27

Membrane Separation and Design

Rohit Ruhal and Bijan Choudhury

Introduction

In recent years, the use of membranes in the food processing industry has become
widespread, with major applications reported in the dairy and beverage industries. In
the 1960s, the dairy industry was the first to implement membrane technology and
the development of newer membrane materials and design has resulted in wider uti-
lization of membranes in this sector. Concentration and fractionation are two major
areas of interest to the membrane specialist in the dairy industry (Daufin et al., 1998).
The use of membranes in the dairy industry has resulted in better-quality products
with minimum waste generation. In the case of concentration, membrane separation
processes replaced thermal processes, resulting in energy efficiency. Similarly, frac-
tionation with membranes resulted in minimum waste generation and recycling of
byproduct. A major motivation for the acceptance of membrane processes in the food
processing industry is their energy efficiency, retention of food quality, and minimum
waste generation (Bruschke, 1995). In recent years it has been reported that mem-
branes can also be used for cold sterilization of liquid food materials, with improved
shelf-life and retention of flavor and nutrients. Membrane technology has also been
more openly accepted in the beverage industry and has improved the quality of product
along with better economics (Memtec Ltd, 1998). Some of the current examples

Handbook of Food Process Design, First Edition. Edited by Jasim Ahmed and Mohammad Shafiur Rahman.
© 2012 Blackwell Publishing Ltd. Published 2012 by Blackwell Publishing Ltd.
770 Handbook of Food Process Design: Volume II

include water desalination and purification and cold sterilization of beverages; recov-
ery and fractionation of proteins from whey; clarification of fruit juice, wines and beer;
removal of bacteria from water; effluent treatment for removal of heavy metals and
organic materials; separation of oil and water emulsions; and removal of volatile
organic compounds from air.
Membrane technology can be subdivided into four different processes depending on
the size of membrane pore: microfiltration, ultrafiltration, reverse osmosis, and nano-
filtration. Microfiltration is generally used for separation of macromolecules and
particles that range in size from 1 to 10 μm. Ultrafiltration separates macromolecules
by molecular mass, generally from 5 to 500 kDa. A membrane with a cut-off of 5 kDa
can retain 90% of macromolecules with molecular mass of 5 kDa. Ultrafiltration finds
wider application in whey protein concentration and fractionation, while reverse
osmosis finds application in the desalination of water. Nanofiltration is a recent addi-
tion to membrane technology and its area of application lies between that of ultrafil-
tration and reverse osmosis.
The material comprising the membrane plays an important role and today com-
mercial membranes are mostly made of polymers or inorganic material. Although
inorganic membranes have the advantage of strength and steam sterilizability, their
cost plays an important role in their suitability in commercial processes. A number
of membrane modules are used in the commercial food processing industry: hollow-
fiber module, spiral wound module, plate and frame module, and tubular module.
Among these, the spiral wound module has the highest specific area per unit volume
but has limited application with a solution containing suspended particles. In the
process flow-sheet, any membrane module can be adapted without much difficulty
and the requirement for less sophisticated control also favors easy replacement of
traditional separation with membrane technology. However, the phenomenon of con-
centration polarization (see section Microfiltration) results in low acceptability of
membrane technology in continuous processes. Thus design parameters have a huge
influence on the successful implementation of membrane processes in the commercial
food processing industry. This chapter discusses the issues involved in the design and
implementation of membrane technology in food processing operations.

Process Flow-sheet for Membrane Operation

A membrane process can be represented by the flow-sheet shown in Figure 27.1. In

commercial membrane processes, permeate or retentate can be a product and, depend-
ing on the requirement, the operation flow-sheet needs to be modified. In most com-
mercial processes, tangential filtration is carried out, where flow of liquid is parallel
to the membrane surface. To improve the filtration rate, high cross-flow velocity is
maintained and this results in reduced thickness of the concentration polarization
layer, which limits flux through the membrane.
 Membrane Separation and Design 771

Feed (C, nf )

( p, np )
Permeate (C

Retentate (Cr , nr )

Figure 27.1 Process flow-sheet for membrane separation process.

