Proceedings of ITP2009 Interdisciplinary Transport Phenomena VI: Fluid, Thermal, Biological, Materials and Space Sciences October 4-9,

2009, Volterra, Italy

ITP-09-09
NUCLEATE BOILING HEAT TRANSFER IN ALCOHOL AQUEOUS SOLUTIONS
Takashi Sakai Department of Aeronautics and Astronautics, Kyushu University, Japan (JSPS Research Fellow DC) Shinsaku Yoshii Department of Aeronautics and Astronautics, Kyushu University, Japan Yasuhisa Shinmoto Department of Aeronautics and Astronautics, Kyushu University, Japan ABSTRACT Saturated pool boiling experiments were conducted by using alcohol aqueous solutions, i.e. 1-Propanol/Water, 2Propanol/Water and Water/Ethylene glycol mixtures at 0.1MPa. The heating surface is a horizontal upward-facing circular flat plate of 40mm in diameter. The increase in the heat transfer coefficients was observed for 1-Propanol/Water and 2-Propaonl/Water mixtures at very low alcohol concentration range, where Marangoni convection towards the three-phase interline is induced by the surface tension gradient along the vapor-liquid interface due to preferential evaporation of alcohol component. The heat transfer enhancement due to Marangoni effect seems to overcome the heat transfer deterioration due to mass transfer resistance. In the moderate concentration range, however, the heat transfer enhancement was turned to the heat transfer deterioration with increasing in the alcohol concentration. For Water/Ethylene glycol mixture, on the contrary, no significant increase and decrease in the heat transfer coefficients was observed in the entire concentration range tested. On the other hand, the critical heat flux was markedly decreased in the low alcohol concentration range of 1-Propanol/Water and 2-Propanol/Water mixtures. Marangoni effect is also suggested as a possible reason for the peculiar trend of the critical heat flux. Marangoni effect seems to promote the extension of drypatches underneath coalesced bubbles and the critical heat flux becomes decreased. Yuuki Tsukinari Department of Aeronautics and Astronautics, Kyushu University, Japan Kazutoshi Kajimoto Department of Aeronautics and Astronautics, Kyushu University, Japan Haruhiko Ohta Department of Aeronautics and Astronautics, Kyushu University, Japan

NOMENCLATURE D mass diffusion coefficient g gravity acceleration La Laplace constant Ma Marangoni number P pressure q heat flux T temperature wx weight fraction of liquid wy weight fraction of vapor x mole fraction of liquid y mole fraction of vapor Greek symbols heat transfer coefficient viscosity density surface tension Subscripts 1 low-boiling component or more volatile component 2 high-boiling component or less volatile component CHF critical heat flux g gas l liquid m mixture sat saturation

Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009

Paper No: ITP-09-09

1. INTRODUCTION Nucleate boiling heat transfer is one of the most effective means for the heat removal from thermal devices because of its high performance of heat transfer and heat transportation. For this reason, boiling heat transfer and critical heat flux (CHF) of several single components and mixtures have been studied by many investigators. In nucleate boiling of binary mixtures, mass transfer resistance causes the variation of liquid concentration and its saturation temperature underneath bubbles along a vaporliquid phase equilibrium diagram. Thus Marangoni force is induced along the vapor-liquid interface by the surface tension gradient due to the variation of concentration and temperature. The Marangoni force induces the flow whose direction is determined by the sign of surface tension gradient along the interface. When the surface tension of mixture increases with decreasing the concentration of more volatile component (positive mixtures), Marangoni force is expected to induce the flow which supplies liquid towards the three-phase interline and prevents the extension of drypatch and the heat transfer enhancement is expected. On the other hand, when the surface tension of mixture decreases with decreasing the concentration of more volatile component (negative mixtures), Marangoni force is expected to induce the flow towards opposite direction and promote the heat transfer deterioration. For alcohol aqueous solutions, the value of surface tension changes significantly in the low alcohol concentration range and the existence of strong Marangoni force is expected. There exist a number of experimental and theoretical researches for the boiling heat transfer of binary mixtures. It is a well known fact from numerous boiling experiments that the nucleate boiling heat transfer coefficients of mixtures are usually lower than those of ideal or, more precisely, hypothetical single components with the same thermophysical properties as the mixtures. Van Wijk et al.[1] explained for the lower heat transfer coefficient of binary mixtures. They noted that the reduction of local liquid concentration of more volatile component increases the local saturation temperature underneath bubbles because more volatile component preferentially evaporates to maintain equilibrium between two phases. Consequently, the wall temperature rises and the heat transfer coefficient based on the saturation temperature of bulk liquid is lowered. Stephan and Krner[2] proposed a simple correlation based on the explanation given by Van Wijk et al.[1]. They defined the ideal heat transfer coefficients for mixtures which are given by the interpolation of wall superheats for both pure single components to represent the mixture boiling heat transfer coefficients in the absence of mixture effects. And they evaluated the heat transfer deterioration rate from the ideal heat transfer coefficients by using the difference between the molar fractions of both phases on the vapor-liquid equilibrium diagram. Calus et al.[3] considered the reduction of the bubble growth rate to evaluate the deterioration rate by using Scriven[4] and Van Stralen[5] analysis of the bubble growth. Thome[6] tried to calculate the deterioration rate by only using phase equilibrium diagram. He proposed a simple correlation which Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009

