performance for

    different reaction rate constants and a wide range of super-

    ficial gas velocities.

    100

    100

    80

    60

    40

    20

    90 0

    0 0.2 0.4 0.6 0.8 1 80 K (1/s)

    Figure 4. Fluidized bed reactor conversion as a function of reaction rate constant 70

    at different superficial gas velocities (E: experimental [21], C: calculated).

    60

    100

    50

    40 80

    30

    0 0.2 0.4 0.6 0.8 1 1.2 60

    U 0 (m/s)

    Figure 2. Fluidized bed reactor conversion as a function of superficial gas

    velocity at different reaction rate constants (E: experimental [20], C: 40 calculated).

    100 20

    90 0

    0 20 40 60 80 100

    80 Experimental Conversion (%)

    Figure 5. Comparison of experimental data of Fryer and Potter [21] with calculated results employing sequential modular approach.

    70

    60

    50

    40

    40 50 60 70 80 90 100

    Experimental Conversion (%)

    Figure 3. Comparison of experimental data of Grace and Sun [20] with calculated results employing sequential modular approach.

    Results of the model presented in this work are compared

    with the data reported by Fryer and Potter [21] in terms of the

    conversion of ozone at different reaction rate constants and

    various superficial gas velocities in Fig. 4. The parity plot of

    calculated against experimental conversions is also given in

    Fig. 5. Similar to the previous case, these figures show that

    there is a good agreement between the proposed model and

    the experimental results in predicting the fluidized bed reactor

    performance for different reaction rate constants and super-

    ficial gas velocities. However, by increasing the reaction rate

    constant, the model prediction deviates from the experimen-

    tal data. According to the discussions made earlier, in the case

    of fast reactions the hydrodynamics becomes the limiting step

    in characterizing the reactor performance. In this case, the

    deviation could be contributed to the fact that the constants of

    the DTP model are evaluated for a particle which is slightly

    different from the catalyst employed by Fryer and Potter [21]

    in terms of particle properties, even though both are Geldart B

    particles.

    The conversions calculated based on the model developed

    in this work are compared with the data reported by Shen and

    Johnston [22], Massimilla and Johnston [23] and Heidel et al.

    [24] in the parity plots given in Figs. 6, 7 and 8, respectively. As

    illustrated in these figures, the agreement between the model

    E: Uo=0.024 (m/s)

    E: Uo=0.046 (m/s)

    E: Uo=0.081 (m/s)

    C: Uo=0.035 (m.s)

    C: Uo=0.058 (m/s)

    E: Uo=0.035 (m.s)

    E: Uo=0.058 (m/s)

    C: Uo=0.024 (m/s)

    C: Uo=0.046 (m/s)

    C: Uo=0.081 (m/s)

    K=0.04 (1/s)

    K=0.14 (1/s)

    K=0.32 (1/s)

    K=0.85 (1/s)

    X A

    (%

    ) C

    acu

    late

    d C

    on

    ver

    sio

    n (

    %)

    X A

    (%

    )

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    K=0.003 (1/s)

    K=0.005 (1/s)

    k=0.008 (1/s)

    80 100

    80

    60

    60

    40

    40

    20

    20

    20 40 60 80 100

    Experimental Conversion (%) 0

    0 20 40 60 80

    Experimental Conversion (%)

    Figure 6. Comparison of experimental data of Shen and Johnstone [22] with calculated results employing sequential modular approach.

    30

    20

    10

    0

    Figure 8. Comparison of experimental data of Heidel et al. [24] with calculated results employing sequential modular approach.

    a number of equal-volume stages in which the gas in bubbles

    moves as plug flow and the gas in emulsion is completely

    mixed. The number of stages was evaluated from the data

    available in the literature and found to be a function of Ha, U0 and Umf. Since the proposed model consists only of the ideal

    reactors, which are available in the commercial process

    simulation programs, it is possible to introduce the nonideal

    fluidized bed reactors in such programs by this model. The

    model is easy to use in all process simulation programs which

    are also developed based on the sequential modular approach.

