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DESIGN PARAMETERS OF BUBBLE COLUMN REACTORS WITH AND WITHOUT SOLID SUSPENSIONS Kozo KOIDE** epazment of Industrial Chemical Kanto Gakuln Uni Yokohama 235 Key Words: Bubble Column, § Transfer pended Particles, Hydrodynamics, Gas Holdup, Mass Transfer, Heat ‘Bubble columns with and without solid suspensions have been used widely as chemical reactors and bio- This paper summarizes research on the design parameters of bubble columns with and without solid suspensions, and introduces new trends in research activities such as applications of computational uid ‘dynamics and of newly developed experimental techniques to bubble columns, and research on high pressure bubble columns. Introduction Bubble columns with and without solid suspen- sions have been used widely as chemical reactors, bioreactors and apparatus for waste water treatment, as the structures of the columns are very simple. For design of a bubble column as a reactor, the axial dispersion model (ADM), the cell model with back flow (CMBF), or other simpler models are used, and the design parameters such as gas holdup eo, volu- metric liquid-phase mass transfer coefficient kxa, and axial dispersion coefficients Ze and E; of gas and liquid have been studied exclusively up to the levels where the design parameters can be estimated for bubble columns with pure liquids at atmospheric pressure. However, estimations of the design param- eters are rather difficult for bubble columns with liquid mixtures and aqueous solutions of surface active substances, as these parameters and the fluid flows in bubble columns are affected very much by bubble size distribution, which is controlled by bubble coalescence and breakup. These phenomena are affected by the physico-chemical properties of the solutions used. Since the early 1990s, computational fluid dynamics (CFD) has been applied to gas-liquid (slurry) flow, mass transfer and chemical reaction in bubbie columns for developing a better model for scale-up and design of bubble columns than one- dimensional models such as ADM and CMBF. Also since the early 1990s, new experimental techniques such as Particle Image Velocimetry (PIV) (Tzeng er al., 1993; Chen et al., 1994; Reese and Fan, * Recsved on June 29, 1996, ** Deceased. Correspondence concerning this article should be addressed to K. Ohtaguehi at Dept of hem, Eng, Tokyo Inst of Technol, Tokyo 152. VOL 29 NO. 5 1996 Table 1 Books and reviews of bubble columns and air lift reactors Deckwer and Schumpe (1987); BC, BCS Chisty (1989); AL. Chisty and Moo-Young (1989); AL Fan (1989); BCS Joshi era. (1990); AL Mills eral. (1992); BC, BCS Deckwer (1992); BC, BCS Saxena and Thimmapuram (1992); BCS Ueyama (1993); BC, BCS, AL Deckwer and Schumpe (1993); BC, BCS. Beenackers and Van Swaaij (1993); BCS. ‘Chaudari and Hoffmann (1994); BC Saxena and Chen (1994); BC, BCS ‘Tsuge (1995); BC, BCS, AL Ranade (1995); BC Research Team of BC and BCS (1996); BC, AL AL: Air Lift Reactor, BC: Bubble Column, and BCS: Bubble Column with Solid Suspensions 1994; Chen et al, 1995), Computer Automated Radioactive Particle Tracking (CARPT) (Yang et al., 1992; Devanathan et a.,1995) and radioactive tracer gas (Hyndman and Guy, 1995a, b) techniques have clarified flow structure and instantaneous phase velocities without disturbing flows in the bubble columns. ‘The effects of high pressure on bubble behavior, gas holdup, hydrodynamics and mass transfer have also been studied. In this decade, research on bubble columns, including air lift reactors, has been very active, and recent books and reviews in these fields are listed in Table 1. ‘The objectives of this review paper are to summarize research on the design parameters of ms bubble columns, and to introduce new trends in research activities in this field. Though a huge number of papers have been published on air lift reactors, they are omitted from this review for reasons of space. 