Material Balance
If a protein is concentrated in a membrane having feed concentration C in a batch
operation, then we can write:

vr + v p = vf (27.1)

Cr v r + Cp v p = Cv f (27.2)

where νr is volumetric flow rate of retentate (m3·s−1), νp volumetric flow rate of perme-
ate (m3·s−1), ν volumetric flow rate of feed (m3·s−1), Cr concentration of protein in
retentate (g·L−1), Cp concentration in permeate (g·L−1), and C concentration of protein
in solution (g·L−1). Now if we define concentration factor (Fc) and recovery factor (Q)
as follows:

Fc = Cr C (27.3)

Q = vP vF (27.4)

then we can write

1 ⎡ CpQ ⎤
Fc = 1−
1 − Q ⎢⎣ C ⎥⎦

which correlates concentration factor and recovery factor. Depending on the desired
concentration, the process can be shut down at any point. However, due to the
772 Handbook of Food Process Design: Volume II

formation of the concentration polarization layer, there is a limit on the achievable

final concentration of protein. In the case of a semi-continuous process, part of the
retentate can be recycled to maintain a pseudo-steady flux across the membrane.

Basic Theoretical Principle, Membrane Operation Mode and

Membrane Materials

Transmembrane pressure is the major driving force for the movement of solution
across a membrane. Because of its larger size, the solute is retained by the membrane;
as the process continues, the concentration of solute increases and this mass of solute
is deposited on the membrane. Therefore there is a concentration gradient on the feed
side of the membrane, with maximum concentration at the membrane surface. This
build-up of solute cake (in membrane filtration) or solute layer (in ultrafiltration)
results in higher membrane resistance and thus decline in permeate flux across the
membrane. The flow of liquid is tangential to the membrane surface, and this flow
attempts to reduce the thickness of the cake. However, the increase in solute concen-
tration may also increase viscosity, which may affect transmembrane flux. Even if a
pseudo-steady state is achieved, operation may not continue for long as there is a pos-
sibility of irreversible fouling of the membrane and eventual shutdown of the opera-
tion. Further cleaning and back-flushing of the membrane may result in restoration
of the original flux. For solutes that are soluble, the concentration adjacent to the
surface may reach the level of insolubility and precipitation of solute may result in
higher membrane resistance and decline in permeate flux. In recent years, efforts have
been made to reduce fouling by optimizing process parameters, design parameters, and
membrane materials.
Diffusion-based membrane processes include diafiltration and pervaporation, where
concentration difference across the membrane is the driving force. Membrane separa-
tion is generally operated in batch or continuous modes. In batch mode, the volume
of solution decreases and concentration of solute increases with time. However, there
is an upper limit on the maximum concentration of solute achievable with membrane
concentration processes. In batch mode, steady state is never achieved and this mode
of operation is suitable for smaller-scale filtration. In continuous mode, the concentra-
tion of solute in retentate remains constant. This mode of operation is suitable for
large-scale membrane separation processes. In other modes of operation, bleeding of
retentate is carried out to maintain a constant level of solute concentration in the
feed. By maintaining a constant concentration, steady-state flux can be achieved at a
constant transmembrane pressure. Commercially, batch mode is more adaptable on
the process flow sheet.
Membrane materials include natural polymers like cellulose acetate, synthetic
polymer membranes, and composite or ceramic membranes. The first commercial
membranes used in reverse osmosis and ultrafiltration were composed of cellulose
acetate, which provides high permeate flux and is easy to manufacture but with the
 Membrane Separation and Design 773

disadvantages that it breaks down at high temperature and is sensitive to chemicals.

Recently, polymer membranes made from polyamide, polyacrylonitrile, nylon, and
polysulfones have been used, especially in ultrafiltration, and these have better
chemical resistance. Ceramic or composite membranes made from carbon, zirconium
oxide, or alumina have the advantage of cleaning and sanitation due to their inert
nature.