uses only temperature difference between dew and bubbling point temperatures at the bulk concentration. Kandlikar[7] theoretically analyzed the mixture property effects on nucleate boiling heat transfer. He introduced a new pseudo-single component heat transfer coefficient as the ideal heat transfer coefficient to reflect mixture property effects more accurately. And the mixture boiling heat transfer coefficient was derived theoretically by estimating the effects of heat and mass transfer at the vapor-liquid interface of a glowing bubble. In the above researches, only heat transfer deterioration of binary mixtures was discussed and Marangoni effect on the heat transfer coefficients of binary mixtures was ignored. On the other hand, there also exist a lot of studies for critical heat flux of mixtures. Several geometries of heating surface were tested and the result of either increasing or decreasing in the critical heat flux was observed. Hovestreijdt[8] first speculated that the Marangoni force affects the critical heat flux of binary mixtures. McGillis and Carey[9] suggested a correlation based on the speculation given by Hovestreijdt. They quantitatively estimated the Marangoni effect as an additional liquid restoring force caused by the surface tension gradient with a modified model derived from hydrodynamics. Fujita et al.[10] also considered the Marangoni effect to evaluate the increase in the critical heat flux of binary mixtures and proposed a correlation using the Marangoni number defined by using thermal diffusivity. McEligot[11] attributed the increase in the critical heat flux of binary mixtures to the increase in effective subcooling because the interfacial temperature is increased due to the preferential evaporation of more volatile component. Leddy and Lienhard[12] quantitatively evaluated the increase in the effective subcooling and suggested a correlation. The above researches, however, considered no geometry effect on the critical heat flux of mixtures. 3. EXPERIMENTAL APPARATUS AND PROCEDURE The experimental setup shown in Fig.1 is composed of three main parts, a boiling vessel, condensers and a heating section. The boiling vessel is made from a stainless steel pipe with inner diameter of 200mm and a volume of 0.023m3. Liquid and vapor temperature are measured by four thermocouples placed in the vessel. The condensers are installed in the upper side of the boiling vessel and control the levels of system pressure and saturation temperature. The detailed structure of heating section is also illustrated in Fig.1. A heating surface, which is the upper edge of the copper heating block, is heated by the cartridge heaters inserted in the bottom of the heating block. The horizontal upward-facing heating surface polished by sandpaper (No. 600) has a dimension of 40mm in diameter and is surrounded by a circular thin fin in order to prevent preferential bubble generation at the edge and minimize the circumferential heating loss from the periphery. In the heating block, eight thermocouples are inserted at the depth of 1, 7, 13, 19mm from the heating surface along two axes at the center and 14mm from the center. A surface heat flux and surface temperature are evaluated from the thermal conduction