1. Flow Regimes and Gas Holdup 1.1 Flow regimes and gas holdup Flow regimes observed in bubble columns are either bubble flow regime or slug flow regime. Most industrial bubble columns are operated in the bubble flow regime. Three different flow regimes are ob- served: homogeneous flow, transition and heteroge- neous flow (churn turbulent) regimes shown in Fi 1fa), (b) and (a). Chen et al. (1994) clarified the macroscopic flow structure of the bubble flow regime by using particle image velocimetry (PIV), and conducted flow visualization of the bubble flow by a laser sheeting technique. They observed three flow regimes: a dispersed bubble regime (homogeneous flow regime), 2 vortical-spiral flow regime shown in Fig. 1(€) and a turbulent flow regime (heterogeneous, flow). The vortical-spiral flow regime observed at Ug=0.021 - 0.049 m-s"! is composed of four flow regions from the column axis to the column wall; the central plume region, the fast bubble flow region, the vortical-spiral flow region and the descending flow region. Chen et al, (1994) have observed that in the fast bubble flow region, clusters of bubbles or coalesced bubbles move upwards in a spiral manner with high velocity, and found that these bubble streams isolate the central plume region from direct ‘mass exchange with the vortical-spiral flow region, and act as a rotating “solid” boundary with axial motion. Deckwer and Schumpe (1981) have proposed a graphical correlation of flow regimes with column diameterand Us. Another attempt has been made to determine the flow regime in bubble columns by using Uo Ws. £6 curve (Koide et al., 1984), igure 2 shows Eqs. (1) and (2) listed in Table 2 proposed by Marrucci (1965) and Koide et al. (1966), respectively, for ein a homogeneous flow regime, and Eq, (3) proposed by Akita and Yoshida (1973) forecin a heterogeneous flow regime for the air-water two- phase system. The region between the curves predi- cted by Eqs, (I) and (3) in Fig. 2 corresponds approximately to the transition regime. The vor- tical-spiral flow regime observed by Chen et al. (1994) might occur in the transition regime when the hole diameter 6 of the gas distributoris small. Koideer al. (1984) recommended that if D8>2x10~ m:, the flow regime is assumed to be a heterogeneous flow regime. In the bubble column with solid suspensions, solid particles tend to induce bubble coalescence, so the homogeneous flow regime is rarely observed, and ™ Fig. 1 Flow regimes in bubble column: (a) homogeneous flow regime, (b) transition regime, (c) vortical- spiral flow regime (Chem, eral, 1994), (d) heter- ‘geneous flow regime Ls Air-water om O thns tm 0327 worse 9) Qe AE GE Ist Te Koide et alta a0 0% 08 10 5 ON Px? ute To oe 20 j—lo outs 23 7 s0 ozais Lo 90 20 do eons tom 20 moms 23 N50 Cac i 0 ame) 08S Us tims 008 as 08 2. Flow regime and gas holdup in bubble column (Koide etal, 1984) the transition regime or the heterogeneous flow regime is usually observed. 1.2 Gas holdup correlations Equation (1) in Table 2is the correlation foregin the homogeneous flow regime, and Eq. (2) is the one for homogeneous flow and transition regimes, which is applicable to the homogeneous flow regime if Boy is very small. Equations (1) and (2) agree with each other very well. Krishna et al. (1994) have recom- mended use of the Richardson-Zaki type equation of ec for the homogeneous flow regime. Equations (3) ~(S) are the correlations for eg in the heterogeneous flow regime. Correlations for e¢ in the transition regime are proposed by Koide et al. (1984) and Tsuchiya and Nakanishi (1992), Addition of a surface active substance such as alcohol to water inhibits bubble coalescences, and JOURNAL OF CHEMICAL ENGINEERING OF JAPAN Table 2 Correlations of gas holdup Marrucei (1965) Uslva= (eg 268) o Koide eral, (1966) Us/va=(1+0.0167Bopy* "90.27 +0.71—ec)"]_ (2) ‘Akita and Yoshida (1973) 26|(1~ee)*= Ai Bo""Gal!"*Fr e A 20 for non-electrolyte soln, and Ai =0.25 for electrolyte soln Hikita er al. (1980) 4 =0.6T2Aa( Us| 04)" Mo* "pe puP (Ha AP o Ao= | for non-electrolyte soln, A2= 10°" for 0 1.0 kmobionm™ Hughmark (1967) eg 12+ G5/ Valu) ou) 72)}} [eg units] (3) ‘Schumpe and Deckwer (1987) 60.2080 GaP" FP o for heterogeneous flow regime. eo=(A(Uot Ui)/Ue+0.35/ Fr o An= Gn 1)/(+ 1+ 3.409290 for slug flow regime. Wilkinson et a, (1992) Vo] Uss. for Uo< Una ® 4 (Uren! Usa) + (Ua Urs)| Vir ° (Case/0u)=2.25 Mo™(Pr/ pa 10) (Winses/o)=(Wsats/ 01) + 24fste( Uo Vian)! 017 XMo™"(o1 oP” ay (Crm| Uss)= (Canon =0.Sexp-193p6-*1,%40)"") [st units} (12) Koide eral. (1984) to f(t 0)*= Ad Vous / an)" Moe X{1+4.356 95 P)/ oP REMY! (13) As=0.277 for water and ag. solns of glycerol and glycol, ‘and As=0.364 for ag. solns of inorganic electrolyte VOL 29 NO. 5 1996 lrogeneous regime Large bubble holdup ‘Smal bubble holdup Fig. 3. Two bubble-class model for gas holdup (Krishna etal, 1991) results in an increase of ¢¢. ‘The effects of alcohols on &q were discussed, and the correlations for e¢ were “obtained by Akita (1987) and Salvacion eal. (1995). Salvacion et al. introduced the parameter (Crok?