Membrane Modules

Four membrane modules are generally used in industrial applications: tubular module,
hollow fiber module, spiral wound module, and plate and frame module.
Tubular membranes are located inside a tube (Figure 27.2). Tubular membranes have
a diameter of about 5–15 mm. Because of the size of the membrane surface, plugging
of tubular membranes is not likely. A drawback of tubular membranes is that the
packing density is low, which results in high capital cost per module. Ceramic mem-
branes are generally assembled in tubular modules. Some of the advantages of tubular
module are easy replacement of membrane and cleaning of membrane surface and no
need for any costly pretreatment of feed. Disadvantages of this module are high energy
cost per unit of liquid treated, low surface area per unit volume, and necessity of high
liquid flow rate to maintain turbulence in the module.
A hollow fiber module (Figure 27.3) consists of a large number of small-diameter
fibers sealed at the ends with epoxy resin, polyurethanes and silicone rubber.
Membranes are asymmetric in nature, the feed side having lower pore size, and are
self-supporting. They have very high specific area per unit volume compared with
tubular membranes, up to 30 000 m2·m−3. It is preferable to use hollow fiber modules
with clean solution, and thus are most used in gas separation or pervaporation. Hollow
fiber membranes have low diameter so the chances of plugging are very high.
Plate and frame modules (Figure 27.4) were initially used for commercial purposes
but their low specific area is unattractive. Plate and frame modules have been adapted
into a conventional filter press. In this module two membranes are sandwiched with

membranes

feed

Retentate

permeate

Figure 27.2 Tubular module. (From EPA Research & Development.)

774 Handbook of Food Process Design: Volume II

Permeate

Fast flush port

Hollow fibers

Flow direction

Feed

Figure 27.3 Hollow fiber module. (From EPA Research & Development.)

Figure 27.4 Plate and frame module. (From USEPA, 2005. Membrane Filtration Guidance Manual
(EPA 815-R-06-009). Office of Water.)

the feed sides facing each other. A spacer is placed between the feed and permeate
sides. To achieve the desired membrane area, a number of such sets are placed in
parallel. Membrane replacement and cleaning is easier and there is no need for costly
pretreatment of feed.
Spiral wound module (Figure 27.5) is an adaptation of plate and frame module, where
membrane sets are wrapped around a central line for collecting permeate. It has the
 Membrane Separation and Design 775

Figure 27.5 Spiral wound module. (From EPA Research & Development.)

advantages of compact structure with high pressure durability. It has the highest spe-
cific surface area among all the modules but feed needs to be free of particles.

Types of Membrane Process

A membrane is a selective barrier and this selectivity is important for separation (Reis
and Zydney, 2007). Various selectivity parameters such as diffusivity, shape, size,
electrostatic charge, physicochemical interactions, volatility, and solubility can be
used to influence product concentration and removal of solute from solvent (e.g desalt-
ing, fractionation, gas separation, pervaporation). Membrane materials include organic
polymers like polysulfone, polyether sulfone, cellulose acetate, polyamides, and poly-
acrylonitrile and inorganic material such as borosilicate glass, pyrolyzed carbon, and
zirconia carbon. The driving forces of membrane processes include concentration
gradient, transmembrane pressure, chemical potential, osmotic pressure, electric field,
magnetic field, and partial pressure. For ultrafiltration, microfiltration, and reverse
osmosis, membranes are classified on the basis of molecular size of pores and trans-
membrane pressure, whereas pervaporation is based on separation driven by partial
pressure and selectivity that depends on solubility and diffusivity of species in the
membrane.
776 Handbook of Food Process Design: Volume II

Reverse Osmosis

Reverse osmosis is essentially a pressure-driven membrane diffusion process for sepa-

