Chemical Enginrcrinx Science, Vol. 47, No. 9-I I. pp. 2475-2480, 1992. 0009-2509/92 $S.OO+O.

OO
Printed in Great Britain. @ 1992 Pergamon Press Ltd

Gas-Liquid Reactor in the Synthesis of Urea

M. Dente, M. Rovaglio, G. Bozzano, A. Sogaro

Dipartimento di Chimica Industriale ed Ingegneria Chimica “G. Natta”
Politecnico di Milano, Italy

A. Isimbaldi
Tecnimont SPA, Italy

Abstract
In spite of the fact that urea has raised to become the most important fertilizer, till now a scant scientific
attention has been devoted to the understanding of the detailed behaviour of the reactor wherein the
urea synthesis takes place. It is a typical gas-liquid reactor involving not only backmixing fenomena. but
also significant aspects of heat and mass transfer between vapor and liquid phases, together with liquid
and g&-liquid h&mogeneous and heterogeneous phases ‘ equilibria- and kinetics_ Fluid dynamic
problems are created by the cocurrent gas-liquid flow through the perforated plates which generates
intermittent bubbles s warms. Purpose of this paper is to present bases and results obtained through a
“ complete” modelling (covering thermodynamic. kinetic and fluid dynamic aspects) of gas-liquid
stagewise reactor, and comparison with real data of commercial units. Original kinetic equation and
some thermodynamic data related to the very complicated equilibria involved are also presented.

1.rntroduction
In the operating conditions range, adopted Into the various urea processes, both gas and liquid phase
are present. Gas phase is constituted by ammonia, carbon dioxide. water and some inerts (including
passivating agents). Their relative amounts. along the reactor. depend on the prevailing operating
conditions (pressure, temperature, N’ H3/CO2, H20/C02 ratios ). The liquid phase contains physically
dissolved and chemically combined CO2. NH3. H20, UREA. Combined components are mainly present
as ions like NH4+. NH2CO2-9 HCO3- and other minor constituents. (In the jargon of the urea plants
specialists, the all is indicated as urea/carbamate solution: in the real situation also bicarbonate is
competing).The main reactions taking place in the liquid phase are the following:
(I) CO2,liq + 2 m3,liq = =I4+ + NH2co2-
(2) H201iq + NH2co2- = I=IQ.liq + HCO3-
(3) NH4+ + NH2co2- = (NH4NH2CO2) =uREA +H2Oliq
The first reaction is strongly exothermic: the second and the third ones are endothermic. The three
reactions are reversible. The first two are so fast, in both the directions, that can be practically
considered at the equilibrium. The third one constitutes the rate determining step for urea formation.
Along the reactor, the liquid is increasing at the expense of the gas phase; ammonia. carbon dioxide,
urea, water (and the ions related to them) change their relative amounts and are exchanged between the
two phases: urea resides into the liquid. Heat and mass transfer between the phases and kinetic of the
urea reaction dominate the behaviour of the reactor. As a consequence the conversion of carbamate into
urea is actually not only dictated by the equflibrium limitations of urea reaction. as conventionally
considered, but also by the fluid dynamics existing into the reactor. The modem reactors are practically
adiabatic. The usual shape is a vertical cilinder fed by, at least, two streams, a vapor one (CO2 rich) and a
liquid one (NH3 rich). both entering from the bottom and generating an upward movement of the phases.
For the most diffused processes, operating at medium pressure (14oC200 bars). the conversion per pass
is such to need recycling of the unconverted matter. Therefore, water, free ammonia. ammonium
carbamate. bicarbonate and some urea are usually present in the liquid stream recycled to the reactor.
Into the reactor, the formation of new carbamate provides the temperature rise that is necessary for
achieving convenient rates for reaction (3). i.e. formation of urea. The temperature profile is
progressively rising inside the reactor. A modem example of an urea reactor, IS schematically
represented in the fig. 1 (Pagani. 1982). Two different zones can be distinguished: between them a stream
of superheated NH3 can be introduced with the aim of increasing further@ the yields by acting on the
NH3/CO2 ratio. If the additional stream is not added. the lowest section is operating only with liquid
phase just as a further resfdence time. The movement of the bubbles swarms is active in promoting the
mixing of the liquid phase: with the aim of reducing the backmixing some perforated plates are usually
introduced into the reactor, giving it a stagewise structure (this is common to all the modem urea
reactors). The reactor can be conveniently considered, for the liquid phase moclelling. like a sequence of
CSTR’ s. Conversely, a plug flow model for the gas phase is suggested for every stage. Some general
considerations regarding the reactor are worthy to be mentioned:
l The ratio N/C in the various processes spans mainly the range from about 2.5 to 4. with a maximum of
5. Correspondingly, the conversion of total CO2 to urea is spanning mainly from about 55% to 70% with
a maximum of 80% (for the highest N/C).

