Journal of Membrane Science, 33 (1987) 299-313 299

Elsevier Science Publishers B.V., Amsterdam - Printed in The Netherlands

HEAT AND MASS TRANSFER IN MEMBRANE DISTILLATION*

R.W. SCHOFIELD, A.G. FANE and C.J.D. FELL

School of Chemical Engineering and Industrial Chemzstry, University of New South Wales,
Kensington, N S. W. (Australaa)
(Received August 12, 1986; accepted in revised form October 22,1986)

Summary

Equations for heat and mass transfer in membrane distillation (MD) have been developed and
tested experimentally. The concept of temperature polarisation is introduced and shown to be
important in the interpretation of experimental results Vapour transport through the membranes
tested is reasonably described by combined Knudsen and molecular diffusion. The significance of
temperature polarisation in the design and operation of large-scale MD modules is discussed, and
hollow fibre and tubular systems shown to be potentially the most effective.

Introduction

Membrane distillation (MD) is a membrane process which is being devel-

oped for the production of high purity water and for the removal of water from
solutions to effect concentration. The process relies on a non-wetted hydro-
phobic membrane through which water vapour is driven by an imposed tem-
perature gradient. Potential applications of MD have been discussed by a
number of workers [l-4] and some experimental and theoretical studies have
also been described [ 4-71.
One aspect of performance of MD which has received little attention is tem-
perature polarisation. This refers to the loss of driving force brought about by
thermal gradients in the fluids bounding the membrane. Figure 1 depicts the
temperature profile for the situation where liquid contacts both sides of the
membrane. The profiles would be marginally different for the case where an
air gap is maintained between the membrane and cold product [ 3,7] I In this
paper, the theories of mass and heat transfer within the membrane and adjoin-
ing fluids have been developed for the conditions of Fig. 1 with a view to char-
acterising temperature polarisation. The resultant equations give both a direct
means of measuring temperature polarisation in experimental systems, and a
method of predicting temperature polarisation in industrial MD modules.

*Paper presented at the Workshop on Membrane Distillation, Rome, Italy, May 5, 1986

0376-7388/87/$03.50 0 1987 Elsevier Science Publishers B V.

 Membrane

Cool
dlstlllate
Tl

Temperature
polorlsotlon
Hot Ti ----TC
solution

Fig. 1. Temperature and pressure profiles in membrane distillation.

Theory

(a) Mass and heat transfer

Mass transfer in MD occurs by convective and diffusive transport of water
vapour across the microporous membrane. The driving force for mass transfer
is the difference in water vapour pressure on either side of the membrane.
Resistance to mass transfer comes from both the membrane structure, and the
presence of air trapped within the membrane. The resistance imposed by the
membrane structure (in the absence of air) can be described by either the
Knudsen diffusion model or the Poiseuille flow model, the latter being domi-
nant when the membrane pore size is larger than the mean free molecular path
of the gaseous water molecules. As the mean free molecular path of saturated
water vapour at 60 0C is around 0.3 pm ( a typical MD pore size ) , both models
must be considered. The mass flux from the Knudsen diffusion model may be
expressed as

where the first term in eqn. (1) is the Knudsen diffusion coefficient corrected
for membrane porosity and pore tortuosity, and the second term is the concen-
tration driving force. Since

and

cl =P1 M/RT

eqn. (1) may be written

 301

N,=1.064$ FT 05(p, -PO) (2)

( >
The Poiseuille flow model is based on viscous flow through a capillary, and
can be expressed as

NP = sporenporeMP, lR T (3)

where sporeis single pore flow,

4pore= nr4AP/8v&

is pore density,
and npore

npore = hr2
Equation (3 ) becomes

N,=O.d-" ;; y;T(PI -PO) (4)

Mass flux through a stationary film of air can be described by the molecular
diffusion model [ 81

ND=$-$FT (P,-P,)
In

The above three models may be useful for predicting mass fluxes in MD;
however, each has its limitations. The Knudsen and Poiseuille models require
knowledge of r, 6 and e, which in general must be estimated by applying the
models to experimental gas fluxes through the given membrane. The molecular
diffusion model is not adequate at low partial pressures of air, for as Y1,,-+O,
Nn is undefined. Clearly N should approach Np or NK as appropriate.
The above three models suggest a relationship of the form,