/01) ‘of bubble coalescence proposed by Marrucci (1968). Addition of inorganic electolyte to water increases & by 20-30% in a bubble column with a perforated plate as a gas distributor (Koide er al., 1984), whereas Akita (1987a) has reported that no increase in e¢ is recognized when a perforeated plate of similar performance to that of a single nozzle is used. Orturk et al. (1987) measured e¢ in various organic liquids in a bubble column, and have reported that e¢ data, except those for mixed liquids with frothing ability, are described well by Eqs. (3) and (4). The correlations Eqs. (6) and (7) for ¢c in viscous media including non-Newtonian liquids were pro- posed by Schumpe and Deckwer (1987) Hikita er al, (1980) and Ozturk er al, (1987), in their éo experiments with various pc, and Idogawa et al, (1985a, b), in thier ec experiments at high pressure observed that z¢ increases with increasing gas density Pc Krishna et al. (1991) performed dynamic gas disengagement experiments, and from these results they have confirmed their earlier finding (Vermeer and Krishna, 1981) that in the heterogeneous bubble flow regime a bimodal bubble size distribution exisits: (1) a small-bubble swarm of da=5 mm and (2) a fast rising large-bubble swarm of ds=50 mm. Based on their ‘experimental results, they proposed the two bubble class model for éc shown in Fig. 3. Wilkinson et al. (1992) have proposed Eqs. (8)—(12) based on the approach proposed by Krishna et al. (1991) and by using éc data obtained at pressures between 0.1 and 2.0 MPa and extensive literature data, Addition of solid particles to liquid in a bubble column reduces é¢ and correlations of ec for heter- ogencous flow and transition regimes were proposed mT Table 3. List of numerical simulations of gas-liquid and gas-slurry flows Authors Drag Euler-Buler models Torvik er al. (1990); BCS uw» Svendsen er al, (1992); BC, AL u Ranade (1993); BC u Hilmer etal. (1994); BCS u Majumdar er al. (1995); BC u Euler-Lagrange models Sokolichin eral (1994); BC u Becker eva. (1994); BC, AL u Lapin etal. (1994); BC us 1) Added mass used instead of drag. by Koide er al. (1984), (Eq. (13)), Sauer and Hempel (1987), and Salvacion et al. (1995). 2. Hydrodynamics 2.1 Flow models In the heterogeneous flow regime, the liquid circulating flow shown in Fig. 1(4) is induced by uneven distribution of gas holdup. This flow is analyzed with the recirculating flow model by Miyauchi and Shyu (1970), Ueyama and Miyauchi (1979), Miyauchi et a. (1981) and Hills (1974, 1976), ‘The momentum equation of liquid flow was solved to give the radial liquid velocity distribution by assuming constant turbulent kinematic viscosity », and by using the radial gas holdup distribution predicted from empirical correlations. Here, vis a parameter for the calculated values ofthe liquid velocity tofit the observed value of the liquid velocity, and it is correlated with Uc and D as given by Eq. (14) (Miyauchi etal, 1981), 4 =0.160 Uel"@D*? [e.g.s. units) aa) ‘The other approach is to use Prandt!’s mixing length and to correlate 7 with experimental conditions. Gharant and Joshi (1992) assumed / and the radial e« distributions as follows, XD as) 6’ = colo’ + 2)/n"I ~ (r/ RY" (16) and proposed correlations of X and n’ for an air-water system with U;=0. x 102 Ug? phos an 11.01 Wes! D> (as) m8 Tnterfacial forces TI? Lift ‘AM? u - u = u u u u v u 2) Turbulence induced by bubbles 3) Used 4) Us; Slip velocity of bubbles is Kumar er al. (1994) deduced / from the Reynolds stresses and the liquid velocity gradients observed, however, they could not obtain a universal correlation of /as a function of D and Uc. Applications of Computational Fluid Dynamics (CFD) to gas-liquid (slurry) flow, mass transfer and reaction in bubble columns with and without solid suspensions have been done since the early 1990s. ‘There are two fluid models: One is the Euler-Euler ‘model (E-E model) where both liquid (sturry) and gas are treated as continuous phases, and the other is the Euler-Lagrange model (E-L model), where liquid (slurry) is treated as a continuous phase, and gas as a dispersed one. In the E-E model, the kc turbulence model is applied to the liquid phase, and as interface forces between gas and liquid, drag foree, lift force (Magnus force) and added mass force are considered. ‘Table 3 shows the models and interfacial forces used in various research works. In some works (Svendsen et ai. 1992, Majumdaret et al., 1995), the effects of turbulence induced by bubbles are considered. Results of gas holdup distributions and liquid velocit distributions calculated by the E-E models listed in Table 3 agree relatively well with those