Chamcd Engmemng Scmcc

1577 Vol 32 PP 229-232

Per@moo Press

Pnnted m Great Bntam

INTERFACIAL AREA FLUIDIZED

CZESJLAW STRUMILCO
L6dz Techmcal Umverslty,

IN THREE-PHASE BEDS
and TADEUSZ KUDRA
Poland

Institute of Chemical Engmeenng,

(Received 14 January 1976, accepted 20 July 1976)

Abstract--On

pseudo-first order reaction method was adapted for the determmation

of our previous mvestmtions, Danckwerts 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 the basis of mass transfer models and the results

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, among other thmgs, m&t be produced by mcorrect mterpretabon of expenmental data caused by neglectmg the different hydrodynanuc condltlons of two-phase gashquld systems, mto which movable packmg elements are mtroduced For the correct mterpretatton of experunental results on heat and mass transfer m three-phase fluidlzed beds, the phenomena at the Interface, mamly surface renewal rate, are of basic unportance In tbs paper the mves@ation has been concerned with the determmation of the mterfacml area m the turbulent bed contactor, takmg mto account the hydrodynanuc characterrstlcs of three-phase flmdlzed beds Danckwerts pseudo-fist order reaction method [S, 91 which enables the independent determmation of mterfacml area and mass transfer coefficient, was adopted 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 Danckwerts model[8] leads to R = acd/(D(k, or
+ s))

-AL-o0

The scheme of expertmental eqmpment IS shown m Fe 1 The construction parameters of the movmg 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 data The mam part of the column-measurmg section was a glass pipe 0 085 m mner 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 experunents 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 hydrodynamic con&tlons of the three-phase Amtied bed, and with

(1)

xzQ2k
c*D

+Qzs

(2)

The absorption rate IS a hnear function of kl If all remammg parameters are constant the plot of expresslon (2) agamst k, should gwe a stratght hne of slope a2 and mtercept Q S In this method the correct results are obtamed when the chemical reactton rate constant IS of the same order as the interfacial surface renewal rate Takmg mto 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 Danckwerts method
229

Fig 1 The scheme of expenmental eqtupment 1 Section V&I movmg bed, 2 Cuculatmg tank, 3 Demster, 4 Turbomd plate, 5 Elements of packmg, 6 Spray, 7 Elecplc heater, 8 Water coohng, 9 Sturer, 10 Onfice meter, 11 Sensor of termoanemometer, 12 Blower, 13 Gauqe, 14 Carbon &oxide flask, 15 Carbon Qoxlde
rotameter, 16 Liqrud pump, 17 Tank, 18 Pressure electromc system, 19 Llqmd rotameter pulsation

230

CZESZAW STRUMIEZO and TADEUSZKUDRA

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 samples 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 determined by rotameter The pressure at several pomts of the apparatus was measured by means of an electromc system 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 C OH- = 2-3 g ion/l before absorption overall hquld volume v=181 gas temperature To = 303K liquid temperature TL = 303K The liquid analysis was carried out by a standard potentlomemc tltratlon[lO] The gas analysis was performed by automatic analyser INFRALYT T

The absorption

rate was determined

from the relation (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 water evaporation and hquld drop entramment, was taken mto account The physical solublllties of CO1 in hydroxide and bicarbonate solutions were calculated by Van Krevelen and HoftlJzer [ 111 log (H/H,..) = - 2 KJ

(5)
the

usmg the values of Kc and H, given by Barrett[l2] The dlffuslvltles were estnnated by means of relation I, T = const

(6)

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

TREATMENTOFDATA

When the gas side resistance 1s neglwble, the basic equation of Danckwerts pseudo-first order reaction method of determination mterfaclal area 1s

y=
The necessary were calculated

R2 = a%1 + u*s p =H2D

reqmred for Danckwerts plot

quantities as follows

Durmg our expenments a constant change Wlfh time of hydroxide ion concentration m the absorbmg solution was observed The relation between hydroxide ion concentration 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

Fe 2 The concentrationof hydrovlde ion vs absorption tune

Intmfaclal area m three-phase fluldmzxi beds 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 indicates 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 IS of the order of 103-lo5 s- Because the range of pseudo-first order reaction rate constant was of the order 104,the 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

