strumillo e kudra
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Chamcd Engmemng Scmcc 1577 Vol 32 PP 229-232 Per@moo Press Pnnted m Great Bntam
INTERFACIAL AREA IN THREE-PHASE
FLUIDIZED BEDS
CZESJ LAW STRUMI LCO and TADEUSZ KUDRAL6dz Techmcal Umverslty, Institute of Chemical Engmeenng, Poland
(Received 14 anuary 1976, accepted 20 July 1976)
Abstract--On the basis of mass transfer models and the results of our previous mvestmtions, Danckwerts’pseudo-first order reaction method was adapted for the determmation of mterfacml area m a three-phase flmtid
bed The results of our expenmental mvesttgattons on the absorption of carbon &oxlde UI aqueous sodturn hydroxtde
are presented The works of other authors are analysed
Turbulent bed contactors have been the SubJeCt of
numerous mvestigations[1-4] One of the essential
parameters for the correct design of such an apparatus IS
the lnterfaclal area&71 Analysis of such data shows
considerable dlscrepancles m results obtamed by each of
the authors both m the character of changes and the
values of mterfaclal area These drscrepancles, amongother thmgs, m&t be produced by mcorrect mterpreta-
bon of expenmental data caused by neglectmg the
different hydrodynanuc condltlons of two-phase gas-
hquld systems, mto which movable packmg elements are
mtroduced
For the correct mterp retatton of experunental results
on heat and mass transfer m three-phase fluidlzed beds,
the phenomena at the Interface, mam ly surface renewal
rate, are of basic unportance
In tbs paper the mves@a tion has been concerned with
the determma tion of the mterfacml area m the turbulent
bed contactor, takmg mto account the hydrodynanuc
characterrstlcs of three-phase flmdlzed beds
Danckw erts’ pseudo-fist order reaction method [S, 91
which enables the independent d etermmation of mterfa-
cml area and mass transfer coefficient, was adop ted
When a first or pseudo-first order lrreverstble reaction
with a rate constant k, occurs, the solution of the dtiuslon
equation on the basis of Danckw erts’ model[8] leads to
R = acd/(Dk , + s)) (1)
or
xzQ2k+Qzs
c*D 1 (2)
The absorption rate IS a hnear function of kl If al l
remammg parameters are constant the plot of expresslon
(2) agamst k, should gwe a stratght hne of slope a2 an d
mtercept Q’S
In this method the correct results are obtamed when the
chemical reactton rate constant IS of the same ord er as the
interfacial surface renewal rate Takmg m to account the
bh turbulence of the fhud stream m a three-phase
flmdlzed bed, carbon dloxlde-so&urn hydroxide was
chosen as a test system Thus system ought to fulfil the
condltlons of apphcabtilty of Danckw erts’ method
-AL-o0
The scheme of exp ertmental eq mpm ent IS shown m Fe
1 The construction parameters of the movm g bed column
(such as free cross section of the turbognd plate, he&t of
measunng sectron and the method of hqntd dlstrrbution)
were accepted on the basis of our earher stu&es and the
hterature dataThe mam part of the column-measurm g section was a
glass pipe 0 085 m m ner diameter and 0 5 m he&t
At the column bottom, the turbognd plate was placed
with free cross section equal to 0 65 and slot width equal
to 2 mm On the bottom plate the layer of packmg
elements with a height of Ii&, was placed
The exp erunents were carried out by carbon &oxtde
absorption m the cuculatmg sodium hydroxide solution
from an au mixture
One experunental pomt was obtamed dunng absorption
of COz m NaOH solution with constant hydrodynam ic
con&tlons of the three-phase Amtied bed, and with
Fig 1 The scheme of expenmental eqtupment 1 Section V&I