observed. However, as Sokolichin and Eigenberger (1994) have pointed out, the problems of the E-E model are that the sign of the Magnus force is changed for bubbles to move radially inwards, which is not justified, and some constants included in the equations of the interfacial forces can be adjusting parameters to fit the calculated values to those experimentally observed. Sokolichin and Figenberger (1994), Becker ea. (1994), and Lapin and Lubber (1994) used the E-L models listed in Table 3, where the drag force or the slip velocity of bubbles is used as the interfacial force, and only the laminar viscosity is used in the liqui phase, without using turbulent viscosity. Their results show that the flow patterns of liquid and bubbles are dynamic in nature, and the time averaged JOURNAL OF CHEMICAL ENGINEERING OF JAPAN ra U, {m/s} Fig. 4 Effect of gas velocity on £7 estimated from various correlations of Ez for air-water system in bubble column with D=0.6m Values of liquid velocity and gas holdup correspond to the familiar results that the liquid rises upwards and ¢¢ becomes larger in the center of the column, and the liquid goes downwards and ¢c becomes smaller near the wall. ‘The advantages of the E-L models are to use no lft force as an interfacial force, to consider no numerical diffusion into the dispersion phase (Sokolichin and Eigenberger, 1994), and the capa- bility of treating bubbles with a size distribution. ‘The disadvantages of the E-L models are the need for ‘more computational power in simulations than in those of the E-E models, as the trajectory of all bubbles with time must be stored in computer ‘memory, and no consideration of the effects of turbulence in the liquid phase. For future advances in these simulations, examinations of the interfacial forces, and further research of bubble coalescence and breakup to affect bubble size distributions are necessary. 2.2. Dispersion coefficients Millies and Mewes (1995a, b) have proposed a method to predict the flow field including several circulation cells, and clarified the relation between the circulation cells and the back mixing of liquid. To design a bubble column reactor with a one- dimensional dispersion mode! or by a cell model with back flow, it is necessary to estimate the values of dispersion coefficients of each phase in the column. 2.2.1 Liquid-phase_and solid-phase dispersion coefficients, Ey and Ep Correlations of E, in the heterogeneous fiow regime, Eqs. (19) - (23), are listed. in Table 4, and are compared in Fig. 4. Estimated values of Ez by Eqs. (19) and (20) agree well with those observed for D=0.3~0.6m (Koide, 1982). The above correlations are applied for a bubble column with Uz below about 0.03m-s'. When Uz is increased, E decreases, and Wachi etal. (1987) have proposed an equation for Ez based on the re-cirulating VOL 29 NO. 5 1996 ble 4 Correlations of E;, Eo, Epand vein bubble columns with and without solid suspen- Kato and Nishiwaki (1971) (WeD] Ei) = 13Fr/(1+6.SPA4) a) Hikita and Kikukawa (1975) [Eu/(gD)71Mo"™ =0.037-+0.188 FH 20) Miyauchi eral (1981) £,=[0.922-+ 1.080(1 — 0.054U¢!2)]Ug'!* D*? fogs. units} 1) Joshi (1980) E,=0.432D[gDUc— Eo" a)" @ Kantak er al. (1994) F,=0.2D"%(Ug/t) @) Oki and Inoue (1970) F,=0.300" Uo!?+ 1708, Exfem?-s], Dfem], Uofem-s""], [mm] (24) Kato and Nishiwaki (1972) UeD/EL= 13Fr/(1 + FPS) @5) For Rep=03-25, UcD/Er=[13Fr/(U+FP*IL+0.009Rep FF) (26) Kato eral. (1985) For Rep=2.5~640 UcD/Ep=[3Fr/U+ FPS +0023F-%) (27) ¥p= MLL + 1S(Ue/ Yn) P 62 28) Morooka eral (1986) Homogeneous flow regime, Spl %p=1+3.5e0Rep 0 ) Heterogencous flow regime, pl 1 WeoRes G0) Matsumoto er al. (1988) Ex {(gD3)!?=0.30(2/ Hp) "Ae Ui/ Ul ~e0)) XL@su— pe) psull" ee! —ea)) on Towell and Ackerman (1972) Ee=19.1UeD* 2 Field and Davidson (1980) Fo=S64D (Ul ec) 3) Kawagoe etal. (1989) Eq=0.66Eo) + 0.39Egs + 0.0078(UeHts/) G4) Eqy=26.XUa/ ta"! es) Eq2=19.(Uo/6)4D™ 6) ‘Wahi and Nojima (1990) Eq=(180/A)UcD??, Ai for water, en m9 ‘Table § Correlations of critical gas velocity required for complete solid suspension ‘Koide eral. (1983) for lat and conical bottom. (Weel %p)= 0801 (Os Pade Pd? Fry 9781 + 807 Mo ™}EL — 1. 20{1 —(Dy/ DP" Bo?) 8) Abraham er al. (1992) Uoc=0.54¥ A 68 654 DIM, estmm) 9 flow model by Miyauchi et al. (1981), which agrees well with observed values of Ez at U.=0 - 1.16 m-s"', The effect of Uc on E: in the homogeneous flow and transition regimes are very complicated, and no reliable correlation of E has been obtained. Kagoet al.