Paper No: ITP-09-09

120 110 100 90

1-Propanol / Water
Bubbling Line Dew Line

Tsat C

Negative system

80
Positive system Azeotrope

70 0

0.2

0.4 0.6 0.8 Weight fraction wx1 (a) 1-Propanol/Water

Fig.1 Schematic diagram of experimental apparatus Table1 Test concentration range Test fluids Test bulk liquid concentrations of alcohol 1-Propanol/Water 0 ~ 90wt% 2-Propanol/Water 0 ~ 89wt% Water/Ethylene glycol 0 ~ 90wt% across the copper heating block by the indicated temperatures of thermocouples. Pool boiling experiments were conducted under saturated conditions. After the enough time is elapsed to confirm the steady state of indicated temperatures of all thermocouples and pressure, heat flux is increased. The condition of critical heat flux is detected by the excursion of temperature in the copper heating block. The heat flux one step before the value resulting temperature excursion is defined as a critical heat flux. The increment of input heat flux near the critical heat flux is 1.0105 W/m2 and the value gives the resolution of measured critical heat flux. The experiments were performed at 0.1MPa on ground. Three alcohol aqueous solutions, 1-Propanol/Water, 2Propanol/Water and Water/Ethylene glycol mixtures were employed as test fluids. Concentration ranges tested are shown in Table1 and the phase equilibrium diagrams of these mixtures are shown in Fig.2. In Fig.3, surface tension behavior of these mixtures is shown. 1-Propanol/Water and 2Propanol/Water mixtures have an azeotropic concentration, so they act as the positive mixture at the lower concentration of 1-Propanol and 2-Propanol than the azeotrope while they act as the negative mixture at the higher concentration of alcohol. For Water/Ethylene glycol mixture, it acts as the negative mixture in the entire concentration range. In the present research, Marangoni effect was evaluated by the Marangoni number using mass diffusion coefficient defined by Eqs. (1) and (2). Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009 3

120 110 100 90 80 70 0

2-Propanol / Water
Bubbling Line Dew Line

Tsat C

Positive system Negative system Azeotrope

0.2

0.4 0.6 0.8 Weight fraction wx1 (b) 2-Propanol/Water

Water / Ethylene glycol

Bubbling Line Dew Line

200 Tsat C 100

Negative system

0.4 0.6 0.8 Weight fraction wx1 (c) Water/Ethylene glycol

0.2

Fig.2 Phase equilibrium diagrams at 0.1MPa

Paper No: ITP-09-09

0.08
1-Propanol/W ater 2-Propanol/W ater W ater/Ethylene glycol

[104] 3 1-Propanol/Water

0.06

2
0.04

q=1.0105 W/m2 q=2.0105 W/m2 q=4.0105 W/m2 Ideal heat transfer coefficients Stephan and Krner correlation Thome correlation

W/m2K
1

N/m

0.02

0.2 0.4 0.6 0.8 1 Weight fraction of alcohol Fig.3 Surface tension under phase equilibrium condition at 0.1MPa

0 0

Azeotrope

0 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (a) 1-Propanol/Water

[10 ] 3
8

[104] 3 2-Propanol/Water
1-Propanol/W ater 2-Propanol/W ater W ater/Ethylene glycol

q=1.0105 W/m2 q=2.0105 W/m2 q=4.0105 W/m2 Ideal heat transfer coefficients Stephan and Krner correlation Thome correlation

W/m2K
1

Ma

0
Azeotrope

-1 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol Fig.4 Marangoni number

0 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (b) 2-Propanol/Water

m x ( y1 x1 )La m 1 Ma = l D
La m

[10 ] 3 Water/Ethylene glycol

4

(1)
2

m
g ( l ,m g ,m )

(2)

W/m2K

q=1.0105 W/m2 q=2.0105 W/m2 5 q=4.010 W/m2 Ideal heat transfer coefficients Stephan and Krner correlation Thome correlation

The calculated Marangoni number for the entire concentration range is shown in Fig.4. The larger heat transfer enhancement is expected for the larger Marangoni number. 4. EXPERIMENTAL RESULTS AND DISCUSSIONS Figure 5 shows the effect of concentration on the heat transfer coefficients at selected heat fluxes (1.0105, 2.0105, 4.0105 W/m2). For 1-Propanol/Water and 2-Propanol/Water mixtures, the increase in the heat transfer coefficients was Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009 4
0 0 0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (c) Water/Ethylene glycol 1

