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© vom (0038-092 (95)00069-0 Solar Energy Vol 58, No.6 pp. 527-535, 1995, Copseight © 1995 Elvi Science Led Printed inthe U.S.A. All ights reserved ‘O03 092N/95 58.50 + 0.00, NEW DEVELOPMENT IN THE THEORY OF HEAT AND MASS TRANSFER IN SOLAR STILLS AHMAD TALEB SHAWAQFEHt and MOHAMMED MEHDI FARIDt Chemical Engineering Department, Jordan University of Science and Technology, Irbid, Jordan (Communicated by TY A. NEWELL} Abstract—A single basin solar still with basin area of 098 « 0.98 m was constructed from galvanized iron sheets and an inclined glass cover. The still was provided with 525 W electrical heating tapes, fixed under the still basin for indoor steady state operation. The variation of basin temperature, glass temperature and evaporation rate were measured during both indoor and outdoor operation. The hourly variation of Solar radiation, ambient temperature, and wind velocity were also taken during the outdoor measurements. ‘Transient analysis ofthe still requires the evaluation of evaporative, convective and radiative heat transfer coefficients, The Dunkle model, which has been widely used forthe prediction of the evaporative coefficient, was found 10 overpredict evaporation rates. The models developed in this work were found to provide better prediction for the evaporation rate measured in this work and in some previous works. INTRODUCTION Even though the use of basin-type solar still was suggested more than one hundred years ago, the first theoretical treatment of the subject, appeared in 1961. Heat transfer between the evaporating surface and the glass cover is con- trolled by free convection. evaporation, and radiation. Hence the understanding of these modes of heat transfer is essential for the predic- tion of the performance of any solar still. Dunkle (1961) has used a modified Grashof number Gr’ to describe free convection in the still following the same approach suggested by Sharpley and Boelter (1938) for evaporation of water into still air. However, Dunkle used the following empiri- cal correlation developed by Jakob (1957) for free convection of air in an enclosure: assuming it to describe the condition inside the still Nu =0.075 Ra" ay or Coke] A =cors|| es ‘| AT'S (2ap where AT =AT+ Pea Pe T rn M,PyAM, — My)— Py | (2b) ‘To whom all correspondence should be addressed at: Department of Chemical Engineering, Clarkson Uni versity, CU Box 3707, Potsdam, NY 13699, US.A. HISES member. Present address: School of Chemical Engineering, University Sains Malaysia, 31750 Tronoh, Perak, Malaysia In order to develop an expression for the evaporative heat transfer coefficient in the still, most investigators have adopted the following relationship, developed cither from a simple mass balance of the water vapor in the still or from a simplified form of the Chilton-Colburn analogy, known as the Lewis relation, as shown by Malik er al. (1982): ne | = M+], "IC, M, Pr" In the above relation, the effect of water vapor was assumed negligible which can be true only at low temperatures as will be discussed later in the paper. If the physical properties of the air at the stil operating temperature range are substituted in eqn (3), the group in brackets would have values ranging from 0.014 to 0015. A value of 0.013 was reported in the literature by Malik er al. (1982) for this group which was obtained by assuming saturated air at 50°C. In order to account for the effect of water vapor pressure, Dunkle (1961) has used an experimental value of 0.0163 for the above group and hence the error introduced in using eqn (1) was eliminated but only within the operating temperature range studied by Dunkle: () h, = 0.0163h, 4 Equations (2) and (4) have been used up to this date by most of the investigators to evaluate the convective and evaporative heat transfer coefficients in solar stills, However, in recent work carried out by Al-Mahdi (1992) new cor- 328 A. T. Shawagfeh and M. M. Farid relations for the convection coefficient were suggested, A literature review shows no development in the theory of heat and mass transfer in the still since it was originally proposed by Dunkle in 1961. The main drawback of the analysis devel- oped by Dunkle and used by other investigators is due to two serious assumptions: (1) Free convection in the still may be described by eqn (1) originally developed for free convection of air without evaporation (2) The use of the constant 0.0163 in eqn (4) is correct only at the operating tem- perature of the still used by Dunkle (1, © 50°C). Extensive literature may be found on the transient analysis of single and double-basin solar stills, based on the Dunkle analysis. However, most of them are theoretical predie- tions and only a few of them include comparison with experimental measurements as in Sodha et al. (1980a, 1980b, 1981a, 1981b), and Kamal (1989). Further, most of these studies were done on stills operating at low basin temperature (less than 50°C) with the exception of the works done by Ahmed (1988), Kamal (1989). and Farid and Hamad (1993), who reported some measurements with basin temperatures of 70-80°C. Uncertainty in still parameters such ay its plate absorptance, glass transmittance, and wind loss coefficient may have played a significant role in hiding the deviation of the Dunkle relation as will be discussed in this paper 2, DEVELOPMENT OF INTERNAL STILL CONVECTION/EVAPORATION TRANSFER COEFFICIENTS The empirical eqn (2), which was used for the evaluation of the convection coefficient by most investigators, was rejected here since it was developed from experiments of free convection in the absence of evaporation, If the exponent 1/3 was retained in eqns (1) and (2) due to the expected turbulence in the still, then these equa- tions may be used directly by replacing the constant 0,075 by another constant (n) to be evaluated from the true measurements in the still. The evaporative heat transfer coefficient defined by eqn (3) is correct only at operating temperatures low enough for the water vapor pressure to be negligible. Hence the analysis based on such assumption and used by most investigators requires some _ modifications. Accordingly, two approaches will be adopted: (1) Analysis similar to that described by Malik et al. (1982), usually known as the Dunkle analysis, but taking into account the effect of water vapor pressure as follows If m, is the mass of dry air circulated through. the still by free convection, then a simple mass balance between the evaporating surface and the glass cover gives mee,“ lea al (5) Heat transfer by convection between the water surface and the glass cover due to mass flux of humid air, mpig. may be written as follows: de = Mais CPT = Te) Mais Pr MC ton My | Py — (Py + Pyyh which simplifies to: cc, Max Pr MCP ME | Py (Py which together with eqn (5) gives 1 1 MMC ra lm a ml ne) In egn (8), water vapor pressure was eval- uated at the average temperatures of the evapo- rating surface and glass cover. This equation provides an evaporative coefficient which is more sensitive to the operating temperature than that shown by egn (3). (2) Chilton-Colburn’s analogy between heat and mass transfer provides another expression for the evaporative heat transfer coefficient. The exact form of Chilton-Colburn’s analogy, as presented by Coulson and Richardson (1977), is te (9) Movin Cre (Padiat Even though the above equation has been widely used to evaluate the rate of evaporation in many unit operations, it has not been used in its exact form to predict evaporation rates in solar stills. An approximate form of Chilton-Colburn’s analogy, which is commonly Heat and mass transfer 529 used in the literature, is obtained by assuming Le= 1 and (P,),4~ Py. This leads to the Lewis equation which is similar to eqn (3). The Lewis equation is expected to deviate significantly from the exact Chilton-Colburn’s equation as may be seen from the values of je-¢ [the ratio P, Le*9/(P,),44] in Table 1 which show a devi- ation of about 58% from the Lewis relationship or Dunkle equation at T, = 70°C and Ty 60°C. In comparing eqn (9) with eqn (8), one may notice that 1 . 1\ 1 1 | Pin (3) (Pa (Pde and hence the difference between the two equa- tions is due to the effect of the Lewis number. The well known Stefan-Maxwell equations, used to describe diffusion of a single or multi- components in a non-diffusing component described by Sherwood et al. (1975), may be used to derive the Chilton Colburn equation, However, Le’? must be used to convert the mass to thermal boundary layer thickness, which is defined by (Kmix Ite} The evaporative heat transfer coefficients defined in eqns (3), (8) and (9) have the units ‘of (W m7? Paé') and they must be multiplied by (Py PyhtTy— Ty) to convert the units to (Wm-?K_~'). Physical properties of the humid air were estimated from the weighted average ‘of the properties of air and water vapor at different temperatures using empirical correla- tions available in the literature. 