N=C(P, -PO) (6)

where C can be considered a membrane mass transfer coefficient for the sys-
tem. Inspection of the three models suggests that C will be slightly temperature
dependent, decreasing by about 3% with a 10’ C increase in mean temperature.
If convective transport is dominant, C will be strongly dependent on the mem-
brane pore geometry. If diffusive transport is dominant, the controlling param-
eter will be the average mole fraction of air present within the pores, Y,,,
As vapour pressures within the membrane are not directly measurable, it is
convenient to express eqn. (6) in terms of temperatures”
302

lv=cg (T, -T*) (7)

Till

Equation (7) is accurate for dilute solutions with values of ( T, - To) less than
lO”C, for which it may be approximated that (PI-P,) /( T,- To) =dP/dT
evaluated at T,. dP/dT can be evaluated from the Clausius-Clapeyron equa-
tion [9],
dP -- PAM (8)
dT ,/RT2
-I 1Tm

using the Antoine equation to evaluate P [ 91:

23.238- ,““‘,, (9)

m
Equation (7) must be modified for more concentrated solutions to account
for the reduction in vapour pressure caused by dissolved species [S] :

N=Cg[(T, -To) -ATth](l-ix,)

where AT,, is a threshold temperature given by

For ( Tl - To) <AT,,, a negative flux is observed due to the reduction in vapour
pressure caused by dissolved species in the distilland. A 20000 ppm salt solu-
tion at T, = 60°C has x:= 0.006 and AT,, = 0.13”C. Thus the temperature cor-
rection AT,, would only be important for concentrated feed solutions or in the
presence of significant concentration polarisation.
Heat transfer in MD occurs by two major mechanisms. Firstly, there is latent
heat transfer accompanying vapour flux, and secondly there is heat t,ransfer
by conduction across the membrane. The latent heat flux for dilute solutions
is simply

Q,,=N~=C~k(T,-To) (12)

The conductive heat flux is

Qc= (htI4CT1 -To) (13)

where kM is the effective thermal conductivity of the membrane, calculated
from the gas and solid conductivities by [ 61
k~=tkg+ (1--E)k, (14)
 303

T, .IL
Q” T,

Q TC
H
b ho
(1,

Fig. 2. Heat transfer in MD.

As Q, serves no useful function, it can be considered as a heat loss, and should

be minimised. This is the rationale behind the air-gap concepts [ 3,7]
Combining equations (12) and (13) gives the total heat transfer across the
membrane as

Q=Qv+Qc

= C$$l+kM/S)(T,-TO)
(

=H(T, -To) (15)

where His the effective heat transfer coefficient for the membrane. It is impor-
tant to note that H increases with T,, as dP/dT increases with T, (cf. eqns.
(8) and (9)).

(b) Temperature polarisation

The equations presented in the previous section require knowledge of the
interfacial temperatures T, and To. However, due to temperature polarisation
( see Fig. 1) , these temperatures may vary markedly from the measureable bulk
temperatures T,, and T,. For example, consider an MD system with a typical
mass flux of 10 kg/m’-hr. The thermal gradient in water necessary to provide
the latent heat is dT /do = QJk= 11 ‘C/mm. Thermal gradients of this mag-
nitude must lead to substantial temperature polarisation.
To quantify temperature polarisation, consider the representation of heat
flows in MD shown in Fig. 2. For heat transfer to and from the membrane
surface we have

Q=hl(Th-T1)=ho(To-T,) (16)
where hl and ho are film heat transfer coefficients for the hot and cold fluids,
respectively. From eqns. (15) and (16)
(T, -To) = (Tr,-T,)/(I+Whi +H/&) (17)
=z(T,-T,)

where r = l/ (1 + H/h, + H/h,) is the “temperature polarisation coefficient”,

representing the fraction of the total thermal driving force ( T,, - T,) that con-
tributes to the mass transfer driving force ( T1- T,,) . Ideally, z should be as
304

----T-F
8:s 1 2 i
I/(dP/dT)x 1000 (K/Pa)

Fig. 3. Analysis of Hanbury’s results.

close to unity as possible; however, as shown below, many systems have r val-
ues closer to zero. It should be noted that 2 varies with T, as H varies with T,,,
hence the notation z ( 60” C ) will be used to denote r at T, = 60 ’ C.
An understanding of temperature polarisation is necessary for both the anal-
ysis of experimental MD data and the design and appraisal of MD equipment.
For the analysis of data, the temperature polarisation equations must be cou-
pled with the membrane mass and heat transfer equations. Combining eqns,
(7) and (17) for dilute solutions, and substituting the overall film heat trans-
fer coefficient h = l/ (l/h, + l/h,) gives

(18)

Substituting H= CLdP/dT+ kM/6 from eqn, (13) and rearranging gives

(19)

where AT= ( Th-- T,).

