Reverse Osmosis of Dairy Liquids
J. H I D D I N K , R. de BOER,
ABSTRACT
Permeate flux during reverse osmosis
of skim milk, Gouda cheese whey at
various pH, desalted whey, ultrafiltration
permeate, and lactose solutions were
studied. The flux-limiting factors of the
feed appeared to be osmotic pressure and
fouling agents. Protein in Gouda whey at
pH 6.6 did not give rise to fouling;
however, after desalting or decrease of pH
to 4.6, fouling by whey protein occurred.
If Gouda whey was concentrated at 30 C
over a concentration ratio of 1.6:1,
calcium-phosphate precipitation caused
strong fouling of the membrane. This
fouling can be prevented by removing
calcium from the whey or by acidifying
to a pH of about 6.0. During reverse
osmosis of skim milk, casein is the
principal fouling material.
To understand better the influence of
the process conditions on the permeate
flux, the effect of concentration polari-
zation and fouling was calculated for
various conditions. It appeared possible
to achieve a reasonably low concentration
polarization and fouling by applying, in a
tubular system, flow velocities of 2 m/s
for whey and of 2.5 m/s for skim milk.
Furthermore, for skim milk an optimum
process pressure was about 3.5 MPa.
INTRODUCTION
In the dairy industry reverse osmosis (RO) is
used more and more as a concentration tech-
nique (6, 11, 13, 26). The main advantage of
RO over evaporation is the low energy consump-
tion (2). In the Netherlands RO has been
in use for some years for the concentration of
whey and ultrafiltration permeate. The main
reason whey is concentrated at the cheese
Received April 2, 1979,
1980 J Dairy Sci 63:204--214
and P.F.C. NOOY
Netherlands Institute for Dairy Research (NIZO)
P. O. Box 20
6710BA Ede, The Netherlands
factory is savings on costs of transport from the
cheese factory to a central whey processing
plant.
At the moment, seven RO plants with a
water removal capacity ranging from 3.5 to 15
m3/h have been installed, four of them using
tubular membranes and three of them using flat
membranes. In principle, two processes can be
distinguished. One process involves concentra-
tion of whey at 30 C in a tubular single-pass
system, to a concentration ratio of about 2:1.
In the second process whey is cooled to 10 or
17 C and then concentrated, batchwise or in a
continuous system, to a concentration ratio of
2:1 or 3:1. An important factor for RO is the
permeate flux, this factor governing to a large
extent the economy of the process. The factors
affecting the permeate flux, in addition to the
properties of the membrane, are the composition
of the feed and the process conditions.
Though RO membranes can be made of a
variety of materials (cellulose acetate, poly-
amide, cellulose nitrate, sulfonated poly-
phenylene oxide, polybenzimidazolone), up to
now only cellulose acetate (CA) has proved to
be commercially acceptable for RO of food and
dairy liquids. For process conditions, tempera-
ture is of particular importance. Raising the
temperature of the feed increases the permeate
flux, but to work under completely safe
bacteriological conditions a temperature below
10 C or above 50 C should be used. Cellulose
acetate (CA) membranes should not be operated
above 35 C since these membranes are subject
to hydrolysis and compaction at higher tempera-
tures. This consideration should lead to a
process temperature of 10 C. In practice,
however, temperatures of 30 C (temperature of
the Gouda cheese whey) and 17 C (temperature
of the whey after cooling with cold milk in a
heat exchanger) are also used. At these tempera-
tures extensive precautions, such as a short
residence time and intermediate disinfection,
must be taken to prevent bacteriological
spoilage.
204
 REVERSE OSMOSIS OF DAIRY LIQUIDS
Concerning the properties of the feed,
osmotic pressure and the fouling tendency must
be considered. The osmotic pressure of dairy
liquids is determined mainly by the low molecu-
lar weight solutes such as salts and lactose. It
must be overcome by the applied process
pressure.
Fouling can be caused by precipitation of
certain salts and by build up of a deposit of
colloidal material. It should be prevented by a
proper pretreatment of the feed and by applying
proper process conditions. A number of investi-
gations referred to in the literature deal with
the fouling properties of the various components
of whey and skim milk and with the composition
of the deposit. Lira et al. (15), Peri and Dunkley
(18), and Mehta (16) concluded that during
concentration of cottage cheese whey, the
principal fouling material is protein, and
particularly casein. The selective concentration
of casein was explained by its low diffusion
coefficient. Smith and McBean (28)investigated
membrane fouling in RO of cheddar cheese
whey and hydrochloric acid casein whey. They
found that calcium plays an important part in
membrane fouling, in particular precipitation of
insoluble calcium salts. The pretreatments
developed by Hayes et al. (12) for reduction of
fouling in uhrafiltration led to increased fouling
in RO. This was ascribed to the higher ionic
concentration that with RO takes place in the
surface layer on the membrane. Glover and
Brooker (10) and Skudder et al. (27) studied by
electron micrographs the structure of deposits
formed during RO of whole milk. The deposit
consisted mainly of casein micelles while
Ca-phosphate was precipitated in the deposit
during concentration.
Concerning the process conditions which
should be applied for RO of whey and skim
milk much work has been done. The essential
difference between the early work (8, 15, 18)
and more recent work (5, 25, 26, 27) is the
difference in applied flow velocity. In the early
work the flow velocity was .10 to .55 m/s (at a
tube diameter of 1.25 cm), but in the more
recent work flow velocities of 2 to 3 m/s were
applied at a similar tube diameter. With these
higher velocities much better permeate fluxes
were achieved. Typical applied pressures in
both cases were 3 to 5 MPa and temperatures
between 10 and 35 C.
Our work was aimed at acquiring a better
205
understanding of the effect of both composition
of the feed and process conditions (temperature,
flow velocity, and pressure) on the permeate
flux. In particular we tried to quantify the
effect of concentration polarization and fouling.
Our study was restricted to skim milk, Gouda
cheese whey, and their derivatives.
MATERIALS AND METHODS
Experimental Procedure
A laboratory recirculation RO plant was
used, consisting of two modules type B1
(length 3.66 m) from Paterson Candy Inter-
national Ltd., England. The modules were
provided with tubular CA membranes type
T2/15W with an inner diameter of 1.3 cm and a
salt rejection of about 93%. The membrane area
per module amounted to 2.55 m 2.
The experiments were by batch; from a tank
the liquid was pumped through the system by a
piston pump and returned to the tank while the
permeate was drained. Each experiment took 2
to 4 h. The process temperature was maintained
at 10 or 30 C. If a process temperature of 30 C
was used, the liquid was heated in the tank
before starting the experiment. Pressures were
between 2.5 and 4.5 MPa and flow velocities
between 1 and 2.6 m/s. The flow velocity was
calculated from the rate of flow divided by the
area of cross-section of the membrane tube.
Before use, the skim milk and the whey were
separated (6800 × g) and pasteurized at 72
C/15 s.
Dairy Liquids
Composition of the dairy liquids tested is in
Table 1. When whey was desalted, a strong acid
cation exchange resin and a weak base anion
exchange resin were used. About 95% of the
mineral matter was removed. The ultrafiltration
permeate (UF-permeate) was obtained by UF
of whey at 10 C. The pH of all liquids referred
to in Table 1 was 6.5 to 6.7 or was adjusted to
that pH. In some of our experiments we used
Gouda cheese whey acidified with HCI to pH
6.0 or 4.6.
In some experiments whey was used from
which 90% or more of the calcium was removed
by ion exchange with a weak cation exchange
resin, which was regenerated with HC1 and
NaOH. After regeneration the resin is in Na +
form. In Table 1 the osmotic pressure for the
Journal of Dairy Science Vol. 63, No. 2, 1980
206 HIDDINK ET AL.