movmg bed, 2 Cuculatmg tank, 3 Demster, 4 Turbomd plate, 5Elements of packmg, 6 Spray, 7 Elecplc heater, 8 W ater coohng,9 Sturer, 10 Onfice meter, 11 Sensor of termoanemometer, 12Blower, 13 Gauqe, 14 Carbon &oxide flask, 15 Carbon Qoxlde
rotameter, 16 Liqrud pump, 17 Tank, 18 Pressure pulsation
electromc system, 19 Llqmd rotameter
229
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230 C ZESZA W STRUMIEZO and TADEUSZ UDRA
constant concentration of CO2 m air Due to CO,
absorption, the hydroxyl Ion concentration changed
durmg the course of the experiment
The concentration of the absorbmg solution was
determined by potentlometic tltratlon of solution sam-
ples taken at regular intervals of 10 or 5 mm
Constant hqud and gas temperatures were mamtamed
by an automatic temperature regulation system
Gas flow rate was measured by or&e plate and
thermo-anemometer ZBS 11 The hquld rate was deter-mined by rotameter The pressure at several pomts of the
apparatus was measured by means of an electromc
system
The absorption rate was determined from the relation
The condltlons of experunent were as follows
packmg elements, diameters d, = 10 0, 7 5 and 5 0 mm
packing elements, density pW= lOSOkg/m’
static bed hewht H,, = 26160 mm
hquld flow rate L = 33-l 10 m3/mz h
superfacial gas flow rate uo = 0 5-3 5 m/s
CO2 concentration m the a=
at inlet (constant m
absorption runs) c = 34% vol
OH- concentration in solution
before absorption COH- = 2-3 g ion/l
overall hquld volume v=181
gas temperature To = 303°K
liquid temperature T L = 303°K
The liquid analysis was carried out by a standard
potentlomemc tltratlon[lO] The gas analysis was per-
formed by automatic analyser INFR ALYT T
TREATMENTOFDATA
When the gas side resistance 1s neglwble, the basic
equation of Danckwerts’ pseudo-first order reaction
method of determination mterfaclal area 1s
y= R2 = a%1 + u*sp =H2D
The necessary quantities reqmred for Danckwerts’ plot
were calculated as follows
(4)
The experunental pomts descrlbmg the dependence of
NaOH concentration m the absorbing solution on tune
were approxunated by a polynomial of second order On
the basis of the prehmmary experiments, the lmear
change of solution volume, resulting from the waterevaporation and hquld drop entramment, was taken mto
account
The physical solublllties of CO1 in hydroxide and
bicarbonate solutions were calculated by Van Krevelen
and HoftlJ zer [ 111
log (H/H,..) = - 2 KJ
usmg the values of K c and H , given by
The dlffuslvltles were estnnated by
relation
I , T = const (6)
(5)
Barrett[l2]
means of the
where a has been taken as 0 85 (after[l3])
The equation aven by Barrett[ 121 were used to
calculate viscosity of solution, dtiuslvlty of CO* m water
and pseudo-first order reaction rate constant
Pa~Qal pressure of COz was calculated as the anthmetlc
mean value of mlet and outlet
RESULTS
Durmg our expenments a constant change Wlfh time of
hydroxide ion concentration m the absorbmg solution was
observed The relation between hydroxide ion concentra-
tion and tune for some of the test series 1s shown m Fig 2
The polynomial coefficient a, by means of which
experimental points were described for all series was of
the order of 10-5-10” gmolell mm* The correlation error
did not exceed 1% It allows us to state that If the
conversion of NaOH does not exceed 30%, the change m
concentration of hydroxide ion with tune may be
described with sufficient accuracy by a straight line The
6
a
oa
I I I T’ I I I I I Itr,._r I
Fe 2 The concentrationof hydrovlde ion vs absorption tune
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Intmfaclal area m three-phase fluldmzxi beds 231
results confum those of Kosew ef al [S] and Porter et
al [14], who observed a sun&r linear relation for the
COrNaOH system
A plot after Danckwerts’ IS shown as an example m