2475
 2476 M. DENTE er al. D6

-The operating pressure, for maintaining most of the

eflluent in the liquid phase, has to be higher as the N/C
ratio is higher: it ranges mainly from 140 to 200 barn with a
lTlaximunl of 400 bars.
l The exit temperature stream ranges from about 185O C to
--
5
195O C. with a msximum of 2100 C (for the highest values of
-- pressure and N/C).
--
7
- The residence time spans from about 1200 to 2500
5 seconds.
--
5
--
.
2.Thethermodynamicfi-amework
-- Za.The liquid php#:the thermodynamic frsmeworkweare
5 referring to has been the basis of a satisfactory simulation
--
model of the entire urea process (Dente et al. , 1988 ). The
a
.- - real components already mentioned dictate the
1 thermodynamic behaviour of the solution. Formation of
15
blunt and presence of inerts dissolved into the liquid, will
-- be disregarded in the modelling. For the global material
14 balances. it is convenient to characterize the solutions by
--
15
“ equivalent components” that are the same, except urea.
-- appearing in the gas phase as real components. They are
--
l.zI equivalent NH3. equivalent CO2 eqnivalent H20 The
deiinition of the equivalent components is represented by
the following equations in terms of molar amounts:
WNH3,tot = WNH4+ WNH2cO2 + WNH3
wcO2,tot = WC02 + WHC03 + WIuH2co2
WH20,tot =WH20 + WHco3
that connect the real components to the equivalent ones.
Fig. 1:Example ofurea reactor The (local) total amount of NE.0 in the liquid phase is then
given by:
(4) WN.tot = WNH3,tot + 2WIJREA
WC. tot = wco2, tot + WUREA
wo.tot = WH20,tot + 2wc.tot
- WCREA
Since the global material balances will be performed in terms of equivalent components whilst both
the urea reaction rate and the rate of exchange between the two phases are governed by the molar
fraction of the real components, it is necessary to evaluate the molar fractions of the six real
components ( NH3. H20. CO2. NH4 +* HCO3-, NH2CO2-) as a iunctlon of local urea. equivalent local
components amounts and temperature. This result is accomplished by adding the electroneutrality
balance of the ions and the equilibria of the reactions (1) and (2):
(7) WNI-I4 = WNH2co2 + WHco3
,loo~? NH2c02TNH4 wtot -Zc02 UrNtIq
WI
*02m32 WC02 WNH3 2
“ IHCO3*INH3 WI-E03 WNH3
(97 K2on=
W2CO2@20 WNI-IzCOzWHzO
where by deflnition
(10) wtot = WNH3 + WC02 + WH20 + WLIREA+ WNH4 + WNH2cO2 + WHC03
The ions content of the solutions is usually so high that no ei&ient theory is available for the a-priori
extimation of the effect of the composition on the activity coeificients ri. They have been determined
through the elaboration of experimental equfflbrium data and empirical formulations: the only condition
to be given to them is to be coherent (in some asymptotic sense) with the behaviour of the system when
the solution become binary and low ionic strength. For developing and tuning the thermodynamic
informations (including the urea equilibrium), several experimental sets of data available in the
literature, have been used (see for instance. Long and McDevit 1952. Inoue et al. 1972. L.emkowitz et al.
1971). The satisfactory results of the thermodynamic assumptions have been already confirmed (Dente
et al. 1988). Without entering into details on this, it has appeared more convenient to express the
equations (8’ ). (9’ ). in terms of “ apparent equilibrium constants” , product of the “ real” equilibrium
constant (that is only function of the temperature) and the pertinent activity coefficient (function of
temperature and composiUon). Therefore, by putting:
YNHZCOZ *INH4
KlCl. 4 = K1° Ul
‘ IcO2 ? NH3

the equations (8’ ). (9’ ). can be rewritten in the (equivalent) way:

D6 Gas-liquid reactor in the synthesisof urea 2477

wtot WNH2cO2 WNH4 WHco3 WNH3

(8) K1 = (9) ~=wNH~co.-pH20
WC02 wNH32
The system of nonlinear algebraic equations (4) to (10). when the local temperature. urea. equivalent
components axnounts are given, allows the determination of the local amounts of the real components.
The expressions for the evaluation of K1.Q. are reported in Dente et al. (1992)
2.b Urea aqulllbrium: for evaluating the rate of the (reversible) reaction 3 it will be necessary to
establish the local vslue of the *‘ apparent equilibrium constant” K3:
WuRKAWH20
(11) K3fT.X) =
WNH4 UrNHzCoz
where the timction K3cT. X ) are given in Dente et al. (1992).
Because K3 is a function of the local equilibrium composition. it is necessary to calculate the
hypothetical complete equilibrium (urea included) of the liquid phase (given the total local amounts of
N. C. 0 and the temperature). Therefore. the equations to be solved are the same as before. together with
eq. (11). The final composition allows the determination of the complete equilibrium and, as a
consequence, the value of the apparent costant K3 ( see Appendix A).
2-c Liquid-vapor equilibrium: the elaboration of the literature data allows the determination of the
heterogeneous equilibria at the interface between the two phases. The equilibrium condition at the
interface follows the usual rules :
(12) figPi = ~*lTi*Xi
By putting ~i’ l-li/f@i it results:
(13) Pi= Ki*Xi
where Xi = XNH3. xco2. xH20. are the molar fractions of the real components. while the interface
equilibrium costants Ki are reported in Dente et al. (1992).
The previous equations give the local gas phase composition (at the interface) as a function of the
composition of the liquid phase. Ki coefficients are combination of liquid and gas thermodynamic
behaviour. The vapor molar fractions at the interface are: yi= Pi/P= (Ki/P)Y$
At the top of the reactor the total pressure is assigned (and stage by stage it is varying as a function of
the hydraulic head): it means that also the condition:
(14) p(l-Winerts/WGtot) = KNH3 XNH3 + KC02 Xc02 + KH20 XH20
has to be locally satisfied. It flxes the temperature at the vapor-liquid interface.
In perforrnlng the global balances stage by stage it is necessary to connect inter-facial mass fraction of
gas components to interfacial mass fractions of liquid equivalent components and interfacial
temperature. The algebraic system of all the equations given up to now constitutes the connection: once
the evaluation has been performed, it is convenient to deduce. stage stage, the ratio Hi between the
gas and the liquid equivalent components mass ii-actions at the intc !Yace (where the homogeneous (1).
(2) and the heterogeneous equilibria (11) are established):
(15) Xi= (W,i/Xi )’
Of course, Hi is just a fictitious proportionality factor, that can be deduced after the local resolution of
the homogeneous and heterogeneous equilibria.
2.6 Enthalpy for liquid phase: the molar enthalpy of the liquid is evaluated by assuming that the
solution is constituted of the “ salts” components (ammonium carbamate and bicarbonate), URKA NH3 ,
CO2 physically dissolved and H20. The molar enthalpy proposed for the “ salts” is the enthalpy of
formation of their solutions into water at nominally InBnite dilution and standard temperature (298 KJ:
(it is like to assume that. at the iniinite dilution, water. ammonia, and urea are equivalent diluents). These
values. are then corrected for the temperature effect. assuming that the “ salts” in the infinltely diluted
solutions have the same molar specific heat of the pure molten “ salts” . Free ammonia and water are
assumed to have the same properties of the pure liquids , at the same temperature and partial pressure.
Urea is assumed to have the same enthalpy of the pure molten urea at 298 K plus a correction Ull to the
local temperature: the molar specific heat takes into account the association effects of urea with
ammonia and water. Free CO2 is assumed to have the same enthalpy of CO2 gas at the same
temperature and partial pressure. The excess enthalpy of the solutions is assumed to have the following
expression, function of both temperature and composition:
(16) Hmlx’ (l- w~~3)[-241 -18.8(2ro~3-1)+34.8(2~3-1)2) (l-O.o02cT-313))
2-e Enthalpy for vapor phase: the gas mixture is assumed to be ideal (no excess enthalw for the vaoor
mixing). The properties &e assumea to be those of the pure components at the same t&xxature &rid
partial pressure . For CO2 and NH3 the corrections against non idealitv are given bv KKS method: for
&I20 the steam tables representation is preferred. O&r its critical ter&xat&e. the pure llquid and
gaseous NH3 is assumed to have the same properttes at the same pressure and temperature. Inerts are
assumed as ideal gas.