TABLE 1. The composition, the osmotic pressure at 10 C and the dynamic viscosity at 10 C of the dairy liquids
used.

Total Whey Osmotic Dynamic

solids Lactose Ash protein Casein pressure viscosity

(%) (MPa) (mPa.s)

Skim milk 8.9 4.6 .7 .7 2.8 .72 2.8
Gouda whey pH 6.6 5.5 4.1 .5 .7 .. .61 1.6
Desalted whey pl-I 6.6 5.1 4.1 .03 .6 .. .35 1.6
UF-permeatc 5.0 4.1 .5 .2 a .. .61 1.5
Lactose solution 4.0 4.0 . . . . . . . . .30 1.4

aNonprotein nitrogen × 6.38.

various liquids is given also. T h e o s m o t i c also. T h e increasing o s m o t i c pressure o f t h e

pressure was d e t e r m i n e d b y m e a s u r i n g t h e
freezing p o i n t d e p r e s s i o n w i t h a K n a u e r l lalb-
m i k r o - O s m o m e t e r t y p e M. T h e o s m o t i c pres-
sures at 10 C a n d 30 C were c a l c u l a t e d f r o m t h e
freezing p o i n t d e p r e s s i o n a c c o r d i n g t o t h e
m e t h o d d e s c r i b e d b y Reid (21).
T h e viscosity o f t h e various liquids was
d e t e r m i n e d b y an E M I L A R h e o m e t e r ( T a b l e 1).
Samples were a n a l y z e d a c c o r d i n g to t h e
f o l l o w i n g m e t h o d s : t o t a l solids b y d r y i n g in an
oven at 105 C; t o t a l p r o t e i n b y t h e Kjeldahl
p r o c e d u r e ( p r o t e i n f a c t o r 6.38); lactose a c c o r d -
ing t o L u f f - S c h o o r l ( 2 4 ) ; ash b y d r y i n g in
an o v e n at 105 C a n d h e a t i n g in an electric
m u f f l e f u r n a c e at 550 C for at least 8 h; a n d
calcium b y a f l a m e p h o t o m e t e r .
r e t e n t a t e caused a decreasing driving f o r c e for
w a t e r p e r m e a t i o n (see A p p e n d i x A, e q u a t i o n
[1] ). T h e d i f f e r e n c e b e t w e e n t h e p u r e w a t e r
flux and t h e calculated curve A in Figure 1
r e p r e s e n t s t h e effect of t h e r e d u c t i o n o f t h e
driving force b y t h e o s m o t i c pressure.
Curve A w o u l d be f o u n d if we h a d to cope
o n l y w i t h an e f f e c t o f increasing o s m o t i c
pressure. Curve B in Figure 1 w o u l d be f o u n d if
t h e effect o f c o n c e n t r a t i o n p o l a r i z a t i o n also is
t a k e n into a c c o u n t . C o n c e n t r a t i o n p o l a r i z a t i o n
is d e f i n e d as t h e b u i l d - u p o f s o l u t e s n e a r t h e
m e m b r a n e , w h i c h as a result causes an increase
9Pr'leate fix ,1121}

~_ pure waler flux

31/ . . . . . . . . . . . . %. . . . . . . . . . . . . . . . .
RESULTS A N D DISCUSSION

Influence of Composition 1

of Feed at 10 C \ effect o~ (on{enlrahon p31arh'dtl )n

A series o f R O e x p e r i m e n t s was w i t h liquids \

\
in T a b l e 1. The liquids were c o n c e n t r a t e d
d u r i n g t h e e x p e r i m e n t s a t a process t e m p e r a t u r e
o f 10 C, an average pressure of 4 MPa, a n d a
flow v e l o c i t y o f 2 m/s. A t this flow v e l o c i t y t h e 5
x• ~
e e 0 0 n9 f ~
tollllng
~a ~deseltedwhey~ "~
R e y n o l d s n u m b e r s were 5 0 0 0 to 2 0 0 0 0 ,
d e p e n d i n g o n t h e viscosity o f t h e liquid. n Z 4 6 8 10 1.2 I4 16 18 20 22 2.4 20
0sm0hc pressure ,~Pal
The experimentally determined permeate
Figure I. Permeate f l u x versus osmotic pressure o f
fluxes are in Figure 1 as a f u n c t i o n o f t h e the b u l k liquid f o r RO o f various liquids. The experi-
o s m o t i c pressure o f t h e b u l k liquid. During mental fluxes are compared with those calculated
c o n c e n t r a t i o n t h e o s m o t i c pressure o f t h e assuming no concentration polarization and no f o u l i n g
r e t e n t a t e increased, a p p r o x i m a t e l y in p r o p o r t i o n (curve A) and with those calculated assuming o n l y
concentration polarization (curve B). Process condi-
w i t h t h e c o n c e n t r a t i o n ratio, w h i l e t h e p e r m e a t e
tions: T = 10 C, P = 4 MPa, v = 2 m/s. • lactose,
f l u x decreased. In Figure 1 t h e p u r e w a t e r flux o UF-permeate, X sweet whey, o desalted whey, and
u n d e r t h e r e l e v a n t process c o n d i t i o n s is i n d i c a t e d skim milk.