3. SOLAR STILL SIMULATION MODEL Transient analysis of solar stills is well described by Malik er al. (1982). It requires the solution of the following two differential equations: ch * de C, Ty 6g A, i gg = (ne de de de My UD (gH. + det de + deen (10) where: de = NAT — Ty) Ge = Hel Tw — Te) T,) ~T). Gen = eas + Haga MT — Ta) ls CL= Cp /Ap. The convective heat transfer coefficient h, was caleulated from eqn (2) for the Dunkle model, and by using the same equation, but with different constants for the other two models. The evaporative heat transfer coefficient h, was calculated for the different models using eqns (3),(8) and (9), The other coefficients are defined explicitly in Malik et al. (1982) ‘The wind loss coefficient was determined from the following empirical correlation developed by Watmuff er al. (1977): iogs =28 +30" Vy (12) which has not been used by the previous investi- gators who used the correlation: Iroge (3) Duffie and Beckmann (1991) have recom- mended the use of eqn (12), stating that eqn (13) overpredicts the loss coefficient as it includes the effect of radiation with the forced and natu- ral convection. However, the constant 2.8 may increase as the glass temperature increased. Equations (10) and (11) were solved using a fourth order Runge-Kutta method with time increment of two minutes. Solar radiation, ambi- ent temperature, and wind velocity were fitted to polynomials for use in the numerical calcula- tions, Equation (12) was used in the theoretical simulation of this work, while eqn (13) was used for the other investigators works. ees T+38*M, 4. EXPERIMENTAL MEASUREMENTS A single basin solar still was constructed from, 1.4 mm thick galvanized iron sheet, with a basin area of 0.98 x 0.98 m as shown in Fig, 1. The Table 1. Evaporative heat transfer coeficient obtained from different models Dunkle oo hy cE) Eek Wm Kp 4 04683 1037 106 30 47.283 mt 1409 © 50 oD 2912 Liss tty 3s Bulk Motion model Chilton-Colburn model 530 A.T. Shawagfeh und M. M. Faid 1. -CONVECTION(4,). 8-BOTTOM LOSSES(a.) 2-EVAPORATION(q,) |inside $—RADIATION(G,) 4-CONVECTION(qege)| outside 5—RADIATIONCGige) Hs GLASS. FRAME 6-REFLECTION | 7 ABSORPTION § GLASS COVER INSULATION (ROCK WOOL) DISTILLATE }-wooo Box OUTLET | COLLECTION al BASIN. PLATE CHANNEL, Fig. 1. Schematic diagram of the experimental solar still heights of the front and back walls were 0.1 and 0.47 m, respectively, giving a glass cover inclina- tion of 19°. The basin of the still was painted black after polishing and spraying with corro- sion resistant paint A rectangular 4mm thick glass sheet was fitted in an iron frame. The frame holding the glass cover was tightened to the still with bolts, using a rubber gasket to avoid vapor leak ‘An inclined rectangular channel was welded at the short side wall of the still from inside for condensate collection, Aplastic channel was fixed inside the rectangular metal channel with insulation between them to avoid evaporation of the condensate as it flowed along the channel. The still was insulated at its bottom and walls with 30 mm thick rock wool insula- tion. A wooden box was used to encase the still and the insulation Electrical heating was added to the still to allow steady state measurements of solar still Five electrical heating tapes with a power of 105 W each were fixed between an asbestos sheet and the bottom of the still. The evenly distributed heating tapes were connected in parallel to an ac. power supply to provide variable heating power to the unit Chromel-Alumel (type K) thermocouple wires were used for temperature measurements, connected to a multi-channel programmable temperature chart recorder. One thermocouple junction was silver welded 1o the basin of the sill, while another was immersed in the conden- sate collected to represent the average of the glass temperature, Direct glass temperature measurements were found inaccurate due to radiation effects, as reported by Farid and Hamad (1993). Another thermocouple was used to measure the variation in the ambient temperature. Solar radiation was continuously measured using a Kipp and Zonen type pyranometer provided with an integrator. Also the wind speed was measured, at hourly intervals, using a wind speedometer. At the end of each hour, the condensate collected was measured with a graduated cylinder. 