(1989) have shown five patterns of log Uc vs. log Ex curves, where one is for the heterogeneous flow regime, and the other four are for the homogeneous flow and transition regimes. Equation (24) in Table 4is applied to the column with a gas distributor with 8551 mmand for Uo below Uonas Where the maximum, value of Ein the log Uc vs. log Ex curve is observed. Wilkinson er al. (1993) measured £; in a column of ‘D=0.158 m for the nitrogen-water system at pressures between 0.1 and 1.5 MPa, As the pressure increases, both cc and Ez increase, and the flow regime changes, from the heterogeneous flow regime to the transition one, They have shown that ¢x£:, observed at pres- sures between 0.1 - 1.5 MPa is correlated with Ucand proposed a method to estimate £ at high pressure, Yanget al, (1992) measured axial and radial eddy diffusivities by a Computer Automated Radioactive Particle Tracking (CARPT) technique, and have shown that the axial eddy diffusivities are much larger than the radial values, and differ from £; estimated from correlations, and suggested that a convection diffusion model which accounts for transport by both convection and turbulent dispersion would provide a better description of mixing in bubble columns. Correlations of £, Erand vp in bubble columns with solid suspensions are listed in Table 4 (Eqs. (25) - G1). Matsumoto et al. (1988) proposed a corre- lation of £z, Eq. (31), based on the turbulent mixing length model, which explained well the effect of Uz on E. 2.2.2 Gas-phase dispersion coefficient Eg Kawagoe ‘etal (1989) have proposed the two bubble-class model (TBCM) of gas-phase mixing where bubble swarms are assumed to be composed of two bubble groups, one in the central region and the other in the peripheral region of the bubble column, Based on. the residence time distributions (RTD) of the gas phase and the model, they correlated E¢ and axial and Ay= 1.114% 109%" for > 1.0 kmolion-m™, Onturk eral. (1987) (kad,?| Di) = 0.6280" Bop! Gagh™ Fri? (01) po) dy=0.003 m. (46) Suh era. (1991) (ka D?/ Dy)=0.018 52 BO ™ Ga FP (1 +0.129) «7 Merchuk and Ben-2vi (1992) kya= 14x 10-6" 8) Akita (1987) kyaD?/ Dy = ky Se!" Bot" Ga") 9) Wilkinson eta. (1994) (xa) / (kia) =Ueodyh Ea)", n= 1L0~ 12 (50) (8ap?Pp] 8)=8.8(Uo Hr) 91) MOE /PGP* (51) Akita and Yoshida (1974) (kis! Dr) =0.582*Gap'!*Bos* 2) (du[ D)=26B0-3Ga 2 Fe 3) aD=(1/3)BO™SGd" "eq!" (4) koa=2X10'D95UP™ —forsingle nozzle (55) koa=2.6X10.DUe™ for porous tube spargers 66) 752 ‘Akita (1987a) measured kya in inorganic aque- ‘ous solutions and proposed Eq, (49) in Table 6, kin Eq. (49) depends on concentrations of water, cation, and anion. Addition of surface-active substances such as alcohols to water increases the &<, however, values of kxa in aqueous solutions of alcohols become larger or smaller than those in water according to the kind and concentration of the alcohol (salvacion et a., 1995). Akita (1987) and Salvacion et al. (1995) proposed correlations of kza in alcohol solutions, Concerning the effect of high pressure on kia Wilkinson et al, (1994) have shown that cc, ka and a increase with pressure, and kya is correlated well with 2, and they proposed Eq. (50) for design purposes. ‘The above cited correlations of kya are mostly applied to estimate Kua in the heterogeneous flow regime. ‘The estimation of ka in the transition regime can be done by estimating ¢« in the transition regime from Koideet al's correlation 1984), and by calculating kya from Eq. (60) in Table 7 with the estimated value of ec. Grund et al. (1992) measurd the gas holdup of small bubble-classes and large bubble classes by a gas disengagement technique, and also measured kya in bubble columns with water and organic liquids. ‘They applied the two bubble class model to the bubble column to analyze the experimental results of kua, and have shown that the contribution of small class bubbles to kza is very large, e.g, about 68% at Us 0.15 m-s" in an air-water system. Muller and Davidson (1992) have shown that small-class bubbles contribute 20-50% of the gas- liquid mass transfer in a column with highly viscous liquid. Grund er al. (1992), in their conclusions, have suggested that a rigorous reactor model should consider two bubble-classes with different degrees of depletion of transport component in the gas phase. 