Journal of Dairy Science Vol. 63, No. 2, 1980

 REVERSE OSMOSIS OF DAIRY LIQUIDS
of osmotic pressure at the membrane surface
(see Appendix A). Curve B was achieved by the
evaluation of equation [6] of Appendix A. In
Figure 1 the experimental permeate fluxes for
RO of the lactose solution, the UF-permeate,
and the whey resemble more or less the calcu-
lated curve B. The experimental permeate
fluxes for desalted whey are lower than those
calculated for only concentration polarization.
Here fouling also plays a role. Fouling is defined
as the deposition of colloidal material on the
membrane surface, giving rise to an additional
hydraulic resistance, acting in series with the
membrane resistance. The difference between
curve B and the experimental permeate flux in
Figure 1 is a measure of the degree of fouling.
For desalted whey the cause of the fouling may
be due to the high degree of desalting, about
95%, because the stability of the whey protein
is affected, which may cause a tendency to
aggregate at the membrane surface.
For skim milk the differences between
experimental and expected (assuming only
concentration polarization) permeate fluxes are
even bigger. The casein in skim milk is respon-
sible for considerable fouling, because its high
concentration and low diffusion coefficient
cause formation of a deposit (gel layer) on the
membrane surface (10, 27).
Under these conditions, the osmotic pressure
was the main governing factor for Gouda whey,
UF-permeate, and the lactose solution. In the
case of desalted whey and skim milk a fouling
tendency also has to be considered.
Influence of Composition
of Feed at 30 C
A second series of experiments was at 30 C.
In Figure 2 are plotted the experimental
permeat fluxes versus the osmotic pressure of
the bulk liquid. The permeate flux calculated
according to equation [6] of Appendix A, for
only concentration polarization, is presented
also (curve B). For Gouda whey and UF-
permeate, the permeate fluxes initially resemble
those calculated. However, at a concentration
ratio of about 1.6:1 (osmotic pressure about 1
MPa) a sudden decline in permeate flux was
found. Obviously considerable fouling of the
membrane t o o k place. Since both whey and
UF-permeate show this behavior, it is not likely
that the whey protein was responsible for this
effect. During the RO of decalcified whey the
207
strong flux decline was not found, and the
permeate flux resembled that of the calculated
curve B. Based on this information it was
assumed that during the RO of whey and
UF-permeate, precipitation of Ca-salts on the
membrane occurred. Solubility of Ca-phosphate
decreases with increasing temperature (1, 20,
23). Apparently during the RO of whey and
UF-permeate at 30 C at a concentration ratio
of about 1.6:1 fouling of the RO membrane by
precipitated Ca-phosphate started. This fact
agrees with observations of Roger et al. (22)
that in UF-permeate heated to temperatures
above 30 C a fine mineral precipitate is formed
which causes fouling of UF membranes.
For the effect of process temperature on
permeate flux, a comparison of Figure 1 and
Figure 2 shows that the pure water flux in-
creases by about 3% per degree. The initial
permeate flux for whey and UF-permeate at 30
C was also about 60% higher than at 10 C, but
due to the strong flux decline at a concentration
ratio of about 1.6: 1, the permeate flux at 30 C
decreased to below that at 10 C.
For skim milk we see that at 30 C, just as at
10 C, the permeate flux was much lower than
the calculated flux, for only concentration
polarization (curve B), so a severe fouling had
to be considered. Probably the fouling was
permeate flux dim 2. h)
50 h -. . .-. . -. . . . . pu_re__waterfI_u_x. . . . . . . . . . .
L L I I L I I
0 .4 .8 1.2 1.6 2.0 2.4 2.8
osmotic pressure (MPa}
Figure 2. Permeate flux versus osmotic pressure of
the bulk liquid for RO of skim milk, whey and UF-
permeate at 30 C, P = 4 MPa, and v = 2 m/s. Curve B
was calculated according to Appendix A assuming only
concentration polarization (no fouling). • Gouda
cheese whey pH = 6.6, × decalcified whey, a UF-
permeate, obtained at 55 C, o UF-permeate, obtained
at 10 C, and o skim milk.
Journal of Dairy Science Vol. 63, No. 2, 1980
208 HIDDINK ET AL.

caused mainly by casein. Since milk is saturated surface may occur. This p h e n o m e n o n agrees
with Ca-phosphate (20), during heating and with that for UF of whey at various pH (9).
concentration a certain precipitation of Ca-
phosphate will take place. The fact that this Influence of Process Conditions
precipitation of Ca-phosphate did not give such
The process conditions such as temperature,
a strong flux decline as in the case of whey and
flow velocity, and pressure have a considerable
UF-permeate may be attributed to the precipi-
effect on permeate flux, and time also can be
tation of Ca-phosphate on casein micelles, and
an important factor. To make the discussion
therefore less precipitation on the membrane.
easier, three resistances to permeation often
In experiments in which UF-permeate,
can be distinguished: the membrane resistance
obtained by UF at 55 C, was concentrated by
Rm, the fouling resistance Rf, and the apparent
RO, the strong flux decline did not occur, the
resistance which can be attributed to concen-
permeate flux being similar to that for decalci-
tration polarization Rp (see Appendix B). The
fied whey (see Figure 2). During UF of whey or
membrane resistance especially is affected by
skim milk at those high temperatures a precipi-
temperature; the higher the temperature, the
tation of Ca-phosphate occurred in the UF
lower the Rm. For the other resistances the
retentate (23). As a result, the UF permeate
matter is more complex as they are particularly
had a lower Ca and phosphate content. In our
dependent on flow velocity and pressure. In the
experiments UF-permeate obtained at 10 C
interpretation of our experiments it is assumed
contained 33 mg Ca and 30 mg P/100 g while
that the effect of time on the permeate flux can
UF-permeate obtained at 55 C had 25 mg Ca
be neglected. This assumption can be justified
and 25 mg P/100 g, which means a reduction of
since each experiment lasted only a few hours.
about 25%. In the latter UF-permeate during
During longer periods the effect of time on the
RO to 30 C apparently no more membrane
permeate flux certainly becomes important.
fouling took place. Roger et al. (22) reported a
similar observation. They found an improvement
Effect of Flow Velocity
in flux of UF-permeate in an enzyme reactor by
removing 15% of the Ca. According to the method in Appendix B, for
Solubility of Ca-phosphate increases at lower
pH (1, 20). At a pH of about 4.9 phosphate
appears to be completely in solution in milk
(20). Some RO experiments were with whey at permeate flux (I/m 2. h)