Equation (19) may be used for the analysis of experimental result~sfor which
Th, T, and N are reported, as dP/dT is a function of T, = ( 7’, + Ti) /2, assum -
ing the temperature polarisation is similar on either side of the membrane.
Provided kJ6 can be estimated or measured, the only unknowns in eqn. (19)
are h and C. A plot of AT /NA vs. l/ (dP/dT) should yield an intercept of l/h,
and a slope of (l/CL) (1+ &‘ah), from which C may be obtained,
As an example, we analyse the results of Hanbury and Hodgkiess [ IO] ) who
report that for their experimental system
Ni/AT=4.9 T,!,,17(W-m-‘-K-l) for30<T,<70°C
A plot of eqn. (19) for these results is shown in Fig. 3 for T,=30, 40, 50, 60,
7O”C, and is found to be linear. From Fig. 3 for Hanbury’s system h== 1100 W-
-‘-K-l and C=8.5~ 1.O-7kg-m-2-set-1 -Pa-l (assuming a typical value of
EM/S-500 W-mp2-Kp’).
 The temperature polarisation coefficient for this system at T, = 60’ C is cal-
culated as follows:
H=C~~dP/dT+k,/S=1800+500=2300 W-m-2-KP’
and
h=llOO W-m-2-KP’
so

~(60°C) =1/(1+2300/1100) =0.32

Hence for this system, when the bulk temperatures are Th = 65 ’ C and T, = 55 a6,
the actual temperature difference across the membrane is ( T, - To) = 3.2 ‘C.

(c) Temperature polarisatlon in MD modules

The temperature polarisation coefficient is a usful tool for the design and
appraisal of MD systems. To illustrate this, values of z have been estimated
for some of the more common membrane geometries and flow characteristics”
The z, values presented in Table 1 account for polarisation on one side of the
membrane. and are based on the membrane distillation of water at a point
alongthe membrane where II=2000 W-mP2-K-land T=70”C. Hence,
z,=l/(l+H/h,) =1/(1+2000/h,) (20)
An overall z can be calculated from the predicted z,values for either side of the
membrane by
2=1/(1/2,+1/2,-l) (21)
The film heat transfer coefficient, h,, was estimated for the various cases by
means of the dimensionless Nusselt number, Nu = hd/k. Values of NU are read-
ily available for simple flow geometries [ 111, based on an appropriate char
acteristic length, d. Table 1 lists some common membrane geometries, flow
regimes and approximate values of h, and z L.The results reported for conduct-
mg films reflect the temperature loss in a film of liquid between a heat transfer
sheet and a membrane. A sample calculation is given in the Appendix,
The results presented in Table 1 indicate that the most thermally efficient
MD systems are likely to be tubular membranes in turbulent flow, and hollow
fibre membranes in laminar flow. It is apparent, however, that temperature
polarisation on the outside of the tubes may be excessive. For the sheet mem-
brane geometries, best results are obtained with very thin conducting films,
however, turbulence promoters may reduce polarisation to an acceptable level
in channel flow.
The overall z for a stirred cell at Re= 32000 can be calculated from eqn. ( 21)
as z = l/ (l/O.4 + l/O.4 - 1) = 0.25, suggesting that stirred cells are not suitable
for MD experiments. From eqn, (19)) the relationship between flux and aver-
306

TABLE 1

Temperature polarisation in various MD systems

Membrane geometry Flow characteristic Nu d h, z,B

(mm) (W-m ‘-K ‘)