5. RESULTS OF INDOOR MEASUREMENTS The indoor steady state measurements were used to generate accurate information on the dependence of the evaporation rate on both basin temperature 7, and the driving temper- ature difference (T,—,). The function AT’ defined by eqn (2b) includes both of these parameters. Figure 2 shows the dependence of the hourly measured evaporation rate, M,., on AT’ for the experimental data of this work as well as Sodha et al. (1980a, 1981b), Yen et al (1985), Ahmed (1988) and Kamal (1989). This figure also includes some outdoor measure- ments. The strong dependence of M,, on AT’ is, due to the fact that AT’ includes the effect of mass transfer enhancement on heat transfer as may be seen from eqn (2b). The data of Fig. 2 were used to calculate the evaporative heat transfer coefficient, hy, by dividing the product of M, and 4, by the driving temperature (T,~T,). The calculated Heat and mass transfer su 000 Malgm/m’.hr Ars) Fig 2. The effect of modified temperature difference AT” on the hourly solar still production, values of fh, were then used to calculate the values of convective heat transfer coefficient. h, using the two models discussed earlier. The results were plotted in Fig. 3(a) for the Bulk Motion model and in Fig. 3(b) for Chilton-Colburn model. The empirical correla- tions obtained from the best fit are: ogy = 0.057 * Ra’ aa) A... = 0.051 #Ra’ «sy These two correlations predict values of , Jower than the values obtained from eqn (2a) which was adopted by Dunkle (1961) and most of the other investigators. As in eqn (2), the above two equations provide expressions for the convection heat transfer coefficient independent of still geometry. Equations (14) and (15), as well as eqn (2) were used with the Bulk Motion, Chilton Colburn, and Dunkle models, respectively, to predict evaporation rates in the still. Figure 4 shows that both Bulk-Motion and Chilton. Colburn models predict the experimental values of M, very well, while Fig. 5 shows that Dunkle model overpredicts the values of My by about 40%. Table 1 shows a comparison between the cal culated values of h, using the three models at different T, and with T, — T, = 10°C. The varia- tion in the ratio h,/h, in Dunkle model is due to the change in the slope of vapor pressure temperature curve, AP/AT only. However, the variation in h,/h, in the other two models is due to the increase in the values of yay and Yee With temperature, as well as due to the increase in the slope of vapor pressure—temper- 25° F geese Tris wom BEE Cd a. {188 i Spb Scat ot Sk Hao} POOF REEREES.”. Ames [1965) © ob enm=0.0574Ro! (is Wor] Ce ee a a ro ead von BLS'S 4 (8, F bones cota & St fant noo | Seppe stn” Rs geaes? So, Y. of necen005teRo (Ins Wor) 9.00 fae peng ani ee to Ro! Fig. 4. The variation of convection heat transfer coefficient with Ra’ using: (a) Bulk Motion model: (b) Chilton-Colburn ‘model We ea (r9as) Soe (1888, {Sooee s0une Sit) 8808} 2oee Gea lf aese ‘$8RGEST. Ahmed (1988) ng Recstiis Wor} Mero (gmn/m!.tr) Fig 4. Comparison between experimental hourly pro duction of solar still with that predicted by Chilton-Colburn ‘and Bulk Motion models, sx f Yeh etal. (1985 ‘Banas Sedna et ai 13 Beppe Sean et Gi/1380e Seen wh kamal 385) feast GTS 138 Bee Maas Grn /-07 he Fig 5. Comparison between experimental hourly pro: duction of solar still with that predicted by Dunkle mode! ature curve, Values of jnwy and yee are a measure of the deviation of the two models from the Dunkle model (which has a value of p= 1.0). 6. RESULTS OF OUTDOOR SIMULATION Verification of the models with outdoor meas- urements was made from the measured values of T, and T,, The results for the three models are shown in Figs 6-8. The use of the measured T, and T, in the calculations of My and h. eliminates any error that may occur due to the use of incorrect values of still parameters such as (tap and (ra}g. The agreement between the measured and the predicted evaporation rate, using both Bulk Motion and Chilton-Colburn. ‘models was reasonable, while the Dunkle model (20000 Tw Exf 5 TEMPERATURE Co Fig 6. Calculated hourly production of solar still, using the three models with the measured basin and glass temper: atures for this work, Irbid, 22 October 1992. A. T, Shawagfeh and M. M. Farid ‘20900 Tw:£x>. IEEE 19:2 RP. Fig. 7. Caleulated hourly production of solar stil using the three models with the measured basin and glass temper: atures for Sodha e? al. (19803) Fig. 8. Calculated hourly production of solar stil, using the Uhtee models with the measured basin and glass temper- “atures for Farid and Hamad (1993). overpredicted the fluxes, similar to what has been observed from the indoor measurements. In the transient analysis of the solar still, an initial estimate was made for water and glass cover temperatures. Predictions of the basin temperature, glass cover temperature, and evap- oration