30 C at various pH. From Figure 3 when . . . . . . p._ur e._w_ater _flEx . . . . . . . . . . . .

50
the whey was acidified to pH 4.6 or even to pH
6.0, the strong flux decline, pH 6.6, did not 40
occur. At pH 4.6 Ca-phosphate is supposed to
be completely soluble so we do not expect
30
Ca-phosphate fouling. At pH 6.0 more Ca-
phosphate is soluble than at pH 6.6. Solubility
20
is improved enough to make possible a fourfold
concentration of whey at 30 C without a strong
10
Ca-phosphate fouling.
The permeate flux (Figure 3) at pH 6.0 was 0
less than the calculated permeate flux (curve l Z 3 4 5
~ i , ~ concentration ratio
B); probably fouling is not avoided completely.
0 14 .8 1.2 1.6 2.0 2.4 2.8
However, the permeate flux at pH 4.6 was osmotic pressure (MPa)
considerably lower than curve B. This effect Figure 3. Permeate flux versus osmotic pressure of
should probably be attributed to the effect of the bulk liquid (concentration ratio) for Re of whey
pH on the behavior of the whey protein (9, 14). at various pH-levels. T = 30 C, P = 4 MPa, v = 2 m/s.
In the neighborhood of the iso-electric point, Curve B was calculated according to Appendix A
assuming only concentration polarization (no foul-
the protein has a low electrical charge. Under ing). • Gouda cheese whey pH = 6.6, DGouda cheese
these conditions aggregation takes place easily whey acidified to pH = 6.0, and o Gouda cheese whey
and accumulation of protein at the membrane acidified to pH = 4.6.

Journal of Dairy Science Vol. 63, No. 2, 1980

 REVERSE OSMOSIS OF DAIRY LIQUIDS 209

a range o f e x p e r i m e n t s with skim milk and ratios R f increases. For 2 × c o n c e n t r a t e d skim

whey, R f and Rp were calculated. In Figure 4
t h e e f f e c t o f the flow velocity on R f and Rp is
given. The main trend is a decrease of Rp and
R f with an increase of the f l o w velocity. F o r
w h e y (2× c o n c e n t r a t e d ) at 10 C, an R f (curve
A) of a b o u t .8 TPa.s/m is f o u n d at a f l o w
velocity of 1 m/s; this is a b o u t 1.7 × the
m e m b r a n e resistance R m at 10 C. At a flow
velocity of 2 m/s, R f has decreased to about
1/5 o f R m . As in Figure 4, a further increase in
flow velocity does not diminish R f to any
extent. F r o m Figure 4 we see t h a t for skim
milk R f is o f m u c h m o r e i m p o r t a n c e than for
whey. Again d e p e n d e n c e of R f on flow velocity
is strong. At 30 C R f for t w o f o l d c o n c e n t r a t e d
skim milk b e c o m e s less t h a n R m at a flow
velocity o f about 2.4 m/s. An increase in flow
velocity o v e r 2.6 m/s m a y have o n l y a marginal
effect. Also presented is R f for a c o n c e n t r a t i o n
ratio of 1.5 and 3. At higher c o n c e n t r a t i o n
resistance (TPa. s/ml
c\
3.5
3.0
2.5 3.0x
20
. B \ \\\ ~+.
milk, Rf at 10 C is m u c h higher than at 30 C; at
a flow v e l o c i t y o f 2.6 m / s we still have an Rf
o f a b o u t 1.0 TPa.s/m, which is m o r e t h a n twice
R m at 10 C. To reach reasonably small Rf at 10
C, m u c h higher flow velocities should be used.
The effect o f f l o w velocity on c o n c e n t r a t i o n
polarization, expressed as Rp, also is in Figure
4. Curve D represents Rp for w h e y at 10 C and
skim milk at 30 C (both t w o f o l d c o n c e n t r a t e d ) .
The Rp is in b o t h cases a b o u t the same since
the p e r m e a t e fluxes are at the same level. The
Rp are considerably less than R f and Rm. It can
be c o n c l u d e d that high flow velocities are n o t
necessary for reducing Rp b u t are particularly
so for reducing Rf.
Lim et al. (15) evaluated Rp and R f for RO
of cottage cheese whey, and c a m e to similar
conclusions a b o u t the e f f e c t o f flow rate on Rp
and Rf. F r o m e x p e r i m e n t s at flow velocities be-
tween 15 and 50 cm/s, t h e y c o n c l u d e d that R f
w o u l d b e c o m e negligible at a b o u t 1 m/s. Since
t h e y had to d e t e r m i n e this by e x t r a p o l a t i o n , it
is understandable that this figure cannot be
accurate.
For skim milk the effect o f the flow v e l o c i t y
on R f and, thus, on the p e r m e a t e flux is stronger
than for whey. Since Rp is small c o m p a r e d with
Rf, it may be assumed that R f is the main
governing factor for the p e r m e a t e flux. If so,
the situation is similar to that e n c o u n t e r e d for
U F . F r o m theoretical considerations o f UF (19)
1 . 1 .
the p e r m e a t e flux J v or -Rf - (since J v a ,Rf - - ) .Is
p r o p o r t i o n a l to the mass transfer coefficient K,