1 mm i d. tube Re = 5000 29 1.0 19000 0.90

Re = 3000 20 1.0 13000 0.85
Re = 1000 4.4 1.0 2900 0.54
0.3 mm i.d. tube Re= 300 44 0.3 9700 0.80
0.6 mm o.d. tube bundle close packed lammar -5 0.9 3700 0.6
Channel 0.5 m long velocity=2 m-set’ 970 500 1300 0.51
Conductmg film
2 mm thick laminar 5.4 8 450 0.15
0.5 mm laminar 5.4 2 1800 04
0.1 mm laminar 54 0.4 8900 07
Stirred cell Re= 8000 54 50 710 02
Re= 32000 120 50 1600 04

“Temperature polarisatron coeffrcrent for one side of the membrane.

age temperature can be derived in terms of the overall film heat transfer coef-
ficient, h. In Fig. 4 this relationship is shown for a range of h values with
dT= 10’ C . Values of the temperature polarisation coefficient at 60 ‘C for the
various h are also shown
Much may be learned from the shapes of the curves in Fig. 4. For example,
for any given MD system, if flux at dT= 10°C appears linear with !I’,,, and
increases by only three-fold over the range 7’, = 30 to 80’ C, this is a fair indi-
cation that temperature polarisation is excessive, with z( 60°C) being around
0.25. If, on the other hand , the flux increases exponentially by five-fold over
the same temperature range, it would indicate that z( 60°C ) is around O-7.
It must be emphasised that temperature polarisation becomes more signifi-
cant as the membrane heat transfer coefficient, H, increases. Equations (8)
and (15) show how H increases with average temperature, T,_ For the system
analysed in Fig. 4, when r( 60°C) = 0.50, the temperature polarisation coeffi-
cients at T,=30 and 90°C are ~(30°C) =0.67 and z(9O”C) -=0.30.

Experimental

A series of experiments was conducted to investigate the transport mecha-

nisms in MD and test the proposed method for analysis of temperature polar-
isation. Three flat sheet hydrophobic microporous membranes were tested
(Enka 0.1 ,um and 0.2 ,um pore size and Durapore 0.45 pm pore size) ; their
reported properties are given in Table 2.
 307

h=oD
Th- Tc = 10°C

h=5000

hollow
flbre

h=2000
sheet
membrane
h=lOOO
stlrred cell
h=500

I 1 1 1 1 1

40 50 60 70 80 90 100

T,,,
f"C)
Fig. 4. Predicted effect of temperature polarlsation on mass flux for a 0.2 pm pore size membrane
having C=5 x 10-7kg-m~2-sec~‘-Pa~‘and 12,/d =500 W-rn-‘-Km’.

Initial experiments involved the measurement of gas permeation rate versus

pressure drop for both air and helium at subatmospheric pressures, to assess
the applicability of Poiseuille or Knudsen flow to the chosen membranes.
Thermal conductivity was also determined, by direct measurement of heat flow

TABLE 2

Properties of membranes used

Membrane Enka Enka Durapow

Polymer Polypropylene Polypropylene Polyvinylidene
fluoride (PVDF)

Nominal pore size, @rn 0.1 0.2 0.45

Thickness, mm 0.10 0.14 011
Voidage 0.75 0.75 0.75
 Membrane area:1 I8 cm*

Fig. 5. Experimental apparatus.

through the dry membranes when sandwiched between two chambers of dif-
ferent temperature. The equipment used for this was the MD cell (described
below), suitably modified.
Figure 5 depicts the sheet membrane apparatus used for MD experiments
The membrane was contacted on either side by a film of distilland or distillate
0.05 mm thick, bounded by a thin stainless steel heat transfer plate. Access to
the membrane surface was facilitated by grooves in the plate. A layer of hydro-
philic tissue paper maintained the fluid film thickness at 0.05 mm, while acting
as a wick to keep the membrane surface wet. The stainless steel plates were
heated or cooled by jets of recirculating water. The design of the module was
intended to minimise temperature polarisation.
All experiments were conducted using distilled water as the distilland. The
feed was partially deaerated at the heating water temperature to prevent air
bubbles forming within the module. Distillate flow rates were measured by
burette, and distillate pressure exceeded distilland pressure by - 50 mmH,O.
Preliminary tests showed that for fixed dT the flux was constant over an
extended period. Subsequent tests were run with heating water temperatures
at 60, 70 and 80’ C, but allowing the insulated cooling water reservoir to rise
gradually in temperature. In this way, each experiment provided values of flux,
N, for various dT.