3.1.2 Bubble size Bubble diameters have been mea- sured by photographic methods, the electro-resistivity| ‘method, the optical-fiber method and the chemical absorption method. Recently, Jiang et al. (1995) applied the Particle Image Velocimetry (PIV) tech- nique to obtain bubble properties such as size and shape in a bubble column operated at high pressures. In the homogeneous flow regime where no bubble coalescence and breakup occur, bubble diam- eters can be estimated by the existing correlations of ds of bubbles generated from perforated plates (Tadaki and Maeda, 1963; Koide et al., 1966; Miyahara and Hayashino, 1995) or porous plates (Hayashi et al, 1975). In the transition regime and the heterogeneous flow regime, where bubble coalescence and breakup occur, observed bubble diameters show different values according to the measuring methods. Figure 7 shows a comparison of dys measured in an air-water system with those estimated by the correlations of JOURNAL OF CHEMICAL ENGINEERING OF JAPAN Table 7 Correlations of kya, kr, ks; kod and bubble diameters in bubble columns with solid suspensions Koide era. (1984) (k00;,/e,Dig)= 2.11829 Mor®!egh* [LE LAT 10 G98 Fr 80-8 Re-OT (60) Yasunishi eta. (1986) 3.09 10-1 = 45/0.6(1 — e/a}! Ue kyals, uefPars), Uofem-s-"] (61) Salvacion eral. (1995) (40, /LD1g)= 12.9824 Mo Bo“ 1 {0.47 +0.53exp[—41.4(k,/spUs) Res!) X (140.6265)! @) Fukuma eral, (19874) dys=0.59(Valte)/8 (3) v= Jol te) Usto(\~ te) «) Fukuma eral (19876) kydys| Di=4SX 10*S25G@ Bo? 665) Sanger and Deckwer ra. (1981) (edy4/PE)<1, Shs=2+2.067Se"epde/r2"™ (66) (egdes/2)> 1, Shs=2+0.6498e!eydet/r 2 (67) Sano eal. (1974) Shs= [2+ 04Se%egdyt/¥ 2)" (68) Sada etal. (1985) kea=170U Kealmol-MPa!+m-s] (69) bubble diameter: Eqs. (43), (51), (53) and (63). dos ‘measured near the column wall by the photographic method (Ueyama et al, 1980) agree with predicted values from Eq. (53) in Table 6, however, they are much smaller than those measured with the electro- resistivity method and averaged over the cross-section bby Ueyama er al. (1980). When a bubble column is operated at high pressures, the bubble breakup is accelerated due to increasing gas density (Wilkinson et al. 1990), and so bubble sizes decrease (Idogawa et al., 1985a, bs Wilkinson et al., 1994). Jiang etal. (1995) measured bubble sizes by the PIV technique in a bubble column VOL 29 NO. 5 1996 ere a 2 a eat vo a TE eee ale Se Cea ata (3) ys im wee 16 Ug trn/s} Fig. 7 Effect of gus velocity on bubble diameters. MN; ‘multi nozzles, SN; single nozzle, Photo; Photo- ‘graphic method, ER; electro-resistivity method operated at pressures up to 21 MPa, and have shown that the bubble size decreases and the bubble size distribution narrows with increasing pressure, how- ever the pressure effect on the bubble size is not significant when the pressure is higher than 1.5 MPa. Wilkinson et al (1994) proposed the correlation Eq. (51) of dw based on data obtained by the photographic method in a bubble column operated between 0.11.5 MPa, and with water and organic liquid. Figure 7 shows d,,, calculated from Eq. (51) for 0.1 MPa, which agrees well to that observed by Ueyama et al (1980). 3.1.3 Liquid-phase mass transfer coefficient ky kx values in a bubble column are obtained either by measuring kya, ec and di, or by measuring kya and a with the chemical absorption method. Because of the difficulty in measuring distribution and the averaged value of bubble diameters in a bubble column, predicted values of k by existing correlations ofkcdiffer. Figure 8 compares k, observed in a COs- water system with those predicted by correlations Eqs. (42), (52) and (65). From these results, more kz data based on accurate data of di, are expected, 3.1.4 Gas-phase_mass transfer Only a few works have been done on koa. To examine the effect of diffusivity on gas-phase mass transfer, the ‘experiments of chemical absorption and vaporization were carried out by Metha and Sharma (1966). Based on experimental observation, they have shown the following relation, koa Do"? Uc Hi Botton et al. (1980) measured koa by the chemical absorption method in an SO: (in ait)-NasCO; aqueous solntion system in a wide range of Ucup to about 4 m: s'!,and they showed that ka varies in a ratio of Ua?” in the range of 0.01&Ue0.3 m:s', and remains almost constant in the range of 0.3 10 nm to liquid increases bubble coalescences and da, and hence decreases both é and kya as shown in Fig. 6. For these cases, Koide et al. (1984) and Yasunishiee al. (1986) proposed correlations of ku, Eqs. (60) and (61) respectively, for particles of pp2=2500kg-m”, The effect of particles on decreasing kya is more pro- nounced in Eq, (60) than in Eq. (61), as Eq. (60) based oon data observed in bubble columns in a batch-wise operation of liquid and particles. Sauer and Hempel (1987) proposed correlations of kua for bubble col- tumns with suspended particles of pp=1020 — 