1.5
20
.x? \ \ \ \ \ ~. which is for t u r b u l e n t flow in tubes propor-
tional to Re.8 (see A p p e n d i x A). However, for
1,5x
UF often the effect of flow velocity is m u c h
ON \\ \
1.0 A\ \ \ " greater than when calculated according to this
relationship (17, 19). An evaluation o f our
.5 .._R_mat 10 C ~-x \ "°~.~'~. results with skim milk and of the results of
Rmat30 C ~ \"-,..'~-~''---,- Skudder et al. (27) showed a p r o p o r t i o n a l i t y to
o ~, -,----~---, ......... -,----:==:=-
- ---T-~ Re 1-3. Due to the relatively narrow range o f
.5 1.0 1.5 2.0 2.5 variation in flow velocity this is not accurate,
flow rate qmls) but it emphasizes the similarity b e t w e e n RO of
Figure 4. Various resistances to water permeation skim milk and U F of protein solutions. In both
as a function of the flow velocity. A) Fouling resist- situations a protein layer is f o r m e d on the
ance (Rf) for whey, 2X concentrated, T = 10 C, P =
membrane.
4 MPa; B) Fouling resistance (Rf) for skim milk, 1.5,
2.0, and 3.0X concentrated, T = 30 C, P = 3.5 MPa;
C) Fouling resistance (Rf) for skim milk, 2X concen- Effect of Pressure
trated, T = 10 C, P = 3.5 MPa; and D) Resistance due Particularly for RO of skim milk applied
to concentration polarization (Rp), o for whey 2×
pressure is a critical factor. Skudder et al. (27)
concentrated, T = 10 C, P = 4 MPa, a for skim milk,
2X concentrated, T = 30 C, P = 3.5 MPa (1 TPa.s/m = p e r f o r m e d a range o f e x p e r i m e n t s b e t w e e n 2.4
1012 Pa.s/m). and 4.1 MPa and f o u n d that the p e r m e a t e flux

Journal of Dairy Science Vol. 63, No. 2, 1980

210 HIDDINK ET AL.

passed t h r o u g h a m a x i m u m in this region. decrease a t pressures a b o v e 4 MPa. In Figure 6

W e carried o u t a similar r a n g e o f e x p e r i m e n t s in t h e p u r e w a t e r f l u x also is p r e s e n t e d , a n d t h e
w h i c h t h e applied pressures were varied f r o m p e r m e a t e f l u x w h i c h c o u l d be e x p e c t e d if o n l y
2.5 to 4.5 MPa at 10 C a n d 30 C. F r o m t h e t h e o s m o t i c pressure were t a k e n i n t o a c c o u n t
p e r m e a t e fluxes t h e f o u l i n g resistance R f was (curve B) a n d t h e p e r m e a t e f l u x if t h e e f f e c t o f
c a l c u l a t e d . In Figure 5, R f is p r e s e n t e d as a c o n c e n t r a t i o n p o l a r i z a t i o n were also c o n s i d e r e d
f u n c t i o n o f t h e a p p l i e d pressure. A t 10 C (curve C). T h e p h e n o m e n o n t h a t t h e p e r m e a t e
( c o n c e n t r a t i o n ratio 1.5:1 a n d 2 : 1 ) R f a t 2.5 f l u x is i n d e p e n d e n t o f t h e applied pressure
MPa are c o n s i d e r a b l y l o w e r t h a n R m . F u r t h e r - a b o v e 3 MPa s h o u l d , a c c o r d i n g t o o u r calcula-
m o r e , linear increase o f R f w i t h pressure is tions, b e a t t r i b u t e d t o increasing f o u l i n g
strong. A t 30 C a n d a t a p r e s s u r e o f 2.5 MPa, resistance. A t a p r o c e s s t e m p e r a t u r e o f 10 C
R f a g a i n are small, a n d a b o v e 3 MPa increase o f t h i s e f f e c t is even m o r e s e r i o u s t h a n at 30 C, a
R f w i t h pressure is a l m o s t p r o p o r t i o n a l . Also, c o n s t a n t p e r m e a t e flux over t h e w h o l e p r e s s u r e
R f d e p e n d s o n t h e c o n c e n t r a t i o n ratio (Figure range in this case.
5); t h e h i g h e r t h e c o n c e n t r a t i o n r a t i o t h e h i g h e r T h e r e s p o n s e o f t h e p e r m e a t e f l u x to p r e s s u r e
t h e Rf. This e f f e c t is m o r e p r o n o u n c e d at v a r i a t i o n s can be u n d e r s t o o d as follows. In a
10 C t h a n at 30 C. s t e a d y s t a t e s i t u a t i o n as m u c h s o l u t e ( i n c l u d i n g
In Figure 6 t h e p e r m e a t e flux for skim m i l k p r o t e i n ) is m o v e d b a c k i n t o t h e b u l k liquid -
at a c o n c e n t r a t i o n ratio 1.5:1 is p l o t t e d versus b y d i f f u s i o n a n d t u r b u l e n c e - as is b r o u g h t to
t h e a p p l i e d pressure. T h e a c t u a l p e r m e a t e flux t h e m e m b r a n e surface u n d e r t h e i n f l u e n c e o f
increased to a pressure o f a b o u t 3.0 MPa, a n d p e r m e a t i o n t h r o u g h t h e m e m b r a n e . T h e trans-
for h i g h e r pressures a c o n s t a n t p e r m e a t e p o r t b a c k i n t o t h e b u l k is g o v e r n e d b y t h e mass
flux was r e a c h e d , w i t h a slight t e n d e n c y to t r a n s f e r c o e f f i c i e n t w h i c h again is d e t e r m i n e d
b y t h e flow velocity. If at a c o n s t a n t flow
v e l o c i t y a h i g h e r pressure is applied, d u e to an
initial higher p e r m e a t e flux, t h e t h i c k n e s s o f
foulin( resistance (TPa.s/m) t h e fouling layer increases, w h i l e at t h e same
time a certain compaction of the deposit may
1.4 9/ A t a k e place. T h e s e e f f e c t s will r e s u l t in a h i g h e r
/
/
/
1.2 //
//
/ permeate flux (l/m 2. h)
l.O 2/ .- A
//
/
/
.8 //
/ +,.- B
/ /
9/ /
.6 / / //
Rmat]O
---
C /
/ /+"
/
.4 - // / . ..,..~/ C
Rm at // +// /
tO // / " o x- D
-;0-c , E

2.5 3.0 3.5 4.0 4.5

applied pressure (NtPa) 0 /~ 2.5
~ ~
3.0 a
3.5 i
40 i
45
Figure 5. Fouling resistance as a function of the pressure (/VlPa)
applied pressure for RO of skim milk at a flow velocity Figure 6. Permeate flux as a function of the applied
of 2.6 m/s. A) T = 10 C, concentration ratio 2.0:1; pressure for RO of skim milk (1.5X concentrated) at
B) T = 10 C, concentration ratio 1.5:1; C) T = 30 C, T = 30 C, v = 2.6 m/s. A) pure water flux; B) permeate
concentration ratio 2.0:1; D) T = 30 C, concentra- flux to be expected without concentration polariza-
tion ratio 1.5:1; and E) T = 30 C, concentration tion and fouling; C) permeate flux to be expected
ratio 1.05:1 (1 TPa.s/m = 1012 Pa.s/m). without fouling; and D) actual permeate flux.