Fig.5 Heat transfer coefficients Paper No: ITP-09-09

observed at the very low concentration of alcohol. In the moderate concentration range, however, the heat transfer enhancement was turned to the heat transfer deterioration with increasing in the alcohol concentration. And at the azeotropic concentration, the heat transfer coefficient has a local maximum. For Water/Ethylene glycol mixture, on the other hand, no marked heat transfer enhancement or deterioration was observed and the heat transfer coefficients gradually decreased with increasing in the alcohol concentration. In the figure, predicted heat transfer coefficients by the existing correlations are also shown. Stephan and Krner[2] correlation and Thome[6] correlation are used, and the heat transfer coefficients of each pure alcohol are predicted by the Kutateladze[13] correlation because the experiments for the pure alcohol were not conducted due to the safety problem inherent in the experimental apparatus. Here, multiplying factors are introduced to adjust the predicted values to coincide with the experimental data for pure water and at the azeotropic concentration. The multiplying factors in the intermediate concentration range between zero (pure water) and the azeotropic concentration and between the azeotropic concentration and unity (pure alcohol) was evaluated by the linear interpolation of these multipliers, where a multiplier of unity was introduced for pure alcohols. As can be seen from Fig.5, both Stephan and Krner[2] correlation and Thome[6] correlation can reproduce the trends of measured heat transfer coefficients in the moderate concentration range for 1Propanol/Water and 2-Propanol/Water mixtures. For Water/Ethylene glycol mixture, however, the prediction of the heat transfer coefficients by Thome correlation is overestimated because its temperature difference between the dew and bubbling temperature at the bulk liquid concentration is too large. And the heat transfer enhancement at the very low concentration range can be reproduced by neither of these correlations. The heat transfer enhancement seems to be caused by the Marangoni effect, and the heat transfer enhancement overcomes the heat transfer deterioration due to mass transfer resistance because the Marangoni number has a peak value in the low concentration range and is markedly reduced with further increasing in the alcohol concentration as shown in Fig.4. Figure 6 shows the effect of concentration on the critical heat flux. The critical heat flux predicted by the Zuber correlation[14] for hypothetical single component liquids with the same properties as mixtures is also shown in Fig.6. In the moderate concentration range, the measured critical heat flux value was gradually decreased with increasing in the alcohol concentration. Zuber correlation can reproduce the critical heat flux trend. In the low alcohol concentration range, however, the critical heat flux was significantly decreased. The peculiar trend of critical heat flux was also reported by using a flat plate heating surface[15] while the markedly increase in the entire concentration range was observed by using a wire heating surface[10,12]. Thus the trend of the critical heat flux depends on the geometry of heating surfaces, but the logical explanation or correlations which consider the geometry effect has not be provided. The low concentration Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009 5