    The comparison between the model results and the experi-

    mental data indicates that the proposed model is able to

    predict the real performance of the fluidized bed reactors

    satisfactorily over a wide range of superficial gas velocities

    (i.e., bubbling and turbulent regimes of fluidization) both

    Geldart A and Geldart B types of particles. A more reliable

    prediction of the reactor performance would be achieved if

    the parameters of the DTP model are evaluated specially for

    the catalyst employed in the process.

    0 1 0 20 30

    Experimental Conversion (%)

    Figure 7. Comparison of experimental data of Massimilla and Johnstone [23] with calculated results employing sequential modular approach.

    prediction and experimental data is satisfactory. However, the

    under- or overprediction of the conversion in some cases

    shown in these figures should be mainly attributed to the fact

    that the number of stages, n, may assume only integer values.

    4 Conclusions

    A new hydrodynamic model is developed for fluidized bed

    reactors based on the sequential modular approach. The

    proposed model is a combination of the tanks-in-series model

    for nonideal reactors and the two-phase concept of fluidiza-

    tion. According to this model, the fluidized bed is divided into

    Acknowledgement

    The financial support of the University of Tehran (grant no.

    613-3-739) is gratefully acknowledged.

    Received: July 24, 2003 [CET 1908]

    Symbols used

    ai [m-1] interphase area per unit volum

    A [m2] cross-sectional area

    Af(1) [-] constant of dynamic two-phase model

    Af(2) [-] constant of dynamic two-phase model Af(3) [-] constant of dynamic two-phase model

    AVoid-b(1) [-] constant of dynamic two-phase model

    AVoid-b(2) [-] constant of dynamic two-phase model

    AVoid-b(3) [-] constant of dynamic two-phase model

    K=0.0446 (1/s)

    K=0.16 (1/s)

    K=0.28 (1/s)

    Cacu

    late

    d C

    on

    ver

    sio

    n (

    %)

    Ca

    cu

    late

    d C

    on

    ver

    sio

    n (

    %)

    Cacu

    late

    d C

    on

    versi

    on

    (%

    )

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    AVoid-e(1) [-] constant of dynamic two-phase model AVoid-e(2) [-] constant of dynamic two-phase model AVoid-e(3) [-] constant of dynamic two-phase model

    CA [kmol/m3] concentration of component A

    DAB [m2/s] diffusion coefficient

    Db [m] bubble mean diameter Db0 [m] bubble initial diameter

    Dbm [m] bubble maximum diameter

    dp [m] particle diameter

    Dr [m] reactor diameter

    G [m/s2] accelaration of gravity

    H [m] bed height

    Ha [-] Hata number ((KDAB)0.5ai/Kbe)

    hmf [m] bed height at minimum fluidization

    condition

    Greek symbols

    ps [kg/m3] solid density

    Eb [-] bubble phase voidage

    Ee [-] emulsion phase voidage

    o [-] bubble phase fraction

    Subscripts

    B bubble phase

    E emulsion phase

    I section no.

    References nd

    J [-] dimensionless number (HaU0/Umf) K [s-1] reaction constant

    [1] D. Kunni, O. Levenspiel, Fluidization Engineering, 2 Heinmen, Boston 1991.

    ed., Butterworth-

    Kbc [s-1] bubble to cloud mass transfer

    coefficient

    Kbe [s-1] bubble to emulsion mass transfer

    coefficient

    Kce [s-1] cloud to emulsion mass transfer

    coefficient

    ND [-] number of orifices in unit area of grid

    N [-] total number of stages

    P [P] reactor operating pressure

    rA [kmol/m3s] reaction rate based on component A

    T [K] reactor operating temperature

    Ub [m/s] bubble velocity

    ubr [m/s] bubble rise velocity

    Uc [m/s] superficial velocity at onset of fluidization

    Ue [m/s] emulsion gas velocity

    Umf [m/s] minimum fluidization velocity U0 [m/s] superficial gas velocity

    Vb [m3] bubble phase volume

    VCSTR [m3] CSTR volume

    Ve [m3] emulsion phase volume

    VPFR [m3] PFR volume

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