3. The reactor model

The formation of urea takes place in a two phases reactor where several phenomena play an important
role. Thermodynamics, kinetic, fluid dynamics as well as heat and mass transfer need to be InvesUgated
for developing a robust and suitable simulation model. Since the thermodynamic framework has been
already given let’ s go now on the other equations needed for the complete description of the unit.
3.a Fluid dynamlca : As pointed out before, Inside every stage the gas moves through swarms of
bubbles. generated by the holes of the sieve tray. The size of the bubbles is such that they will coalesce
2478 M. DENTE et al. D6

before crossing the n& tray: because of the fact that the liquid and vapor simultaneous passage
through the holes is physically not allowed, the consequence becomes that the bubbles swarms arc
intermittent. In this case the local gas fiacUon within the swarm fs higher, the sfze of the bubbles fs
larger, their rising velocity is lower than fn the case of a continuous bubbles swarmf ng. Thfs aspect has
been taken into account in the modellfng of the average volumetrfc mass and heat transfer
coeMcfents.The average diameter of the bubbles in a swarm generated through a sieve tray is gfven
(Schaftfefn and Russel. 1968) by:

(17) Db=2.s4[~~]“ .071[~]1’3_h_ we= do220 Fr - &-

The bubbles are flattened because of their size. Their termfnal velocity in a quiescent liquid is then
approximately gfven by (see for fstance RatcheIor . 1970):

In theusuaf oondftfons vt is quite higher than the superfWal velocities of both gas and lfqufd. Thfs fact
allows some sfrnplfflcations in extimatfng the volumetric gas holdup. within the bubble swarms. in
presence of fntermfttency. by the following expression:
r
3vG+vb 3VG + Vb 2 4VG
(19) hg= 0.5
I( 1+
vt I-I/(
l+

The average g& holdup fn a &age is given by:

vt 1 -F
.
1

(20) F= hg I@
where @ is an “ intermfttency factor” evaluated as
(21) + vG
(vc. + vr)
(It takes into account that the fntermfttent 8 warms of bubbles are separated by slug of continuous liquid
phase) More details about the correlations used can be found fn Refth et al. (1963). Pavlfca and Olson
(1970). Considering that pnxctfcally only the cap of the flattened bubbles is mostly active for heat and
mass transfer, the active fnterfacfal area becomes per unit volume of a stage :
&F
(22) a= -
The geometry of the trays (sometimes
only part of their area is perforated), the
specfffc situation of the ffrst stage
(where the fmmfssion of vapor is made
through perforated vertical pipes) and
so on, have suggested to introduce a
kfnd of “effectiveness factor” of a stage,
as a multiplier of the specfflc surface
.ThL parameter has been ratfonallzed in
some way: the expression proposed is
the followfng:

3.b Chemical Kinetic : the slow

chemical step involved in this system is
constituted by the reaction (3) occurring
in the liquid. Very few results can be
found in the lfterature on this subject.
The only available data on bench scale
continuous reactor are those of
IGol’dbeg and Al’tshuler (1963). On the
basis of them and of several other data
Pressure (a t m ) from commercial units it has been
Fig. 2: C-G&Men experimental and model possible to propose and check the
following expression for the kinetic rate
of reaction (3).

(24) r= K e-Eatt/RT X ~4 -2~02 - x uy34” ” )

where K3 is the afore’ mentioned apparent equflfbrfum co&ant of the reaction. The values of K and
Eatt have been establfshed (Meottf, 1986) as: K= 4.2 lo1 1 Kmol/m3/s: Eatt/R = 16000 K
The small sfze of the experfmental reactor (0.01 m diameter. 15.0 m length). e place to a slug flow of the
lfqufd and gas. t can be observed (varying the pressure) the transition Ffv rom a fluid dynamic regime
domfnated by mass and heat transfer (low pressure) to a regime dominated by chemical kfnetfcs (high
pressure): in the latter, the pressure has no more effect on the urea yield. because most of the volume is
occupied by the liquid phase. Figure 2 compares the experimental results and the model prediction. The
comparison is satisfactory on the total range of condftfons.
3.c Mass and heat bda na sr : t he reactor model is based on the followfng assumptions:
- the liquid phase (in the stage) fs completely mfxed and the gas phase fs a plug-flow:
 D6 Gas--liquid reactor in the synthesisof urea 2479