2780 ke oc Sada et al. (1986, 1987) and Schumpe er al (19874) showed that both gq and kya increased at a small loading of very fine particles with d<10 um. Sada eral. (1986) explained this phenomenon was due to bubble coalescences hindered by fine particles in the liquid film layer around the bubbles. Sada et al. 134 (1986) and Schumpe er al. (1987a) proposed correlations of kxa in bubble columns with solid particles of dy<10 pm. Ina bubble column with fairly nonwettable solid particles, kya is severerly reduced (Schumpe et ai, 1987b, Godbol er al. 1990), as particle agglomeration at the interface reduces both the gas-liquid interfacial area and kxa (Godbol et a., 1990). Sun and Furusaki (1989) have shown that when gel particles are used, the intraparticle diffusion of dissolved gas in gel particles has a large effect on the estimated value of ka, and they proposed a method to estimate kya. Sun and Frusaki (1989) and Salvacion| eral. (1995) showed that kya decreases with increasing solid concentration in gel-particle suspended bubble columns. Salvacion er al. (1995) showed that ad- ition of alcohol to water increases or decreases kia depending on the kind and concentration of the alcohol added to the water, and proposed a corre- lation Eq. (62) of kra including a parameter of retardation of surface flow on bubbles by the alcohol. 3.2.2 Bubble size Addition of solid particles to liquid increases bubble coalescences and so bubble size. Fukuma et al, (1987a) measured bubble sizes and rising velocities using an electro-resistivity probe, ‘and showed that the mean bubble size becomes largest ‘ata particle diameter of about 0.2 mm for an air-water system, Based on these observation they proposed a correlation, Eq. (63) of dus, which is shown in Fig, 7. 3.2.3 Liquid-phase mass transfer coefficient ky and liquid-solid_mass transfer coefficient k, Fukuma ‘ef al. (19875) evaluated the values of k, from dividing ca in their previous paper (Yasunishi et al., 1986) by 4a (=6ec/du)._ They have shown that the degrees of dependence of kon both da, and the liquid viscosity are larger than those in a bubble column, which is indicated in Eq. (52), and they proposed Eq. (65) for ky. Schumpe er al. (1987a) have shown that low concentrations of high density solids of dp<10 um increase kz by a hydrodynamiceffect on the liquid film around the bubbles. From measurements of solid-liquid mass trans- fer in bubble columns, Sanger and Deckwer (1981) hhave shown that A; increases with increasing Uc, however, it reaches a limiting value at a gas velocity which roughly agrees with the transition from the homogeneous flow to the heterogeneous one, and ky decreases with increasing dp and liquid viscosity. Based on these observations they proposed the correlations Eqs. (66) and (67) of ks, which are similar and agree to Eq. (68) proposed by Sano et al. (1974). 3.2.4 Gas-phase mass transfer Sada et al. (1985) measured koa by using chemical adsorption of lean CO» into NaOH aqueons solutions with suspended Ca(OH) particles, and proposed the correlation, Eq. (69) of kca. The predicted values of kea from Eq. (69) agree well with those observed by Metha and JOURNAL OF CHEMICAL ENGINEERING OF JAPAN ‘Table 8 Correlations of heat transfer coefficient Nishikawa eral. (1977) SEPPML04 (r= Po) CREFPY" w/w Fo. Ud) 0) Vg<1000 m/h, Ui=S4 m/h, 0.054 U¢!!* Ue<1000 m/h, $4 Ur 500 m/h, F=0.054 Ue!(Ui/54)! Ue<1000 m/h, Ur=54 m/h, F=0.3 Deckwer (1980) S1=0.1[ReFAPPP o Deckwer and Schumpe (1980) Slurry bubble column; Eq. (71) with Psi=s05+¢r0r, si = HU +4505), Cysr= dseps-+ bépz and krsi= kril2kra + krs~ 28s (kerr ~ kro] X kre hrs + ostkra— kr" i) Sharma (1966) and Botton et al. (1980) in a bubble column, 4. Heat Transfer in Bubble Columns with and without Solid Suspension Kumar and Fan (1994) carried out local heat transfer measurements in bubble columns and three- phase fludized beds with viscous Newtonian liquids, and showed that the increased transfer is mainly dueto increased bubble velocity caused by the increased bubble-wake interactions. The liquid-phase heat transfer coefficients hz at ‘the walls of the jacket and coil increase with increasing ‘gas velocity, however, in the range of U¢>0.28 m:s', hh, showed a constant value (Nishikawa et al., 1977). The correlations of hz by Nishikawa er al. (1977) and Deckwer (1980) are shown in Table 8, To estimate the slurry-phase heat transfer coefficient hs, Deckwer and Schumpe (1980) proposed that hz iscorrelated by Eq. (71)if the properties of the slurry shown in Eq. (72) in Table 8 are used. Research on