rate were then calculated after every two minutes. The experimental measurements of this work, Sodha et al. (1980a), and Ahmed (1988) were used to test the validity of the three models at different still operating conditions, as shown in Figs 9-12 These figures show the similar prediction of the three models. It is expected that any varia- tion in the value of h, due to the use of different models, will cause opposite change in T, —T, to compensate the effect of h,. This is to satisfy the energy balance on the still defined by eqns Heat and mass transfer 533 faves 1,550" E05) 500) 100 290 faanee uate so E eer an | FOSS NEBr ‘eo 9, ahr : “ TIME ( Fig 9. Hourly variation of Hi 995, Tek Irbia. October Thea TeeN = Te:bunite 0g Fig 10. Comparison between the predicted and measured performance of solar still for this work, Irbid, 22 October 1992 ERATURE Fig. 11. Comparison between the predicted and measured performance of solar sul for Sodha er al. (19804), Fig. 12. Comparison between the predicted and measured performance of solar still for Ahmed (1988). (10) and (11), which explains the insignificant change in the evaporation rate predicted by the different models. In spite of the close agreement between the prediction of the three models, their agreement with the measurements was not always satisfac- tory. This is believed to be due to uncertainty in some of the parameters used in the simulation such as (t2)p, (ta),, and wind loss coefficient. It can not be attributed to models failure since any error in the estimated value of h, will not affect the estimated evaporation rate signifi- cantly as discussed previously Figure 12 illustrates a discrepancy in the measurements, showing glass cover temperature higher than water and ambient temperatures, a situation which can not be described by the models. This is why the calculated glass cover temperature decreased rapidly to very low values initially before it started to increase close to the experimental values. However, the predic- tion of both water temperature and evaporation rate were excellent during the whole period of operation. It is worth indicating that Ahmed (1988) has not given any prediction for the water and glass cover temperatures in his paper. The results of Ahmed were used to test the validity of the models even with the existence of the errors mentioned in his measurements. This is due to the scarcity of the experimental measurements on solar stills at temperatures above 70°C in the literature. Most of the previous investigators have used a constant wind velocity, an assumption found to affect the prediction of the glass cover temper- ature significantly sa Fig, 13, Hourly performance of solar still for different values of (rth this work: Irbid. 22 October 1992 In order to realize the possible causes of the overprediction of the fluxes by the three models, the effect of some reduction in the value of (+2}p was tested and the results are shown in Fig. 13 A decrease in (r2}p from 0.7 to 0.6 is likely to happen due to the deterioration of the absorber plate coating with time. Figure [3 shows that such effect may reduce the evaporation rate by about 20%, giving better agreement with the measured values. However, the predicted glass cover temperature will be lower also. Figure 13 also shows that it is unnecessary to include the hourly variation of (zap. during the day as it has insignificant effect Another source of error in the theoretical prediction may be due to the use of eqn (13). by all previous investigators which overpredicts the wind loss coefficient significantly. The use of a high wind loss coefficient allowed the use of a relatively high evaporative coefficient nor- mally predicted by Dunkle equation. The uncer- tainty in the values of these parameters suggest that the experimental values of 7, and 7, should be used for accurate evaluation of the evapora- tive heat transfer coefficient. The common pra tive of varying h, (usually called hy.) to improve the agreement between measurements and pre- diction should not be followed. 