rating dissolved solvents. During the process, feed solution at high pressure is passed
over the feed side of the membrane. The operating pressure is kept higher than the
osmotic pressure of the feed solution so that water will flow from the more concen-
trated solution to the more dilute solution through the membrane. Reverse osmosis
is used for desalination of seawater. The attractive features of the process are that
there is no no requirement of phase change and it is a relatively low-energy requiring
process. Normally, solvent (e.g. water) flows across a semipermeable membrane from
the dilute solution to the more concentrated solution until equilibrium is reached.
Thus applying high pressure at the high-concentration side will cause this process
to reverse. This application of high pressure at the feed side results in solvent migra-
tions from the concentrated solution, leaving a higher concentration of solute. In
process application, the waste stream containing salts flows past the membrane,
resulting in solvent permeation (e.g. water) through the membrane and the remaining
solutes (e.g. organic or inorganic components) get concentrated on the feed side of
the membrane.
Most reverse osmosis membranes are made of polymers like cellulose acetate, and
aromatic polyamides, and are rated at 96–99% NaCl rejection. These membranes are
generally of two types: asymmetric or skinned membranes and thin-film composite
membranes. The support material is commonly polysulfones, while the thin film is
made from various polyamines and polyurea. Reverse osmosis membranes have the
smallest pore structure, with pore diameter ranging from about 5 to 15 Å (0.5–1.5 nm).
The extremely small size of these pores allows only the smallest organic molecules
and uncharged solutes to pass through the semipermeable membrane along with
the water. Greater than 95–99% of inorganic salts and charged organics get rejected
due to the repulsion of similar charge present at the membrane surface at process
conditions.
The major advantage of reverse osmosis is requirement of low power for recovery
of salts and chemicals from process effluents. No latent heat of vaporization is involved
for affecting separations; the main energy requirement is a high-pressure pump. It also
requires low floor space (compact high-capacity units) as compared to traditional unit
operation. The major problem of reverse osmosis is susceptibility to fouling. This is
caused due to particulate and colloidal matter that is present at high concentration at
the feed side of the membrane surface. Fouling of membranes by soluble components
or colloids present in solution causes failures. Thus pretreatment is used to remove
particulate matter from the feed water. A system operating at a high permeate flux is
more likely to experience high fouling rates and thus require intermittent chemical
cleaning. Low operational temperature range is another limitation of reverse mem-
brane process. For cellulose acetate membranes, the temperature operation range is
18–30 °C; while lower temperatures result in decreased fluxes and higher temperatures
increase the rate of membrane hydrolysis. These membranes are not chemically inert.
 Membrane Separation and Design 777

Strongly acidic or basic solutions, strong oxidizing agents, solvents, and other organic
compounds should be avoided as these agents cause dissolution of the membrane.
Some concentrated solutions may have high initial osmotic pressures and these solu-
tions are economically unattractive for reverse osmosis process.

Ultrafiltration
Ultrafiltration is a membrane separation process that operates under a pressure gradi-
ent and it can fractionate components of a liquid with respect to their solvated size,
molecular weight, and structure. Even electrostatic charges play a role in fractionation
of solutes. Ultrafiltration membranes have a pore diameter of 0.01–0.1 mm and typi-
cally remove high-molecular-weight substances, colloidal materials, and organic and
inorganic polymeric molecules, whereas microfiltration membranes remove all bac-
teria and some viral contamination, even though viruses are smaller than the pores
of a microfiltration membrane (Bailey et al., 2000). This is because viruses can attach
themselves to bacterial bio film. Ultrafiltration membranes can also filter viruses.
Permeability generally depends on pore size but other factors like electrostatic charge
on membrane surface and solute also play a role. Ultrafiltration also depends on
applied pressure, nature of feed material, temperature of operation, feed concentration,
and flow rate of feed stream across the membrane.
Ultrafiltration membranes are produced from variety of synthetic polymers and
have high thermal stability and chemical resistivity but are unable to tolerate harsh
cleaning chemicals. Polyethersulfone is most preferably used as an ultrafiltration
membrane material as it has high rigidity, creep resistance, and good thermal and
dimensional stabilities. The choice of membrane is guided by molecular weight cut-
off, chemical and thermal resistance. However in recent times membrane surface
properties like hydrophilicity have also become important criteria for selection of
ultrafiltration membrane. Hollow fiber, flat sheet cassettes, spiral wound cartridges,
and tubular modules are generally used as the ultrafiltration module in the commer-
cial process. Some of the advanced techniques, especially for protein, use charged
ultrafiltration membranes, electro-ultra filtration, and ultrafiltration in the presence
of an ultrasonic field. Ultrafiltration is most suitable for concentrating protein in
whey, cheese-making process, reduction of salt concentration in process stream, and
fractionation of whey protein. Ultrafiltration membrane finds widespread application
in the dairy industry.