Results and discussion

The results for the permeation tests on the 0.1 pm pore size Enka membrane
are presented in Fig. 6, showing that N&P and N/dPccM” ‘. This suggests
that for gas transport the mechanism is predominantly Knudsen diffusion
From these results, the membrane pore geometry component of eqn. (2 ) was
measured as re/~S = 5.8 x lop4 for air and 5.1 x 10e4 for helium. From the
assumed membrane properties (Table 2 ) , the predicted value is 1.9 x lo- 4 (for
x = 2 ) , showing poor agreement, possible due to the basis of defining nominal
 (cl DURAPORE 0 45 pm
J

o 10 20 30 40 50 60

P, - PC IkPa) l/k,P/dT)r1000 (K/Pa)

Fig. 6. Gas permeation results for Enka 0.1 pm polypropylene membrane.

Fig. 7. Experimental results for the membrane distillation of water using Enka 0.1 pm and 0.2 pm
polypropylene, and Durapore 0.45 pm PVDF membranes.

pore size. For the Knudsen diffusion of water vapour, rt/~6 was estimated as
5.5 x 10P4, from the air and helium data. Gas permeation data for the other
membranes gave r-c/Xc? values of 6.5 x 10 -*and 11.6 x 10e4for the 0.2 pm Enka
and the 0.45 ,um Durapore, respectively; predicted values were again low being
2.7~ 10P4and 7.8~ 10P4.
The thermal conductivity of the dry air-filled 0.1 pm Enka membrane was
measured as Izh?=0.046 -+0.005 W-m-*-KP1. This compares favourably with
the value predicted by eqn. (14) of kM= 0.052 W-m-l-K-l. It would be expected
that most commercial microfiltration membranes would have a thermal con
ductivity between 0.04 and 0.06 W-mP1-K-l, increasing with decreasing
porosity.
Experimental MD data have been plotted according to eqn. (19), AT /N.Avs.
I/ (dP/dT) , in Fig. 7 (a,b,c) for the three membranes. The linearity of the data
provides support for the form of eqn. (19) for average temperatures from 40
to 75”C, and for ( T, - To) ranging from 1 to 10 ‘C. The experimental scatter
in Fig. 7 is predominantly due to the sensitivity of measuring distillate volumes.
Table 3 presents the measured film coefficient, h (from the intercept on Fig.
7), the polarisation coefficient, z( 60’ C ) ) and the membrane mass transfer
310

TABLE 3

Measured and predicted transport characteristics

Membrane

Enka Enka Durapore

Pore szze (,um) 0.1 0.2 0.45

Temperature polarisatLon
h film coeficient, W-m-‘-K 2440 2380 2490
z( 60 GC) polarisation coefficient 0.63 0.65 0.62

Experimental mass transfer

coeffccient 4.5 4.3 4.8
C ( X 107), kg-mp2-s m1-Pa-1

PredLcted mass transfer coeffLclents

CD molecular diffusion ( x 107) 8.8” 6.3 8.0

(i) from measured pore geometry

rt/x6 ( X 104) 5.5 65 11.6
CK Knudsen diffusion ( X 107) 15h 1% 32
Cc combined diffusion ( x 107) 6.3 5.5 7.6
(11) from specified pore geometry
rt/x6 (104) 1.9 2.7 7%
CK Knudsen diffusion ( x 10T) 52 74 21.3
Cc combined diffusion ( x 107) 3.5 3% 68

“Equations (5) and (6) with 0=2.88X lo-“m2-set ~I, Y,,=O.% andX=2
bEquatlons (2) and (6) with T=GO”C.

coefficient, C (from the slope of Fig, 7) for each of the membranes tested. Also
presented are values of the mass transfer coefficients predicted from molecular
diffusion theory, CD, and Knudsen diffusion theory, CK, based on both the
measured and the specified pore geometries. The combined mass transfer coef-
ficient, Cc, accounts for the mass transfer resistances of both molecular and
Knudsen diffusion [ 12 ] ,

cc= (Y,,/cn+l/G-l (22)

