02638762/02/$10.00+0.

00 # Institution of Chemical Engineers Trans IChemE, Vol 80, Part A, April 2002

HEAT TRANSFER COEFFICIENT PREDICTION FOR FALLING FILM EVAPORATION USED FOR SOLVENT REMOVAL FROM HIGHLY VISCOUS LIQUIDS
V. V. WADEKAR
HTFS, AEA Technology-Hyprotech, Harwell, Oxfordshire, UK.

he paper deals with the mixture effect correction for falling lm evaporation of solutions containing dissolved solids. It is shown that the correction arises from vapour-liquid equilibrium effects similar to those observed for boiling of multicomponent liquid mixtures. The predictive method reported here uses the HTFS correlation1 to obtain the heat transfer coef cient for the highly viscous equivalent pure uid, and then applies a mixture effect correction to it. Data for falling lm evaporation from aqueous solutions of polyethylene glycol are predicted reasonably well by the method. Keywords: falling lm evaporation; high viscosity liquids; solvent removal; mixture effect; mass transfer.

INTRODUCTION Falling lm evaporators are often used for removing water or organic solvents from solutions containing dissolved solids. During such a process only solvent is vaporized at the vapour-liquid interface; the dissolved solids, being nonvolatile, remain in the solution. Invariably these solutions also have very high viscosities. The evaporative process is, thus, characterized by high viscosity as well as the mixture effect arising from the loss of the volatile component, i.e. the solvent. This paper attempts to address the effect of vapour-liquid equilibrium and mass transfer due to vaporization of solvent at the vapour-liquid interface. These effects, collectively known as the mixture effect, are examined rst for boiling of multicomponent liquid mixtures and then extended to solutions containing dissolved solids. Predictions of heat transfer coef cient are then obtained by applying the mixture effect correction to the HTFS correlation for falling lm evaporation of a single component liquid. This correlation is applicable to uids of a wide range of viscosities including ultra high viscosities1. Finally, the predictions are compared with the measured data reported by Tuzla et al. for solvent removal from highly viscous liquid lms2. MIXTURE EFFECT IN BOILING For a non-azeotropic mixture the equilibrium compositions of the vapour and liquid phases are different. During a phase change process, such as boiling or evaporation, this causes concentration gradients, and therefore, diffusional mass transfer near the vapour-liquid interface. These effects, 267

which cause degradation in boiling heat transfer, are collectively called the mixture effect, and are documented fairly well in the published literature for binary liquid mixtures, for example references 3 and 4. The concept of the mixture effect can be explained as follows. During vaporization of a multicomponent liquid mixture there is a preferential loss of the light component from the liquid phase. This leaves the liquid at the vapour-liquid interface depleted in the light component, creating concentration gradients in the vicinity of the interface. This has two effects. Firstly, the concentration gradients trigger the process of counter-diffusion of the light and heavy components to minimize the depletion of the light component at the interface. Secondly, the depletion of the light component causes a rise in the bubble point temperature at the interface. The rise in the interface bubble point temperature, shown schematically in Figure 1, leads to a reduction in the available wall superheat, which in turn results in a lower boiling heat transfer coef cient de ned in terms of the equilibrium bubble point temperature. In the subsequent discussion, the similarity between the mixture effect for a binary liquid mixture and a solution containing dissolved solids is examined. On establishing the similarity, the model for handling the mixture effect for a binary liquid mixture is described. The model is then modi ed to deal with solutions containing dissolved solids. Similarity Between a Solution and a Binary Liquid Mixture As discussed above, the underlying cause of the mixture effect for a multicomponent liquid mixture is the preferential