Journal of Dairy Science Vol. 63, No. 2, 1980

 REVERSE OSMOSIS OF DAIRY LIQUIDS
Rf, and this process continues until such a high
R f is built up t h a t equilibrium exists again
b e t w e e n the a m o u n t o f solute transported to
and f r o m the m e m b r a n e surface. Ultimately
this results in an unchanged p e r m e a t e flux. The
slight decrease in p e r m e a t e flux at higher
pressures can be explained by a m o r e serious
c o m p a c t i o n o f the fouling layer. Skudder et al.
(27) report that the position o f the m a x i m u m
in p e r m e a t e flux d e p e n d s b o t h on f l o w velocity
and t e m p e r a t u r e . The higher the f l o w velocity
and t e m p e r a t u r e , the lower the R f and the
higher the o p t i m u m pressure.
In our e x p e r i m e n t s with w h e y an effect of
pressure on p e r m e a t e flux was similar but only
at pressures above 4.5 MPa. Such an effect for
w h e y also was f o u n d by D o n n e l l y et al. (5).
The l o w protein c o n t e n t o f w h e y and the
high diffusion coefficient for w h e y protein
c o m p a r e d to casein m a y m e a n that for w h e y at
higher pressures o n l y (i.e., higher p e r m e a t e
fluxes) a considerable fouling resistance is built.
Structure of Fouling Layer
Lim et al. (15) distinguished within the
fouling layer ( e x p e r i m e n t s with cottage cheese
whey), a cake layer which should be a c o m p a c t
layer " a t t a c h e d " to the m e m b r a n e surface, and
a viscous layer b e t w e e n the cake layer and the
circulating bulk. The characteristic difference
b e t w e e n those t w o layers is that the viscous
layer is removed by rinsing with water while the
cake layer remains a t t a c h e d to the m e m b r a n e .
In our e x p e r i m e n t s with skim milk there was
also a proteinaceous fouling layer as for Lim et
al. (15). This layer was divided into a cake layer
and a viscous layer (see A p p e n d i x B). In Table
TABLE 2. Distribution of the fouling resistance over a viscous layer and a cake layer for RO of skim milk.
Rcake = fouling resistance a f t e r w a t e r rinsing. Rviscou s = Rf - Rcake. (1 TPa.s/m) = 1012 Pa.s/m).
Rviscous (TPa.s/m)
1.05 2.0
P = 2.5 MPa v = 2.6 m/s .01 .01
P = 3.5 MPa v = 1 . 4 m/s .16 .88
v = 2.0 m/s .12 .29
v = 2.6 m/s .05 .10
P = 4.5 MPa v = 2.6 m/s .07 .22
211
2 the results of our e x p e r i m e n t s are given. F o r
b o t h layers a fairly strong d e p e n d e n c e on
c o n c e n t r a t i o n ratio, pressure, and flow v e l o c i t y
was f o u n d , which makes it d o u b t f u l that there
was a characteristic difference b e t w e e n t h e t w o
layers. We think it is m o r e useful to consider
the fouling layer as a whole and to distinguish
within the fouling layer a certain gradient in
c o n c e n t r a t i o n and firmness. This m o d e l agrees
with that for c o n v e n t i o n a l filtration with a
p o r o s i t y gradient (30). The effects in Table 2
can be u n d e r s t o o d as follows. The higher the
f l o w velocity (shear rate), the m o r e will be
scraped o f f o f the fouling layer and the lower
the remaining fouling resistance after water
rinsing. High pressures will cause a greater
c o m p a c t i o n of the fouling layer, which again
causes a firmer and m o r e fouling resistance
after water rinsing.
CONCLUSIONS
For reverse osmosis of dairy liquids, b o t h
the c o m p o s i t i o n o f the feed and process condi-
tions have an i m p o r t a n t effect on p e r m e a t e
flux. F l u x limiting factors include o s m o t i c
pressure and fouling tendency. F o r G o u d a
whey, processed at 30 C, fouling o f the m e m -
branes due to Ca-phosphate precipitation is an
i m p o r t a n t factor, while for skim milk, desalted
w h e y , and acid whey, protein is the i m p o r t a n t
fouling agent. Fouling by G o u d a w h e y can be
limited by decreasing the p H or by decalcifying
the whey.
F u r t h e r m o r e , it is possible, by p r o p e r
process conditions in which the flow v e l o c i t y
plays an i m p o r t a n t role, to decrease the resist-
ance due to fouling and c o n c e n t r a t i o n polariza-
Rcake (TPa.s/m)
Concentration ratio
3.0 1.05 2.0 3.0
. . . . 02 .03 ...
. . . . 63 .66 ...
.54 .18 .21 .24
.24 .04 .07 .09
. . . . 13 .20 ...
Journal of Dairy Science Vol. 63, No. 2, 1980
212
tion considerably below the resistance of the
membrane. An important step needed to reach
a h i g h e r p e r m e a t e f l u x is t h e d e v e l o p m e n t o f
membranes with higher water permeabilities
and resistance to high temperatures.
REFERENCES
1 Brule, G., E. Real del Sol, J. Fauquant, and C.
Fiand. 1978. Mineral salts stability in a q u e o u s
phase o f milk: Influence o f heat treatments. J.
Dairy Sci. 61:1225.
2 de Boer, R., J. N. de Wit, and J. Hiddink. 1977.
Processing of whey by m e a n s o f m e m b r a n e s and
applications o f whey protein concentrate. J. Soc.
Dairy Technol. 30:112.
3 Dejmek, P. 1975. Permeability o f the concentra-
tion polarization layer in ultrafiltration o f macro-
molecules. Page A2.26 in Separation processes by
m e m b r a n e s , ion exchange and freeze-concentration
in food industry. A.P.RA.A., Paris.
4 D e l a n e y , R.A.M., and J. K. Donnelly. 1977.
Applications o f reverse osmosis in the dairy indus-
try. Page 417 in Reverse osmosis and synthetic
m e m b r a n e s . S. Sourirajan, ed. Nat. Res. Counc.
Can., Ottawa.
5 Donnelly, J.K., A. C. O'Sullivan, and R.A.M.
Delaney. 1974. Reverse osmosis-concentration
applications. J. Soc. Dairy Technol. 27:128.
6 Eriksson, P. 1977. Concentration of whey by
reverse osmosis-inventory and operating experi-
ences. Nordeuropaeisk Mejeritidsskrift. 43 : 238.
7 Evans, E. W., and F. A. Glover. 1974. Basic prin-
ciples of reverse osmosis and ultrafiltration. J. Soc.
Dairy Technol. 27:111.
8 Fenton May, R. I., C. G. Hill, C. H. A m u n d s o n , M.
H. Lopez, and P. D. Auclair. 1972. Concentration
and fractionation of skim milk by reverse osmosis
and ultrafiltration. J. Dairy Sci. 55 : 1561.
9 Forbes, F. 1972. Considerations in the optimisation
of ultrafiltration. Chem. Eng.:21.
10 Glover, F. A., and B. E. Brooker. 1974. The
structure of the deposit formed on the m e m b r a n e
during the concentration of milk by reverse osmo-
sis. J. Dairy Res. 41:89.
11 Glover, F. A., P. J. Skudder, P. H. Stothart, and E.
W. Evans. 1978. Reviews of the progress of dairy
science: reverse osmosis and ultrafiltration in dairy-
ing. J. Dairy Res. 45:291.
12 Hayes, J. F., J. A. Dunkerley, and L. L. Muller.
1974. Studies on whey processing by ultrafiltration.
Austr. J. Dairy Technol. 29:132.
13 J o h n s t o n , A. N. 1977. How European cheese
APPENDIX A
Calculation of Concentra-
tion Polarization
The permeate (water) flux through a reverse