231

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 NiJsmg 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 IS shown by way of example m Figs 4 and 5 It 1s to be seen from the figures that an mcrease 111 gas 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 maximum value A(u, s 3 m/s, H,, s 120 mm) were correlated by the empmcal relationship
A = 2 15 Y~~L~H~~~ ~;;O~, m2/m2

N = (c, - cr) d/(Dls + k,) sunphfies to the form N = (c, - C,)V/(Dkl)

(7)

(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 tbs case It 1s not only the speed of chemical reactron which controls the total 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)

(11)

The eqn (11) was obtained on the basis of statistical

t50
A ~r&n? 5 75 10

The analysis of the results of works by Kosew et al IS] Gelperm et al [71 and Woimak and Bstergaard [6], carried

d,lmml

I
50

I
80

L /mJ/m*h Ij
110

Fig 3 Danckwerts plot

Fig 4 Dataof mterfaczal area measurements

232
150 20 LO Im2/m3 60 80 100

CZ~WAW STRUMIUO and TADEUSZKUDRA

120
IL0 I60

ItlmmmJcEs

J~rrn7rnl

[l] MIodzmskl B and Warych I, Nowa Technrka WNT, Warszawa 1973 [2] Koch R and Kuhsa R, Kokumny polkowe z warstwu ruchomego wypeln#enur Prace naukowe Inst Lnz Chem I Urzadzen Cleplnych P W . Wrociaw 1973 [31 Stumdlo Cz , Adarmec J &d Kudra T , Ch&tuckyPrrimysl

1974 24 85 c41 Strumdlo Cz , Adamlec J and Kudra T , Znt Chem Engng

ISI Kosew A, Peev G and Elenkow D , Verfohrenstechnlk

5 340 Wozmak M and Ostergaard 161 K

1974 14 652

1971

, A report on mass transfer

c.@n/sI

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 was equal 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 three-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
NtYI ATlON

mterfaclal area per unit volume of floating bed mterfacial area per umt cross section of column concentratton of carbon dtoxlde at interface dtiuslvlty of carbon dloxlde m hqmd solubfllty 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 Indices 1
W

bed contactor Techmcal Unrverslty of Denmark, Department of Chemlcat Engmeermg, Lyngby. Denmark 1972 [71 Gelpenn N I , Grlszko W Z , MlchaJlow W A and Sokolow W I, CHZSA 72 181 Danckwerts P V , Gus-Lrquul Reuctrons McGraw-Hill, New York 1970 191 Danckwerts P V , Kennedy A M and Roberts D , Chem Engng Scr 1963 18 63 WI Ewmg G W , Instrumental Methods of Chemical Analysrs, McGraw-Hdl, New York 1960 Cl11 Van Kreveien D W and HofQzer 0 I, Chum Znd Congris International de Chemle Zndustnelle 1948 168 WI Barrett P V L, Ph D Thesis, Umverslty of Cambrrdge (1966) R A T D , Hendrlksz R H , Kramers H , Chem 1131 NIJS~II~ Engng Scr 1959 10 88 r141 Porter K E , Kmg M B , Varshney R C , Trans Znst Chem Engrs 1966 44 274 WI Kudra T , Ph D Thesis, Technical Umverslty, Lodz (1975) [161 Pohoreclu R , Prace Nuukowe Pohtechmka Warszawska. Chenua nr 5, 1970 Z , tmpubhshed materials, Instytut Inzymeru 1171 Pakowslu _. Chemiczne] PL [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 rnuestrgutlons m a turbulent
APPJmDlx

COINaOH reachon takmg place m ths system wdl be of pseudo-fist order d the mequahty aven by Danckwerts and Sharma[l9]

Dk, &s)J( -zc 1

?r

,COH_

(12)

of hquld

dc,dt

instantaneous value water rate of absorbent change

active

part

concentration

IS fulfilled Under the experunental conditions, takmg D = 153 X lo- cm*/s H = 1 46 x lo- mole/cm3 at, z = 2, s = k, = 5 51 x lo4 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 10-4C, thus satisfying the Isothermal absorption 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]