fy. and hs in baffled slurry bubble ‘columns is summarized in the review by Saxena and ‘Chen (1994). Reactor Models ‘The axial dispersion model (ADM), the cell ‘model with back flow (CMBF) and other simpler models have been used as reactor models. Deckwer VOL 29 NO. 5 1996 (1992) and Ueyama (1993) discussed the characteris- tics of both models and their aplications. Wachi and Morikawa (1987) investigated chlo rination of ethylene in a boiling bubble column re- actor, and applied CMBF to predict axial distri- butions of e¢ and temperature, and the conversion of, chlorine. The agreements between experimental and predicted results were fairly good. Torvie and Svendsen (1990) applied the Euler- Euler model mentioned in section 2.1 to a slurry reactor to estimate the production of methanol from synthesis gas. They compared the results of this simulation with data and ADM analysis of Ozturk et al (1988), and presented the following results: 1) Their model gives about the same trend of the axial distribution of conversion as ADM, however the axial dispersion is not constant through the column, but high atthe bottom, 2) The effect of column diameter D on decreasing the conversion with increasing D is not so pronounced as predicted from ADM. 3) The radial conversion profiles show that conversion is highest close to the wall. This is due to the gas phase retention time being higher in this part due to back flow of both gas and slurry phases along the walls. Conelusion For a while, the design of a bubble column reactor might be done by using a one-dimensional model (ADM, CMBF) or other simpler models, but in the future, it may be possible to design the reactor with the aid of CFD. For future advances of the application of CFD to bubble columns, accurate data of bubble size distribution and hydrodynamics in bubble columns, and further research on the mechanism of bubble coalescence and breakup, and on mass transfer from individual bubbles are necessary. Nomenclature 4 Hamaker constant uo a pectic gas-liquid interfacial area based on ‘erated liquid or slurry volume tw) ’ |= specific gas-liquid interacial area based on Sate liquid or surry volume [im Bo Dp, {o, Bond number a Bos gdp, |. Bond number a Bow = gdepy/oy, Bond number i) c (ex) RTYdog| de + (inf fAlned 1. (+ Gam/en ™ = parametr of bubble coalescence proposed by Marrueci (1969) Q heat eapacity| Uke stale +), average solid concentrarion in taste slurry kg) ene = concentration of components I and 2in liquid [mol-m?} D = column diameter Te] De diameter of gas distributor f=) Do, De = Molecular difusvity in gas and liquid, respectively Its] 755 Fra Res bubble diameter (= mean diameter of particles tm volume mean diameter of bubbles (os) volume-surface mean diameter of bubbles [mi] axial dispersion coefficient [mer] Ug, energy dissipation rate per unit mass To Ua}igb)!?, Froude number vale)". Froude numbee Uclteds)"* Froude number activity coefcent of component in guid Door gD", Gallet number ‘tds! Galilei number aravitational acceleration im Hency’s law constant static gud or sury height level of arated liquid or slurry during action tm) deat transfer coetiient [Wem] ‘onic strength of cectroyte sottion {kmolion-m?] fluid consistency index Pas] (220 J4r9)" [o'} liquid-phase mass transfer coeficient —_[ms"] volumetric liquid-phase mass transfer coefficient based on arated liquid or slurry volume fs") ‘volumetric iquid-phase mass transfer coetTicient based on static liquid or slurry volume (5"] thermal conductivity [WemK-) ~(dor{deiX3Usre/2Du)"/raRT il ining length (a ‘u/c, Morton number at ‘number of nozzle or holes in gas dstebutor [—] fist normal sess difference (Pa flow behavior index ial parameter defined by Ea. (16) a pitch of holes in gas distor ty acyl, Prandtl number tl fas constant U-K mot DUciry. Reynolds number ty dlls/ny, Reynolds number i dwn, Reynolds number a radial distance te] bub radius tm) [Dio tag) Dv, Schmidt number [=] lou We, Stanton number M1 temperature KI time tl locity based on cross section tos] efitical gas velocity required for complete suspension of particles fms" ‘sing velocity of large bubbles [ms] setting velocity of particles [ms] slp velocity of bubble swarms fms" sing velocity of small bubbles [ms] Ue at flow regime transition [ms] drift fux of gas (ms!) settling velocity of particles fms] terminal velocity of single bubble [ms] terminal velocity of asinge particle [ms] molar volume of components Land 2 liquid [im -mot v/s, Weissenberg number i parameter defined by Eq. 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