Microfiltration
Microfiltration is a technique that allows concentration of the liquid containing
insoluble particle, and the liquid passing through the filter is known as microfiltrate.
Pore diameter of microfiltration membrane ranges from 0.1 to 10 mm. Cross-flow
microfiltration is used for applications like removal of bacteria and micelle casein.
The material properties of the membrane determine its efficiency. Previously
778 Handbook of Food Process Design: Volume II

polysulfone and polycarbonate were used but their performances were not satisfactory.
Polyethersulfone is now the standard material of microfiltration membranes used in
biological applications. The pore size of commercially available microfiltration ceramic
membranes ranges from 0.1 to 20 mm. Ceramic membranes are most advantageous in
the dairy and food industry because of their strong mechanical resistance and wide
pH tolerance. The operation of microfiltration leads to a higher solute concentration
closer to the membrane surface than in the bulk feed stream; this phenomenon is
called concentration polarization and is caused by diffusive back flow of solute to the
bulk feed.
Microfiltration needs to be started with care as it can avoid rapid fouling. In the
dairy industry, microfiltration membranes are first filled with warm water and then
milk (Saboya and Maubois, 2000). Other dairy applications of microfiltration include
removal of microorganisms from milk to produce the sterilized raw material used to
prepare fluid milks, cheeses or long- storage dairy products. The reason for this cold
sterilization process is that milk collected from farms is contaminated with various
pathogenic bacteria.
Microfiltration offers an economically interesting alternative to heat treatment. In
microfiltration, skim milk heated to 50 °C is circulated at a velocity of 7.2 m·s−1 along
the membrane with uniform transmembrane pressure around 0.5 bar (0.05 MPa).
Another application is the selective separation of micellar casein and selective frac-
tionation of globular milk fat. Microfiltration is also used in microbial fermentation
(upstream and downstream processing of biomass) and concentration of other metabo-
lites in batch and continuous process operations.
Microfiltration is commonly used to recover macromolecules and retain suspended
colloidal particles and is being integrated into both upstream and downstream proc-
esses. Large numbers of MF applications are reported, including removal of small
molecules from bigger protein molecules, clarification of suspensions for cell harvest-
ing, and sterilization of heat sensitive liquids to remove viruses and bacteria (Saxena
et al., 2009). Another important role is protein separation and purification, for
example recovery of extracellular proteins from biomass. Other applications in the
food industry include processed meat, nutritional beverages, infant formulas and
dairy products.

Pervaporation
Liquid mixtures can be separated on nonporous polymer membranes by partial evapo-
ration. The procedure is called pervaporation because the substance crossing the
membrane changes phase state (Marriot et al., 2001). The substance encounters the
membrane as a liquid and leaves it as a vapor, vacuum pressure on the permeate side
causing the vapor to desorb. The membrane used in pervaporation can be hydrophilic
or organophilic depending on its composition and is generally nonporous. Pervaporation
is used in the wine industry because it can produce a more concentrated alcohol per-
 Membrane Separation and Design 779

meate and thus the wine becomes less dense compared to membrane filtration process
where only the consistency of the wine product changes slightly. In pervaporation,
temperature is a very important parameter and choice of optimum temperature is the
main goal for optimum process design. In comparison with other membranes, per-
vaporation has higher temperatures leading to higher flux and less membrane surface
demand, which makes it economical because it increases efficiency and production.