Fig 3 In all the test series, the experunental points
on Danckwerts’ plot lay on a straight line with a mean
devlatlon of 2% It shows the apphcabrllty of Danckwerts’
model m descnbmg mass transfer m a three-phase
fludlzed bed Also It ndicates that the mterfacral area and
mass transfer coefficient might be determinable by
Danckwerts’ method
It was found, that the surface renewal rate m the
three-phase flmdlzed bed I S of the order of 103-lo5 s-’
Because the range of pseudo-first order reaction rate
constant was of the order 104, he observed results can be
treated as correct The CO,NaOH system has been used
by many workers, because the reaction hnetlcs are well
known In these studies the reaction between carbon
dloxlde and hydroxide ions was treated as mstantaneous
The rightness of such an assumption arose from the fact
of very small surface renewal rate m comparison wtth the
absorption rate constant In such case the equation
N = (c, - cr) d/(Dls + k,) (7)
sunphfies to the form
N = (c, - C,)V/(Dkl) (8)
which 1s vahd for absorption with a very fast chemical
reaction
In this paper It has been shown, that the surface
renewal rate 1s comparable quantltatlvely urlth the
chemical reaction rate constant, so that 111 bs case It 1s
not only the speed of chemical reactron which controls thetotal mass transfer rate According to eqn (7) the mass
transfer coefficient for the absorption of CO* m NaOH
solution m a turbulent bed contractor should be calculated
from the equation
k= = d(Dls + k,) (9)
The analysis of the results of works by Kosew et al I S]
Gelperm et al [71 and Woimak and Bstergaard [6], carried
0 t 2 3 4 5 6 7 8
Fig 3 Danckwerts’plot
out on the absorption of CO, m NaOH solutions m
columns with moving beds, showed that they applied the
method of determination of mterfaclal area for sieve
plates
Consequently, for calculating the hqud phase mass
transfer coeficlent they used the equation
(10)
We found [151on the basis of the analysis of the relations
between parameters E, E , and M (fully discussed by
Danckwertstg]) that the method of determination of
mterfaclal area used m[S-71 1s not appropnate and could
lead to erroneous estlmatlon of this important parameter
Moreover, It was found that they used m their
calculations the reaction rate constant values gven by
Nllsmg et al [ 131 However, the work by Pohoreclu[16]
shows that the reaction rate constant, data of NiJ smg
tiers from the values obtamed by others authors by
about 40%
So, the values of interfacial area obtained m the
work 15-71 can not be treated as completely
unquestionable
The change of mterfaclal area w&h some parameters of
turbulent bed contactor performance obtamed from the
basis of the present mvestlgations I S shown by way of
example m Figs 4 and 5
It 1s to be seen from the figures that an mcrease 111 as
velocltles and static bed height up to a certam value leads
to an increase m the mterfaclal area At higher values of
those parameters the interfacial area decreases It has
been stated on the basis of pressure osclllatlon[17], that m
this range of gas velocity and static bed he&t, the
homogemety of the floatmg bed was disturbed
The results of our own experiments up to the maximumvalue A(u, s 3 m/s, H,, s 120 mm) were correlated by
the empmcal relationship
A = 2 15Y~“~L”~H~~~‘~;;O~, m2/m2 (11)
The eqn (11) was obtained on the basis of statistical
t505 75 10
A ~r&n? d,lmm
/
0 I I L /mJ/m*h j50 80 110
Fig 4 Dataof mterfaczal area measurements
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232 CZ~WAW STRUMIUOand TADEUSZKUDRA
150 20 LO 60 80 10 0 120 IL0 I60
A Im2/m3 J~rrn7rnl
0 c.@n/sI
0 05 10 r5 20 25 3,0 35
Fig 5 Data of mterfacml area measurements
methods, using multiple regressron[l81 For the level of