- the interface is at the equilibrium for the real corresponding components;

- the mass balances in the liquid refer to the equivalent components. as already defined;
- inerts are considered only in the gas phase.
Therefore, the other equations of the model become. into the single stage:
- vapor phase (plug-flow) (251%~ 41 a(bNH3, CO2. HZO,
(inerts are not exchanged with the liquid)
- liquid phase (completely mixed) (26)hout-L,m =Jia+ viMi rV
( ‘= NH3eq. C02eq. H20eq. UREA]
3.d Conditions at the Interface: In order to express the mass fluxes as a function of only the bulk
compositions of the phases two properties are necessary. Fllstly the continuity of the mass fluxes at
the interface. i.e.:
(27) Ji’Gl = mtotw’c,i * P&(G’(eG.i - OIG.3 = Ji[Ll = mtot O’L.i + PL%n)(olL,i - %.i)
(containing both the convective and diffusional contribution)
Secondly the interface equilibrium condition expressed by the equations (151, introducing the fictitious
correlation coefficient Hi _ By combining (27) e (28) the interfacial mass fractions are derived:
(pc +& i +PLKI~ -LJ)
(28) &,.I =
m&l-Hi) + ph &(G)Hi + PLK$L)
--_
and the inter-facial mass fl6ces~become:
(29) Ji = mtot@Gm(G)q.‘ + PL=(LIHiorL.i )+ PGKi(G1(W.i - Hi0L.i)
mtot(1 - HiI + p~Ki(~'Hi+ PL@
Hi has to be evaluated at the interface conditfons. however it is a relatively weak function of the
compositions: therefore, in order to avoid numerically cumbersome solutions of the system (28). it is
worthy to exUmate Hi at the bulk composition but with the interface temperature (Hi =w*,i/co~i) where
aG*,i are the values of the gas phase at the local equilibrium corresponding to the bulk liquid
composition. Incidentally this is coherent with the assumption of very high enhancing factors for the
mass transfer coetllcients in the liquid phase ( because of the very high rates of the reactions (1) and (2) 1.
The interface composition is practically disappearing from the list of the unknowns and Jf can be
approximated by :
c30) J‘=mtot &G,‘ + PG k,‘ ( %.I - @G.d
3.e Enthalpy balance: every stage is practically adiabatic, so that:
(31) 3 h,LcqLout+~h‘G~Gout= %?pJ Lin + WiG CoiGin
where index is extended to all the re components of the liquid phase_
3.f Contin IA ty of the energy fluxes at the interfkce : as a good approximation the equation is :
(32) & Ji (hiG- hi.eqL ) = h~cTi - ‘fg) + hbmi - T L)
where hL i.eq are the enthalpies. per unit per mass, of the equivalent components NHQ,~~, COZ,~~.
H20, in the liquid phase, so that hiG. hi,eqL is just the equivalent of a pseudo-vaporization heat
(inclu 8 ing the decomposition of the NT-4NI-i2CO2 and NlQHCO3 together with the vaporization of NH3
and H20 from the solutions): the combination of the algebraic equation (28- 33) allows the
determination at the interface of the liquid and gas composition. temperature, mtot. mass fluxes Ji as a
function of the bulk properties of gas and liquid. Some more simplifications. based on realistfc
assumptions, reduce the computational efforts and have been adopted into the mathematical model of
the reactor.
3.g_ Mass and Heat transfer coefticients: they are derived from the following dimensionless formula:
C;; ,,,,,-51 -
N-2+0.0187 Re 0.484 Pro33s

wher NUT= \f(h D&l with h = l‘ql tli d orgas heattransfercoemcents

(KG,‘ w
NUrn = 0.66 Reoe5 SC1 i3 where Num I

Q-t3Tbi
4. Comparison of the Model Results with
CommercialPlant Data
193 In the following tables a sample of the comparisons between
the results of the model and the data of commercial plants
is presented. The agreement on yields and final
189 temperatures is well satisfactory. Generally speaking, it has
to be pointed out that, the previous kind of data are the only
experimental informations available. However, sometimes
173 also the temperature nroflle. taken in some intermediate
1Sb7911lsls stages is avaihxble. Fig&e 3 shows a typical simulation of the
liquid temperature profile along the reactor. The few
experimental data conArm the shape of the profile. The data
Fig. 3 : T)qidliqiq b;e pnsented here. part of all those available, cover a wide range
of operating condltiona and reactor size. such to contlrm that
the proposed model can be considered suitable and reliable.