7. CONCLUSIONS This study showed that the Dunkle model may overpredict evaporation rates by about 30%. The models developed in this work on a more sound basis, provided better prediction of the rate of water evaporation in the still The effect of (r2}p and the wind loss coeffi- cients were found significant on the predicted ALT. Shawagfeh and M. M. Farid Ty. T, and M,. The uncertainty in these parame- ters is enough to make the transient analysis of the still not suitable for the prediction of the evaporative heat transfer coefficient, hy In order to eliminate the effect of these still’s parameters, the measured values of T, and T,, in the outdoor operation, should be used for the evaluation of fh. Indoor measurements under controlled conditions are an even better choice for this purpose. NOMENCLATURE A, surface area of the glass cover (m: Ap surface area of the basin plate (m*) Bulk Motion model CC Chilton-Colburn model lass heat capacity per unit area (J m~? K~') CE heat capacity of water in the still per unit area Um?k) Cp, specific heat capacity of the glass ke! K~*) Cp specific heat capacity of the water (J kg“! K~") Ch, specific heat capacity of ai (J kg~' K~*) Caz specific heat eapacity of the water vapor-air mixture Uke K-4, Da diflusvity of water vapor in air (m? s“*) "e gravity acceleration (m s~=) Zivgh AT. Grashof number (dimensionless) " AT, modified Grashof umber (dimensionless) fh, bottom loss heat transfer coefficient (W m=? K*) Ac convection heat transfer coefficient (W m=? K™") fz evaporative heat transfer coefficient (W m7? K!) og, sonVectiON heat transfer coefficient, using Bulk Motion model (Wm? K>") h., convection heat transfer _ coefficient, ‘Chulton. Colburn model (Wm? K-¥) , convection heat transfer coefficient, using Dunkle model (Wm? K-!) lye convection wind loss coefficient (W m=? K~!) TN radiation heat transfer coefficient, inside the still Wak radiation heat transfer coefficient, outside the stil Wak) 1, solar radiation intensity (W m~*) Ay thermal conductivity of water vapor-air mixture using Wm kK) foe thermal conductivity of water vapor-air mixture wmitk ys Le koa WiC rn Dans Lets number (dimensionless) M, wvoleclar Weight of dry air (kg kgmmol~") ‘m, mass of dey abr cicculated in the sill per unit time tkes Maye moleculae weight (ke kgmol-") res Mass-of humid air circulated in the still pee unit time (kes) M,_ mass of mole flux of water evaporated per unit ime tkgm=?s-" or kemolm=?s—") 41.2; hy, Nusselt umber (dimensionless) log meg of the sir partial presture (a) partial pressure of dry aie atthe glass cover condi tons (Pa) partial pressure of dry air at the basin of the still onditians (Pa) of water vapor-air mixture Na Padi Ph Pay Heat and mass transfer 535 partial pressure of water vapor at the glass cover conditions (Pa) , total pressure in the still (Pa) Py partial pressure of water vapor at the basin of the still conditions (Pa) 4. fheat loss from the bottom ofthe still (W m~*) 4, heat transfer rate in the still due to convection wm) 4, heat transfer rate in the still due to evaporation wm) dys heat transfer cate from the glass to the ambient due to the convection and radiation (W m~*) 4g, heat transfer rate in the still due to radiation (Wm (ei gBC,Z"AT ta (FPE29) pastegh ander dimensiones HBP) cry a (PAPC) 97°15 moitied Raseigh number w) (wm a) T, ambient temperature ( C) Jy glass cover temperature ( C) f, basin temperature ( C) ¥ wind speed (ms!) Z thickness of the diffusion boundary layer (m) Greek symbols # WT, coefficient of thermal expansion of the sull(K") AT (T, ~ Ty), temperature dilference between basin and eliss cover ('C) AT’ as defined by egn (211 C) (Weciet oe) (A st | isiensionle Le) co (=) tamensiontess latent heat of vaporization of water hg Ti wsonty of the water vapors mixture team's fy dest ofthe water vapor ate mitre keen) REFERENCES Ahmed S. T. Study of a single-effect solar stll with an internal condenser. Solar Wind Technol. 5, 637-643, (1988), AL-Mahdi N. Performance prediction of a multi-basin solar still. Energy 17, 87-93 (1982), Coulson J. M. and Richardson J. F. Chemical Engineering, 3rd edn, Vol. I. Pergamon Press, New York (1977). Due J. A. and Beckman W. A. Solar Engineering of Ther- ‘mai. Provesses, 2nd edn. Wiley-Interscience, New York (1991), Dunkle R. V. Solar water distillation: the roof type still and 4 muhiple effect diffusion still, ASME Proc. Int. Heat Transfer Cont. Part V. Int. Develop. 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N. and Tyagi R.C. Simple multiple wick solar still; analysis and perfor- mance. Solar Energy 26, 127-131 (1981a). Sodha M.S., Kumar A., Singh U. and Tiwari G. N, Further studies on double” basin solar still Energy Res. 5, 341-352 (1981) \Watmulf J. H., Charters W. W. S. and Proctor D. Solar and wind induced external coefficients for solar collectors Comples 2, (1977) Yeh H., Ten L. and Chen L. Basin-type solar distillers with ‘operating pressure reduced for improved performance, Energy 10, 683-688 (1985).

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