slgmficance equal to 0 05, the correlation coefficient wasequal to 0 945 In the range of 95% of confidence mterval
were 93% of expernnental pomts
It seems, that the proposed method of determmmg the
mterfaclal area 111 hree-phase fluldued beds could help m
obtammg a better understandmg of the heat and mass
transfer mechamsm m a turbulent bed contactor and
permit the correct design of such eqmpment
mterfaclal area per unit volume of floating bed
NtYI’ATlON
mterfacial area per umt cross section of column
concentratton of carbon dtoxlde at interface
dtiuslvlty of carbon dloxlde m hqmdsolubfllty of carbon dioxide m liquid
iomc strength
pseudo-fist order reaction rate constant
solubdlty factor
rate of mass transfer
parttal pressure
rate of absorption of carbon dloxlde per umt
absorbing volume
surface renewal rate
tune
volume of absorbent m the column
stolchlometic coefficient of reaction
Greek symbol
7 vlscosrty of hquld
I ndices
1 instantaneous value
W water
dc,- rate of absorbent
dt change
active part concentration
It lmmmJcEs
[l] MIodzmskl B and Warych I, Nowa Technrka WNT,
Warszawa 1973
[2] Koch R and Kuhsa R, Kokumny polkowe z warstwu
[3 1
c4 1
ISI
161
[7 1
181
191
WI
Cl11
WI
1131
r141
WI
[161
1171
ruchomego wypeln#enur Prace naukowe Inst Lnz Chem I
Urzadzen Cleplnych P W . Wrociaw 1973
Stumdlo Cz , Adarmec J &d Kudra T , Ch& tucky’ Prrimysl
1974 24 85
Strumdlo Cz , Adamlec J and Kudra T ,Znt Chem Engng
1974 14 652
Kosew A, Peev G and Elenkow D , Verfohrenstechnlk 19715 340
Wozmak M and Ostergaard K , A report on mass transfer
rnuestrgutlons m a turbulent bed contactor Techmcal
Unrverslty of Denmark, Department of Chemlcat Engmeer-
mg, Lyngby. Denmark 1972
Gelpenn N I , Grlszko W Z ,MlchaJ low W A and Sokolow
W I, CHZSA 72
Danckwerts P V , Gus-Lrquul Reuctrons McGraw-Hill,
New York 1970
Danckwerts P V , Kennedy A M and Roberts D , Chem
Chemiczne] PL
Engng Scr 1963 18 63
Ewmg G W , I nstrumental Methods of Chemical Analysrs,
McGraw-Hdl, New York 1960
Van Kreveien D W and HofQzer 0 I, Chum Znd Congris
I nternational de Chemle Zndustnelle 1948 168
Barrett P V L, Ph D Thesis, Umverslty of Cambrrdge
(1966)
NIJ S~II~ A T D , Hendrlksz R H , Kramers H , Chem
Engng Scr 1959 10 88
Porter K E , Kmg M B , Varshney R C , Tr ans Znst Chem
Engrs 1966 44 274
Kudra T , Ph D Thesis, Technical Umverslty, Lodz (1975)
Pohoreclu R , Prace Nuukowe Pohtechmka Warszawska.
Chenua nr 5, 1970
Pakowslu Z , tmpubhshed materials, Instytut Inzymeru_.
[IS] Volk W, Applred Staflstrcs for Engmeers, McGraw-H&
New York 1969
[19] Danckwerts P V and Sharma M M , I Chem E Review
Senes No 2 The Chemical Engmeer, CE 244, 1966
APPJmDlx
COINaOH reachon takmg place m ths system wdl be of
pseudo-fist order d the mequahty aven by Danckwerts’ and
Sharma[l9]
&s)J( 1k, ,COH_
?r -zc (12)
IS fulfilled
Under the experunental conditions, takmgD = 153 X o-’ cm*/s
k, = 5 51 x lo4 s-‘. H = 146 x lo-’ mole/cm3 at, z = 2, s =
1 34 x l(r s-‘, p = 2 76 x 10m2at, con- = 2 mole/I, we have found
the nght-hand side of the relation (12) lo3 times of the left side
The temperature rise near the Interface. calculated accordmg to
Danckwerts[l] was about 10-4”C, thus satisfying the Isothermalabsorption assumption
The error Introduced by neglectmg the gas-side mass transfer
resistance was estunated on the basis of experunents with
absorption of pure carbon &oxlde m sodium hydroxide solution
This resistance was found to be less than 3%[15] The error m
evaluatron of rnterfacml area by eqn (3) does not exceed 5% (on
the basis of error analysts)
The experlmental matenal and the calculation of the results as
well as the mterpretatlon of the theoretlcal and expenmental data
is given in[15]