osmosis membrane is u s u a l l y d e s c r i b e d , in a
Journal of Dairy Science Vol. 63, No. 2, 1980
HIDDINK ET AL.
plants save costs in w h e y processing t h r o u g h
reverse osmosis system. Dairy and Ice Cream Field
160:1160.
14 Lee, N. D., and R. L. Merson. 1976. Chemical
t r e a t m e n t s o f cottage cheese w h e y to reduce
fouling of ultrafiltration m e m b r a n e s . J. Food Sci.
41:778.
15 Lim, T. H., W. L. Dunkley, and R. L. Merson.
1971. Role of protein in reverse osmosis o f cottage
cheese whey. J. Dairy Sci. 54: 306.
16 Mehta, B. 1973. Processing o f model compositional
whey solutions with pressure driven membranes.
Ph.D. thesis, The Ohio State University, Columbus.
17 Muller, L. L. 1976. Whey utilization in Australia.
Australian J. Dairy Technol. 31 : 92.
18 Peri, C., and W. L. Dunkley. 1971. Reverse osmosis
of cottage cheese whey. 1. Influence o f composition
o f the feed. J. Food Sci. 36:25.
19 Porter, M. C. 1972. Concentration polarization
with m e m b r a n e ultrafiltration. Ind. Eng. Chem.
Prod. Res. Develop. 11 : 234.
20 Pyne, G. T. I 9 6 2 . Reviews o f the progress o f dairy
science. Some aspects o f the physical chemistry of
the salts o f milk. J. Dairy Res. 29:101.
21 Reid, C. E. 1972. Principles of reverse osmosis.
Page 109 in Industrial processing with membranes.
R. E. Lacey and S. Loeb, ed. Wiley-Interscience,
New York.
22 Roger, R., J. L. T h a p o n , J. L. Maubois, and G.
Brule. 1976. Hydrnlyse du lactose c o n t e n u dans
l'ultrafiltrat de lair ou de lactosdrum en r~acteur
e n z y m a t i q u e ~ m e m b r a n e . Le Lait 5 5 1 - 5 5 2 : 5 6 .
23 Rose, D., and H. Tessier. 1959. Composition of
ultrafiltrates from milk heated at 80 to 230 F in
relation to heat stability. J. Dairy Sci. 42:969.
24 Schoorl, N. 1929. Suiker titratie. Chem. Weekblad
26:130.
25 Short, J. L., and R. K. Doughty. 1976. An evalua-
tion of m o d u l e s and m e m b r a n e s for the concentra-
tion of cheddar cheese whey by reverse osmosis.
New Zealand J. Dairy Sci. Technol. 11 : 237.
26 Short, J. L., and I. R. Hughes. 1978. The concen-
tration of separated milk by reverse osmosis. New
Zealand J. Dairy Sci. Technol. 13:114.
27 Skudder, P. J., F. A. Glover, and M. L. Green.
1977. An e x a m i n a t i o n of the factors affecting the
reverse osmosis o f milk with special reference to
deposit formation. J. Dairy Res. 44: 293.
28 Smith, B. R., and R. D. Macbean. 1978. Fouling in
reverse osmosis. Australian J. Dairy Technol.
33:57.
29 Sourirajan, S. 1970. Reverse osmosis. Academic
Press, New York.
30 Tiller, F. M., and J. R. Crump. 1977. Solid liquid
separation: An overview. Chem. Eng. Progr. 73:65.
somewhat simplified form, by the following
equation:
Jv = (AP- ATrw)/Rm [11
where
 REVERSE OSMOSIS OF DAIRY LIQUIDS
Jv flux through m e m b r a n e ( l / m 2 . h ) or
--
(m/s)
AP= hydrostatic pressure difference across
the m e m b r a n e (Pa)
ATrw = o s m o t i c pressure difference across the
m e m b r a n e (Pa)
R m = resistance to water p e r m e a t i o n o f the
m e m b r a n e (Pa.s/m)
If restricted to high rejection membranes,
the o s m o t i c pressure at the p e r m e a t e side m a y
be neglected; then &Trw equals Zrw, which is the
osmotic pressure at the m e m b r a n e surface at
retentate side. As a result of the rejection of the
solutes by the m e m b r a n e , at the m e m b r a n e sur-
face a local c o n c e n t r a t i o n (and local o s m o t i c
pressure) is found which is higher than in the
bulk of the solution. This c o n c e n t r a t i o n polari-
zation is c o u n t e r a c t e d by diffusion of solutes
back into the bulk, by t u r b u l e n t eddies, and by
shearing of the fluid near the m e m b r a n e . At
equilibrium the transport o f solutes back into
the bulk occurs as fast as solutes are brought up
to the m e m b r a n e . A t equilibrium the concen-
tration o f solutes ( o s m o t i c pressure) at the
m e m b r a n e surface is given by (7, 19):
C w / C b = Ztw/~ b = exp (Jv/k) [2]
where
CW =c o n c e n t r a t i o n o f solutes at the m e m -
brane surface (kg/kg)
C b = c o n c e n t r a t i o n of solutes in the bulk
(kg/kg)
Ti'b = o s m o t i c pressure in the bulk (Pa)
k= mass transfer c o e f f i c i e n t (m/s)
It is assumed that the o s m o t i c pressure is directly
p r o p o r t i o n a l to the solute concentration. A
c o m b i n a t i o n of equations [1] and [2] results
in:
Jv = (AP - 7rw)/Rm
[3]
= (& P / R m ) - ( z r b / R m ) exp (Jv/k)
If k is k n o w n , the p e r m e a t e flux J v can be calcu-
lated. F o r a calculation o f k, for t u r b u l e n t flow
in tubes, generally the following dimensionless
correlation is used (19):
Sh = .023 Re.8 Sc.33 [41
213
where
Sh = kd/ID ( S h e r w o o d n u m b e r )
Re = dv//) ( R e y n o l d s n u m b e r )
Sc = u/ID ( S c h m i d t n u m b e r )
and
d = d i a m e t e r of the t u b e (m)
v = f l o w velocity in the t u b e (m/s)
ID = diffusion coefficient (m2/s)
v = kinematic viscosity (m2/s)
For the calculation of k, e q u a t i o n (4) can be
written as:
k = .023 ID '67 v ' 8 / ( d "2 /).47) [5]
Equation [31 was evaluated for the liquids
referred to in Table 1. For such an evaluation
the physical properties o f the liquids m u s t be
k n o w n . The viscosity and o s m o t i c pressure
were d e t e r m i n e d e x p e r i m e n t a l l y , the values o f
the diffusion coefficient were taken f r o m the
literature (Table A.1). In our calculations con-
cerning c o n c e n t r a t i o n polarization, we o n l y
a c c o u n t e d for those c o m p o n e n t s which are
contributing to the o s m o t i c pressure (i.e.,
lactose and salts). Since lactose and salts have
different diffusion coefficients and, thus,
different k-values, e q u a t i o n [31 was e x t e n d e d
to two c o m p o n e n t s as follows:
Jv = (AP/Rm) - (/Tbl/RM)'exp (Jv/kl)
[6]
- ( r r b 2 / R m ) - e x p (Jv/k2)
It appeared that an evaluation o f e q u a t i o n [3]
resulted in a p e r m e a t e flux versus o s m o t i c
pressure of the bulk liquid which nearly coin-
cides for w h e y , U F - p e r m e a t e , and lactose, see
curve B in Figure 1. The variations were less
than 1 liter/m 2.h. This can be u n d e r s t o o d f r o m
the fact that the mass transfer c o e f f i c i e n t k
for these liquids is about equal which again is
caused by t h e fact that the process c o n d i t i o n s
are the same and the viscosity, density and diffu-
sion coefficients do not differ much. The calcu-
lated p e r m e a t e flux for skim milk tends to be
s o m e w h a t lower (.5 to 2.0 l i t e r / m 2 . h ) than
curve B in Figure 1. This can be u n d e r s t o o d
f r o m the higher viscosity o f skim milk.
Journal of Dairy Science Vol. 63, No. 2, 1980
214 HIDD1NK ET AL.