Flux Equations

Membrane filtration can be divided into two zones, a pressure dependent zone and a
pressure-independent zone (Ghosh, 2006). In the pressure-dependent zone transmem-
brane pressure is the driving force, whereas in the pressure-independent zone mass
transfer is the only limiting mechanism. In the case of a clean membrane, with pure
solvent, permeate flux (Jv) is only dependent on transmembrane pressure and this can
be represented as:

Δp
Jv = (27.5)
Rm

where Δp is transmembrane pressure (Pa) and Rm membrane resistance (Pa·s·m−1). In

the case of ultrafiltration of solute, the additional resistance of the concentration
polarization layer (Rc, Pa·s·m−1) reduces permeate flux compared with pure solvent flux
at the same hydrodynamic conditions and transmembrane pressure:

Δp
Jv = (27.6)
(Rm + Rc )

In the case of the concentration polarization layer, driving force is also reduced due
to osmotic pressure (Π) of concentrated solute around the membrane, so permeate flux
can be represented as:

(Δp − ΔΠ)
Jv = (27.7)
(Rm + Rc )

The van’t Hoff equation gives the osmotic pressure of such a concentration polariza-
tion layer as:

Π = MRT (27.8)

where Π is osmotic pressure (kPa), M molar concentration (mol·m−3), T absolute tem-

perature (K), and R universal gas constant (8.314 J·mol−1·K−1). In the case of ultrafiltra-
tion, the concentration polarization layer is a problem that leads to increased resistance
780 Handbook of Food Process Design: Volume II

and lower permeate flux, so the above equation is limited to a restricted range of pres-
sures in the pressure-dependent zone. Hence in the pressure-independent zone with
concentration polarization layer resistance, mass transfer in ultrafiltration can be
described by a diffusion equation (assuming pseudo-steady state) (Earle and Earle,
2004):

J v = k ′ ln(Cw / C) (27.9)

where Cw and C are the solute concentrations at the interface and in the bulk solution
respectively. The effect of the physical properties of the material can be predicted from
known relationships for the mass transfer coefficient k′ (m·s−1). This equation has been
found to predict, with reasonable accuracy, the effect on the mass transfer of changes
in the physicochemical properties of the solution. This is done through well-established
relationships between diffusivity D, mass transfer coefficient k′, and other properties
such as density (ρ), viscosity (μ), and temperature (T) giving:

( k ′d D) = a [(dvρ μ ) m] × (μ ρD) n (27.10)

or (Sh ) = ( k ′d D) = a (Re ) m (Sc ) n (27.11)

where d is the hydraulic diameter, (Sh) the Sherwood number (k′d/D), (Sc) the Schmidt
number (μ/ρD), and a, m, and n are constants. In the case of microfiltration, permeate
flux is represented by the following equation:

ΔP
Jv = (27.12)
μ ( Rm + RC )

where μ is permeate viscosity (Pa·s), Rm membrane resistance (m−1), and RC cake resist-
ance (m−1) = rVc/Am where r is specific cake resistance (m−2):

r = [180 (1 − ε ) / ε 3 ](1 / ds2 ) (27.13)

where ε is cake porosity, ds particle diameter, and Am membrane area (m2). In the case
of dialysis, the driving force is the concentration difference across the membrane and
this can be represented as:

J v = ΔC Rm (27.14)

In the case of dialysis, two solvents pass through the feed side and permeate side
(dialyzate side) and thus overall flux of solute depends on membrane resistance
(Rm), feed side mass transfer resistance (Rf) and dialyzate side mass transfer resis-
tance (Rd):
 Membrane Separation and Design 781

ΔC
Jv = (27.15)
Rm + Rf + Rd

Sieving Coefficient in Ultrafiltration

It has long been predicted that the ratio of the diameter of the macromolecule to the
diameter of the membrane pore is the only criterion for selecting an ultrafiltration
membrane with appropriate molecular weight cut-off. However, it was experimentally
observed that sieving of macromolecules through an ultrafiltration pore is also depend-
ent on environmental parameters (pH, ionic strength, etc.), hydrodynamic parameters,
and membrane properties. Thus to select an appropriate membrane, a new parameter,
intrinsic sieving coefficient, was introduced and is defined as (Ghosh, 2006):

ψ = Cp Cw (27.16)

The difficulty in determining Cw has resulted in the introduction of a new parameter

known as apparent sieving coefficient, ψa, defined as:

ψ a = Cp C (27.17)

It was observed that sieving coefficient and apparent sieving coefficient are related by
the following mathematical expression:

ln [ψ a (1 − ψ a )] = J v k + ln [ψ (1 − ψ )] (27.18)

Thus by determining the apparent sieving coefficient at various values of permeate

flux (Jv), intrinsic sieving coefficient (ψ) and mass transfer coefficient can be calculated
for a particular solute. However, it is worthwhile noting that ψ needs to be constant
in the permeate flux range studied. It has been reported that ψ also depends on JV, but
at low permeate flux and high permeate flux is independent of Jv. Apparent sieving
coefficient can be used for determining the selectivity of a membrane for fractionation
of two macromolecules:

α = ψ a1 ψ a2 (27.19)

where ψa1 is apparent sieving coefficient of more transmitted solute and ψa2 is apparent
sieving coefficient of less transmitted solute.