Considering the difference in their pore sizes, the three membranes per-
formed in a surprisingly similar manner, as evidenced by the experimental
mass transfer coefficients, C, presented in Table 3. This suggests a mechanism
based largely on molecular diffusion, which is independent of pore size (eqn.
5). However, mass transfer coefficients estimated from molecular diffusion
theory, CD, were higher than the observed coefficients, C, by 50 to 100%.
Inspection of the various predicted mass transfer coefficients in Table 3 indi-
cates that the combined molecular/Knudsen diffusion coefficients, Cc, best
describe the mass fluxes observed. This should be regarded as a preliminary
 311

attempt to elucidate the nature of vapour transport in MD with further work

being required.
The temperature polarisation coefficient for the experimental system was
measured to be z (60’ C) = 0.63 t 0.02. This result is important in two respects‘
Firstly, high transmembrane temperature differences may be obtained using
this apparatus, resulting in a high range and accuracy of experimental condi-
tions. Secondly, this is confirmation that sheet membrane systems can indeed
be designed with acceptable levels of temperature polarisation. Despite the
high thermal efficiency of the apparatus used, failure to account for tempera-
ture polarisation in the experiments conducted here would result in overesti-
mation of the mass transfer driving forces by 60%, with a corresponding
underestimation of the experimental mass transfer coefficients by 40%. These
results highlight the fact that any attempt to compare a membrane distillation
transport model with measured data must take into account the significant
influence of temperature polarisation.

Conclusions

For the membrane distillation of aqueous solutions through polymeric

microporous membranes:
(i) Conduction of heat through the membrane can be estimated by the
equation

Q= (kMld)(T1 -To)
where
IzM=Ekp + (l-e)Iz,
(ii ) Vapour flux through the membrane can be described by the equation
dP
N’CE (T, -T*)

where the membrane mass transfer coefficient, C, may be reasonably esti-

mated from a combination of Knudsen and molecular diffusion theories.
In many experimental and industrial MD systems, the bulk of the available
thermal gradient is lost in temperature polarisation. Of the commonly used
MD systems, tubular and hollow fibre membranes show the least temperature
polarisation.

Acknowledgements

The authors gratefully acknowledge support from: Memtec Limited; the

National Energy Research, Development and Demonstration Council of Aus-
tralia; and the Commonwealth of Australia.
312

List of symbols

C concentration, kg-m-”
c membrane coefficient, kg-rn-*-seccl-Pa-l
d hydraulic diameter of channel, m
D diffusion coefficient, m2-set-l
h film heat transfer coefficient, W-m-2-Kp1
H membrane heat transfer coefficient, W-m-‘-K -I
k thermal conductivity, W-m-1-K-1
M molecular weight, kg-mol-’
N mass flux, kg-m-‘-set-l
P pressure (of water vapour) , Pa
4 volumetric flow rate, m3-set ~’
Q heat flux, W-m-’
R gas constant, J-mol-l-K-l
r membrane pore radius, m
T temperature, K
V channel velocity, m-set-l
X mole fraction of dissolved species, [ - ]
Yhl mole fraction of air (log-mean), [- ]
s membrane thickness, m
E porosity, [ - ]
gas viscosity, Pa-set
1 latent heat of vaporisation, cJ-kgg1
P liquid viscosity, Pa-set
P liquid density, kg-md3
z temperature polarisation coefficient, [ - ]
x tortuosity factor, [ - ]
Nu Nusselt number hd/k, [ - ]
Re Reynolds number pud/p, [ - ]

Subscripts
P Poiseuille flow model
K Knudsen diffusion model
M molecular diffusion model
C combined diffusion model
h,l,m,O,c defined in Fig. 1

References

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Appendix

Sample calculation for temperature polarisatron coefficient

Membrane tube; inside diameter, d = 0.001 m
Average velocity u = 2 m-s-‘; Re =pvd/p= 980 x 2 x 0.001/0.00042
=4700
Heat transfer from Dittus-Boelter equation
Nu =I0.023 Re” ‘Pro 4

Pr=C&k=2.6 (at 70°C)

At some point along the tube where H = 2000W-m ~ ‘-K-~ ’
Nu=0.23x4700°s x2.604=29.2

h= kNu/d = 0.66 x 29.2/0.001= 19000 W-m-*-K-’

Polarisation coefficient
z( 70°C) = l/ (1+ 2000/19000) = 0.90