en 47719/11-x
2480 M. DENTE er al.

canposi~~enios(maes fraction) 1 stager number 15

co2 @'Hs H20 tm.p.-c e trays perforated area (8 on total):
0.34 0.68 0.5 0.01 202 e 2 3 and 4 17 l
inlet liquid flow-rate 150000 Kg/h
co2 NH3 H2O urea wmp.'C
0.44 0.40 0.12 0.04 180
further NH3 to stage 1 30000 Kg/h
temperature 167 'C t liq. temp.

let liquid flow-rate 25000 Kg/h

CC2 NH3 H20 urea temp.oc

Example s: Conventional macfoT g@oxnetryof 1MK) t/d capacl~

Plvce88 mm oamllatry dam
top pressure 150 tin internal dlametar 25 m
inlet gas flow-rata 4650: Kg/h total height 38 m
comDoaitions wass fraction) total mtaaeo number 11
co2 NH3 l-l26 inel-tx tenlp.~C sieve t&s perforated area (S on total):
0.99 0.0 0.0 0.01 120 fron atage 2 to 11 0.6 +
inlet liquid flow-rata 160000 Kg/h c IRP. PBm
I
CO2 NH3 H20 wea tmp.oc Yield 60 60 9
0.19 0.67 0.13 0.1 135 Outlet 11q. temp. 190 oc 190 oc

Symbology
:ectlvc-- KG.L.I :-hnIuli?r~cicrlta of-polwti
: molar fraction8 of -iponult : liquld-vqor tC&Ihbrium constant of component 1
% :acth-e- 2 :p====
Atot :tDtal- Pt :pamal~of-ponent1
:buwtc-e T :tCalpXshlXe
: hole dIamctar Y
; : fLI&pdtycacmctalt of -pmlent I ; Z_.Z”
G.L :totaIgpsandllquld maMfkmmtcB k :molar~oC-poncnti
hG.L : heat trsnsfer coef3dcnts n : actMty cacffldcnt of component 1
Y : “ pseudo-Hemy’ -tmnt of componentI t :vqorpmmmxmof-pomnt1
4 :-nwcfor-poncnti P : damtty
I@ : real equllibllum constant :8UTfWCtUN&lX&
K1.z.s : apparent equililxium constant G : maaa6-actlaM of component 1
=TOT :total-etratlon~p~ Di : diffixdon weIRcent of c component
: chclmal dmuemg
It :vaporpramureof-panaltt

Batchelor : ” An introduction to Fluid

rQn=F, Plerucd , Sogam, Carlcml. Wgo 1:
%na?Z%~~bP%unfvcraity~~~~)Comp. Chem. Engng. 12, 389

~$~~&~e.~ 2 pubbhd ( 199%

acronco ic Kinetics and Mechanism of the synthesis of urea from ammonia and carbon
diode” . t Chem. En+ 2. IQ0 (1
rnoLle*Kanat. otsuka : Eqlimm m oi Urea Syntheti I”. Bull. Chem Sot of Japan. 43 4339 1972
Inoue.Kanai.Oteuka : ” Equilibrium of Uma BynthesIa II”, Bull. Chem. Sot. of Ja 4s: 18Q8 bQ72{
’ mthadfortheumarcactor” . y Icogaku. 37. 96 tlm
Yinuur, Van den Berg : ” Bubble pa t measurement In the ammonia-carbon dtoxfdc system” , J.
Appl. C$c-hS+!ioL, 21.229 (1971)
: ” A&Wily Coeffkienta of Nonelectrolyte Solutes fn Acqueoua 8alt 8olutlon” . Chdc. Rev., 61, 119
ff%)
mcesa” , Nitro@m. 127.29 (1982)
for Continuous-Contact Mass Transfer Operations” , Ind. Chem. Eng.. 62.48
yzi) Benken. Israel “ Gas Holdup and Axial Mixing in the fluid phase of bubble cohanns” , Chen~ En& Ski.. 23,619