Mode of Operation

Membrane operation is generally carried out in two modes: batch operation (Figure
27.6) and continuous mode (Figure 27.7). In large-scale operations, continuous mode
782 Handbook of Food Process Design: Volume II

Membrane

Feed tank

Pump

Figure 27.6 Batch operation.

Permeate

Retentate

Feed

Membrane

Feed tank

Figure 27.7 Continuous mode.

of operation is important as low membrane area in batch operation cannot provide

desired permeate flux.

Design of Membrane

The calculation of membrane area is the desired objective using known variables like
recovery factor, feed flow and composition, temperature, transmembrane pressure,
 Membrane Separation and Design 783

permeate flow, permeability for solvent flow, and rejection factor. The concentration
polarization layer effect is not considered in this method. The steps involved in deter-
mining the area of membrane are as follows.

1. Calculation of the concentration of the permeate stream:

Cp = 2C (1 − R) (2 − Q) (27.20)

assuming nearly complete rejection of solute, where R is rejection of solute.

2. Calculation of the flow of retentate (νr) from the global balance Equation 27.1 and
Q value:

v r = v f (1 − Q)

3. Calculation of the concentration of the retained stream (Cr) from Equation 27.2
using previously determined Cp.
4. Calculation of the mean concentration of the concentrated solution:

Cm = (v r Cr + v f C ) (v r + v f ) (27.21)

5. Determination of the concentration of the permeate stream:

Cp = Cm (1 − R) (27.22)

6. Steps 3, 4, and 5 are repeated using this value of the concentration of the perme-
ate stream to obtain a new value of such concentration. If this final value coincides
with the Cp value calculated in Equation 27.19, then the process is finished; oth-
erwise steps 3, 4, and 5 are repeated in an iterative way until the values
coincide.
7. Calculation of the osmotic pressure of the concentrated solution using as concen-
tration value that of the weighed mean and Equation 27.8.
8. Determination of the solvent flux from the following equation:

J v = ε ( ΔP − ΔΠ )

where ε is permeability of membrane for solvent.

9. Calculation of the membrane area needed to carry out the separation is given by
A = vp/Jv.

Another approach for designing membranes has been proposed by Lombardi and
Moresi where the concentration polarization layer is included (Ibraz and Barbosa-
Cánovas, 2002).
784 Handbook of Food Process Design: Volume II

Fouling of Membrane in Ultrafiltration and Microfiltration

Fouling of the ultrafiltration/microfiltration membrane occurs due to of adsorption of

the membrane surface and leads to increased resistance to flow, which can reduce
filtration flux rate and process economy, efficiency and recovery. Membrane fouling
refers to the irreversible alteration in membrane properties caused by feed stream
components. Fouling may be due to formation of a gel layer due to concentration
polarization, adsorption or deposition, and pore blocking. Generally, fouling is char-
acterized by measuring clean water flux decline at constant pressure.
Fouling in microfiltration membranes, particularly those used for purification of
proteins, has been overcome with the introduction of microsieves, which have well-
structured morphology and controlled porosity that improve separation behavior and
which show high feed flow rates. These lead to improved permeate flux, low operating
pressures, and improved process economics. Other anti-fouling methods include
surface modification by chemical methods to, increase surface hydrophilicity, coating,
and graft polymerization over membrane surface. The membrane material can also
influence fouling: in ultrafiltration, surface-modified polyvinylidene fluoride (PVDF)
membranes have been found to have low fouling properties.