268

WADEKAR Schlunder4 carried out important work in applying the theory of multicomponent boiling. He analysed the mixture effect for nucleate boiling by applying the lm theory model around the growing vapour bubbles. This can be used to obtain the rise in the interfacial temperature, DTm used in equation (2). However, Schlunders use of the Stefan Maxwell equations in obtaining the derivations conceals the physical processes and makes it dif cult to relate the derivation to the underlying physical model. In order to address this problem, the governing equations for the mixture effect were derived by considering the physical process of diffusion using the lm theory model5. According to this derivation, if the areas of heat and mass transfer are equal, the interface compositions xi and y* are related to i the bulk liquid phase composition xb by the following equation: _ where, y = q=Dhv rl bl Note that the interface compositions xi and y* are related i to each other through the vapour-liquid equilibrium relationship. Equation (3), can thus, be solved using the vapourliquid equilibrium data. From values of xb and xi the corresponding bubble point temperatures can be obtained to calculate DTm from equation (1). Equation (3) can be modi ed to the following form to take into account the effect of rate of mass transfer on the mass transfer coef cient as documented by Bird et al.6. (xb xi ) = ey 1 (y xb ) (4) i Note that equation (4) is identical to the equation derived by Schlunder4, using the Stefan-Maxwell equations. Schlunders original approach was proposed for nucleate boiling heat transfer. A similar approach was later suggested for the two-phase convective component of ow boiling heat transfer5. It now appears that the approach works for the convective heat transfer component if the vapour-liquid interface is relatively well de ned and quiescent, which is the case for falling lm evaporation involving highly viscous liquid lms. It is worth noting that in falling lm evaporation, where the liquid phase ows as annular lm, the assumption of near equality of areas for heat and interfacial mass transfer is more likely to be valid. Extension of the Model to Solutions Containing Dissolved Solids The basic theory underlying equation (4) in the above model for a binary mixture can easily be extended to a solution containing dissolved solids. As noted earlier the vapour generated from such a solution contains only the solvent vapour, i.e. y* = 1. With this information and on i some rearrangement, equation (4) becomes: xi = 1 ey (1 xb ) (5) (xb xi ) = y(y xb ) i (3)

Figure 1. Reduction of wall superheat from (Tw 7 Tbub(xb)) to (Tw 7 Tbub(xi)) due to mixture effect.

loss of the light component from the liquid phase. In this respect, solutions containing dissolved solids are similar to binary liquid mixtures, representing only a limiting case where the light component, i.e., the solvent is vaporized and not the solute. The loss of solvent will cause a rise in the interfacial solute concentration and trigger the diffusional mass transfer of solvent molecules through the solute rich layer close to the interface. A direct consequence of the rise in the interfacial solute concentration is the rise in the saturation or bubble point temperature at the interface. This rise in the interfacial temperature will have a similar impact on the heat transfer coef cient as in the case of a binary liquid mixture. It should be noted at this point that the equations developed by various researchers3,4 for boiling of multicomponent liquid mixtures, could not be applied directly to solutions containing dissolved solids. In order to apply these equations knowledge of phase equilibrium data, encapsulated in a classical vapour-liquid equilibrium diagram consisting of bubble point and dew point is required. For solutions containing dissolved solids there exists only a saturation temperature curve, corresponding to the bubble temperature curve, and no dew point curve. This particular dif culty could be one of the reasons why the standard mixture correction approach has so far not been attempted for evaporation or boiling of solutions. In order to develop a methodology for solutions, the basic equations used for derivation of the mixture effect correction need to be examined and appropriately modi ed. This task is performed in the following section. Model for Binary Liquid Mixtures Figure 1 illustrates the model for a binary mixture . The rise in the interfacial temperature, DTm, responsible for the degradation in boiling heat transfer, is given by: DTm = (Tbub(xi ) T(xb ) ) (1)
5

If the heat ux is known, the degradation in boiling heat transfer coef cient can be allowed for by expressing the mixture heat transfer coef cient, am, as: 1 1 DTm = + am aepf q _ (2)

In equation (2), aepf is the heat transfer coef cient for the equivalent pure uid i.e. an hypothetical uid with the same physical properties as that of the mixture but without any mixture effect.

Instead of using the normal bubble point curve, a saturation temperature against the solute concentration curve is used to convert the concentrations xb and xi to the corresponding saturation temperatures. Subsequent use of equations (1) and (2) in the overall model remains unaltered. It should be noted that equation (5) would also be applicable to solutions of liquids where one liquid has an extremely low volatility. It Trans IChemE, Vol 80, Part A, April 2002