TABLE A . I . Solute-water diffusion coefficients for some components of milk at 20 C.

Diffusion
coefficient (m2/s) Reference

Lactose 5% 3.8 × 10-10 (4)

Ash(KCI.74%) 18.4 X 10 -1° (29)
Whey protein (/3-1actoglobulin 1%) .64 X 10 -10 (4)
Casein 3% .19 × 10 -1° (4)

APPENDIX B Jv = (AP - rrw)/(Rm + Rf) [71

Evaluation of Resistance due to
Fouling and
Concentration Polari- Next the c o n c e n t r a t i o n polarization resistance
zation from the Experiments Rp can be calculated f r o m the following equa-
tion:
Strictly speaking, c o n c e n t r a t i o n polarization
reduces the driving force. However, the effect
Jv = (AP - "trb)/(Rm + Rf + Rp)
of c o n c e n t r a t i o n polarization o f t e n is translated
into an additional resistance to p e r m e a t i o n o f
To divide the fouling resistance (Rf) in a re-
the m e m b r a n e , when the original driving force
sistance of a cake layer (Rcake) and the
is considered. However, a fouling layer on the
resistance of a viscous layer (Rviscou s) the
m e m b r a n e m a y cause a real additional hydraulic
following procedure was followed. The bulk
resistance acting in series with the m e m b r a n e
liquid was r e m o v e d by water; then the pure
resistance (28).
water flux was measured under the same
The m e m b r a n e resistance R m can be deter-
c o n d i t i o n as previously used for t h e liquid.
mined f r o m the pure water flux for the clean
F r o m this pure water flux Jw, Rcake was
membrane.
calculated according:
F r o m the e x p e r i m e n t a l p e r m e a t e flux for
the liquid concerned, after an evaluation of the
mass transfer coefficient k, the c o n c e n t r a t i o n J w = A P / ( R m + Rcake ) [8]
polarization modules Cw/Cb = rrw/Zrb can be
calculated f r o m A p p e n d i x A, e q u a t i o n [21. N e x t Rviscuu s can be calculated f r o m :
If k n o w n nw the value of the fouling resist-
ance R f can be calculated since Rviscou s = R f - Rcake [9]

Journal of Dairy Science Vol. 63, No. 2, 1980