107

1-Propanol/Water
Experim ental results Zuber correlation

qCHF W/m2

106

105 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (a) 1-Propanol/Water

107

2-Propanol/Water
Experim ental results Zuber correlation

qCHF W/m2

106

105 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (b) 2-Propanol/Water

107

Water/Ethylene glycol
Experim ental results Zuber correlation

qCHF W/m2

106

105 0

0.2 0.4 0.6 0.8 Weight fraction of alcohol wx (c) Water/Ethylene glycol

Fig.6 Critical heat flux Paper No: ITP-09-09

range, where the peculiar decrease in the critical heat flux was observed, corresponds to the peak Marangoni number. Consequently, Marangoni effect is suggested again as a possible cause for the peculiar trend of the critical heat flux. How Marangoni effect influences to the critical heat flux mechanism is deduced as follows. Marangoni force is directed towards the three-phase interline underneath primary bubbles because of the preferential evaporation of alcohol for positive mixtures. The Marangoni effect supplies liquid spontaneously to the microlayer of the primary bubbles. As a result, evaporation of microlayer is enhanced and heat transfer coefficient is increased. On the other hand, the enhanced evaporation causes finally the shortage of liquid stored in macrolayer and drypatches are extended from some locations where primary bubbles were existed. The extension of drypaches is continued under a coalesced bubble, and the excursion of surface temperature occurs before entire part of liquid in macrolayer is consumed. Thus the critical heat flux condition seems to be realized independent of the period for the detachment of a coalesced bubble and it varies with the intensity of Marangoni force induced around primary bubbles. This mechanism might be true for the flat plate heating surface where liquid supply to primary bubbles is indirectly via the formation of macrolayer during the detachment of coalesced bubbles and not directly by bulk liquid. 5. CONCLUTIONS The boiling heat transfer and the critical heat flux of alcohol aqueous solutions were investigated through the saturated pool boiling experiments using 1-Propanol/Water, 2Propanol/Water and Water/Ethylene glycol mixtures at 0.1MPa. The following conclusions were derived. (1) The increase in the heat transfer coefficients was observed at the very low alcohol concentration of 1-Propanol/Water and 2-Propanol/Water mixtures while the critical heat flux was markedly deceased in the same alcohol concentration range. (2) The above trends of the heat transfer and the critical heat flux are deduced to be caused by the Marangoni effect, which accelerates the evaporation of the primary bubbles in macrolayer underneath coalesced bubbles. ACKNOWLEDGMENTS This work was supported by Grant-in-Aid for JSPS Fellows (211862) from Japan Society for the Promotion of Science (JSPS). The authors express the appreciation for the support. REFERENCES [1] W.R. Van Wijk, A.S. Vos, & S.J.D. Van Stralen, Heat transfer to boiling binary liquid mixtures. Chem. Engng. Sci., 5: 68-80 (1956).

[2] K. Stephan & M. Krner, Calculation of heat transfer in evaporating binary liquid mixtures. Chem. Ing. Tech., 41: 409-417 (1969). [3] W.F. Calus & D.J. Leonidopoulos, Pool boiling - Binary liquid mixtures. Int. J. Heat Mass Transfer, 17: 249-256 (1974). [4] L.E. Scriven, On the dynamics of phase growth. Chem. Eng. Sci., 10: 1-13 (1959). [5] S.J.D. Van Stralen, Bubble growth rates in boiling binary mixtures. Br. Chem. Eng., 12: 390-394 (1967). [6] J.R. Thome, Prediction of binary mixture boiling heat transfer coefficients using only phase equilibrium data. Int. J. Heat Mass Transfer, 26: 965-974 (1983). [7] S.G. Kandlikar, Boiling heat transfer with binary mixtures : Part I - A theoretical model for pool boiling. Trans. ASME, 120: 380-387 (1998). [8] J. Hovestreijdt, The influence of the surface tension difference on the boiling of mixtures. Chem. Eng. Sci., 18: 631-639 (1963). [9] W.R. McGillis & V.P. Carey, On the role of marangoni effects on the critical heat flux for pool boiling of binary mixtures. Trans. ASME, 118: 103-109 (1996). [10] Y. Fujita & Q. Bai, Critical heat flux of binary mixtures in pool boiling and its correlation in terms of Marangoni number. Int. J. Refrig., 20: 616-622 (1997). [11] D.M. McEligot, Generalized peak heat flux for dilute binary mixtures. AIChE J., 10: 130-131 (1964). [12] R.P. Reddy & J.H. Lienhard, The peak boiling heat flux in saturated ethanol-water mixtures. Trans. ASME, 111: 480486 (1989). [13] S.S. Kutateladze, Heat transfer in condensation and boiling. USAEC Report, AEC-tr-3770 (1952). [14] N. Zuber, Hydrodynamic aspects of boiling heat transfer. USAEC Report, AECU-4439 (1959). [15] G.I. Bobrovich, I.I. Gogonin, S.S. Kutateladze, & V.N. Moskvicheva, Critical heat fluxes with the boiling of binary mixtures.Zh.Prikl. Mekhan. I Tekh. Fiz., 4: 108-111 (1962).

Interdisciplinary Transport Phenomena VI, Volterra, Italy, 2009

Paper No: ITP-09-09