HEAT TRANSFER COEFFICIENT PREDICTION would be possible to derive equation (5) directly from the lm theory but the derivation shown here links it to the standard treatment of the mixture effect theory for binary mixtures of miscible liquids, typi ed in equations (3) and (4). FALLING FILM DATA FOR SOLVENT REMOVAL In the open literature only a limited amount of information is available on falling lm evaporation used for the solvent removal process. The reason for the paucity of information is that such a process usually needs to handle highly viscous liquid lms under high vacuum. Recently, Tuzla et al.2 conducted a systematic series of experiments in this dif cult area, and reported valuable data for aqueous solutions of Poly Ethylene Glycol (PEG) at varying concentrations. Although the PEG solutions are liquid at the test temperatures, the PEG itself is solid at ambient temperatures. These PEG solutions are excellent modelling uids for the process of solvent removal from highly viscous liquid lms. The relationship between the saturation temperature for the PEG solutions and the PEG weight fraction is shown in Figure 2 for two typical pressures used in the experimentation2. Note that the relationship is relatively at at low PEG concentrations and it becomes increasingly steep as the PEG concentration increases. Due to the relatively at nature of the saturation temperature pro le at low concentrations, the measured data at 0.5 PEG weight fraction showed very little or no mixture effect. HEAT TRANSFER PREDICTIONS FOR PEG SOLUTIONS In order to calculate the predicted heat transfer coef cient for PEG solutions, an equivalent pure uid coef cient is required. The HTFS correlation for single component uid was used for this purpose. It was shown1 that the correlation works well over a wide range of liquid viscosities, predicting the data of Alhusseini et al.7 for single component uids within a mean error of less than 6%. The equivalent pure uid heat transfer coef cients, aepf, obtained from the HTFS correlation are corrected for the mixture effect using equations (2) and (5). In order to calculate the parameter, y, used in equation (5), the mass transfer coef cient, b, for diffusion of water in aqueous PEG solutions is required. As no information is available in the

269

literature, suitable values of mass transfer coef cient needed to be assumed. In his work, Schlunder assumed a constant value of 0.0002 m s1 for the mass transfer coef cient. In the present work it was thought more appropriate that the coef cient should be a function of the lm Reynolds number. The following dimensional equation for the mass transfer coef cient, b, was found to provide a best- t to the data: b = 2 106 Re0:8 (6)

It is recognized that further work may be required to incorporate the Schmidt number effect in this equation. Note that the mass transfer coef cients calculated with equation (6) are somewhat lower than the typical values used in the gas absorption process. DATA AND PREDICTIONS The predicted heat transfer coef cients for aqueous PEG solutions are compared with the measured data of Tuzla et al. in Figures 3 to 7. The ratio of the predicted to measured heat transfer is used in Figures 3 to 6. The ratio is plotted against the lm

Figure 3. Coef cient ratio against lm Reynolds number for 0.65 weight fraction PEG.

Figure 2. Saturation temperature data for aqueous PEG solutions at two test pressures2.

Figure 4. Coef cient ratio against lm Reynolds number for 0.69 weight fraction PEG.

Trans IChemE, Vol 80, Part A, April 2002

270

WADEKAR Reynolds number in Figures 3 and 4 at PEG weight fractions of 0.65 and 0.69; similar graphs are presented in Figures 5 and 6 using heat ux as abscissa. Two sets of the ratio were obtained by calculating the predicted heat transfer coef cient with and without the mixture effect correction. These two sets are shown as hollow and solid circles with two respective best- t lines in Figures 3 to 6. The dotted line is best- t line for ratios without mixture effect and the solid line with mixture effect. It can be seen from these gures that in general the ratios based on the mixture effect correction are closer to the unity ratio line than those without. Figures 3 and 4 suggest that there may be a parametric trend of decreasing mixture effect with increasing Reynolds number. The likely cause for this is the onset of wavy laminar region with increasing Reynolds number, with a consequent decrease in the mass transfer resistance. Figures 5 and 6 indicate a similar trend with respect to heat ux. It should be noted that when the HTFS single component correlation is applied to the single component data such a trend is not exhibited. A possible explanation for this trend with mixtures is the decrease of the mixture effect as a result of increased rate of evaporation with increasing heat ux. However, not much should be read in these parametric trends. The data used to decide the parametric trend of a given variable should be obtained by holding all other relevant variables constant. For example, to obtain the trend for the mixture effect with respect to the lm Reynolds number, other variables such as heat ux, pressure etc must be held constant. However, the available data were too limited to extract such subsets required for the parametric analysis. It can be seen from Table 1 that for a total of 188 data points the average deviation of errors is 0.76% and the mean deviation of errors about 8.4%. The breakdown of errors at three individual concentrations also appears promising. Without the mixture effect correction, the data at PEG weight fractions of 0.65 and 0.69 were overpredicted by about 16% to 17%. It is worth noting that at the PEG weight fraction of 0.5, the data are well predicted without the mixture effect correction. Equally reassuring is the fact that, even with the mixture effect correction, the data are well predicted. This implies that the predicted mixture effect correction at this composition is in line with the observation of very little or no mixture effect for these data. The data shown in Table 1 are plotted in Figure 7 as a graph of the predicted against measured heat transfer coef cients. Figure 7 shows that the predictions are in good agreement with the measured data. This con rms that both the equivalent pure uid coef cient and the mixture effect correction are predicted well.
Table 1. Summary of the predictions. PEG weight fraction 0.501 0.651 0.690 All data No of data points 39 118 31 188 Average Error % 1.51 1.08 2.82 0.76 Mean Error % 7.26 8.53 9.82 8.43

Figure 5. Coef cient ratio against heat ux for 0.65 weight fraction PEG.

Figure 6. Coef cient ratio against heat ux for 0.69 weight fraction PEG.

Figure 7. Comparison of predicted and measured data at three different PEG concentrations.

1 P haExp aCalc i 100 aExp n n h i 1 P ABS(aExp aCalc ) %Mean Error = 100 aExp n n %Average Error =

Trans IChemE, Vol 80, Part A, April 2002

HEAT TRANSFER COEFFICIENT PREDICTION CONCLUSIONS The mixture effect, which occurs during evaporation of solvent from falling lms of highly viscous solutions, is similar to that observed for boiling of multicomponent liquid mixtures. The HTFS correlation for falling lm evaporation of highly viscous single component uids appears to provide a correct basis for the predictive method for viscous solutions. Finally, the predictive method itself appears to be successful in predicting the data of Tuzla et al.2 for highly viscous aqueous solutions of PEG. NOMENCLATURE
q _ T x y* heat ux, W m 2 temperature, K liquid composition equilibrium vapour composition

271

REFERENCES
1. Wadekar, V V 2000, Heat transfer to falling liquid lms with high . ., Prandtl numbers, Proc 3rd Euro Thermal Sci Conf, 2: 851856. 2. Tuzla, K., Palmer, T. R. and Chen, J. C., 2000, Experimental study of heat transfer in laminar falling lms at high Prandtl numbers, Proc Boiling 2000, 1: 4165. 3. Calus, W. F. and Rice, P., 1972, Pool boilingBinary liquid mixtures, Chem Eng Sci, 27: 16871697. 4. Schlunder, E. U., 1983, Heat transfer in nucleate boiling of mixtures, Int Chem Eng, 23(4): 589599. 5. Wadekar, V. V 1994, Convective heat transfer to binary mixtures in ., annular two phase ow, Proc 10th Int Heat Trans Conf, 7: 557562. 6. Bird, R. B., Stewart, W. E. and Lightfoot, E. N., 1960, Transport Phenomena (John Wiley and Sons, USA), p 663. 7. Alhusseini, A., Tuzla, K. and Chen, J. C., 1998, Falling lm evaporation of single component liquids, Int J Heat Mass Trans, 41(12): 16231632.

ACKNOWLEDGEMENTS
The work was carried out under the research programme of the Heat Transfer and Fluid Flow Service (HTFS). Permission given by HTFS to publish this paper is gratefully acknowledged.

Greek symbols a heat transfer coef cient, W m 2 K 1 b mass transfer coef cient, m s 1 Dhv molar latent heat of vaporization, J kg mole 1 r molar density, kg mole=m 3 y parameter given in equation (3) Subscript b bub Calc epf Exp i l m bulk bubble point calculated equivalent pure uid experimental interface liquid with mixture effect

ADDRESS
Correspondence concerning this paper should be addressed to Dr. V V Wadekar, HTFS AEA Technology-Hyprotech, Gemini Building, . . Fermi Avenue, Harwell, OX11 0QR, UK. E-mail: Vishwas.Wadekar@hyprotech.com The manuscript was received 19 November 2001 and accepted for publication after revision 12 December 2001.

Trans IChemE, Vol 80, Part A, April 2002