Cleaning and Sanitation

Cleaning of membrane equipment depends on the nature of the membrane material

and availability of high quality water. Water should be free of suspended colloidal
particles or microorganisms that are likely to cause irreversible blockage. A commonly
used membrane cleaning cycle includes the following steps: (i) rinse with heating at
50 °C; (ii) alkaline cleaning with ternary detergents at 65–70 °C for 20 min; acid clean-
ing with HNO3 (0.5%) for 20 min at 50 °C followed by rinse with water at 50 °C.

Cost

Membrane separation is a highly cost-effective unit operation as as observed with the

production of apple juice, in which the gross profit and return on investment were
higher using a membrane process with or without pervaporation or reverse osmosis
in comparison with conventional operation. The annual manufacturing cost was also
low in the membrane process while payback time was also low compared with con-
ventional operation (Cuperus, 1998).

Applications

Membranes in their various configurations, including spiral, hollow fiber, and plate
and frame, are used throughout the food industry. The two main benefits are improved
 Membrane Separation and Design 785

production process and the recovery of valuable products (Slater, 1989). Improved
production processes include consistent high-quality permeate and retentate, reduced
operating cost, low maintenance, low pressure drop, chemical resistance, and longev-
ity of membrane (Strathmann, 1981). Microfiltration is used for clarification and
sterilization, both of which are the best options compared to centrifugation and heat
sterilization. Thus microfiltration can be used for the efficient removal of suspended
particles, fat globules, and high-molecular-weight proteins. Ultrafiltration is used for
fractionation, concentration, and purification, for example concentrated skimmed
milk has more calcium and protein content compared to conventionally treated milk,
while in fruit juices ultrafiltration removes polysaccharides, microbes, viruses, and
yeasts that make the final product unstable. Reverse osmosis has the advantages of
high-quality product separation without heat damage, reduced waste treatment
volume, and hence lower capital investment. Unique applications of membranes in
the food industry include concentration of oil emulsions, recovery of proteins, clari-
fication of wines, concentration of fruit juices, and treatment of food processing waste
products. Potential applications of various membrane systems in food processes are
wide, for example in sugar mills ultrafiltration has helped in the production of color-
less sugar and improved the sugar extraction process.
Membrane-based techniques have a fundamental role in the separation and puri-
fication of proteins. Ultrafiltration, microfiltration, and nanofiltration have greatest
application in protein purification. Microfiltration is used mainly for the recovery of
extracellular protein produced by the fermentation of bacteria but also for removal
of microbes and viruses in preparation of therapeutic proteins. Much effort has been
made to improve mass transfer in ultrafiltration and microfiltration membranes.
Some examples include rotating disk filters, cylindrical taylor vortex devices, and
conically shaped rotors (Saxena et al., 2009). A material like polyethersulfone has
been designed for selective permeation and protein recognition/purification and is
used in the purification of soya protein. Electrically enhanced membrane filtration
(EMF) is an advanced technique that utilizes an electrical field for filtration. An
electric field has been found to have good impact on protein transmission and selec-
tivity (Nagarale et al., 2006). In one approach ultrafiltration in the presence of ultra-
sonic waves is used to separate proteins, which can solve the problem of polarization
and fouling (Saxena et al., 2009).
Glucose syrup can be used as a food ingredient for biscuits, soft drinks, jams, and
food preservatives. Ultrafiltration is used to eliminate suspended solids and proteins
from wheat hydrolysate, and does not even affect dextrose equivalent in filtered sugars
(Pinelo et al., 2009). In the case of vegetable proteins and their various derivatives
used for a variety of beverages, processing with membranes has the advantages of
reduction of transport cost and better manufacture of intermediate products.
Membranes are also used for separation and harvesting of enzymes and microorgan-
isms. In fermentation, cells are harvested by centrifugation but for economic reasons
the harvesting must be continuous, which is implemented using continuous cross-
flow membrane filtration.
786 Handbook of Food Process Design: Volume II

In the beer industry, membranes are used to increase brightness (Le, 1987) and
clarity, while filtration removes solids and particles from malt, hops and yeast. Rough
beer is filtered in order to eliminate yeast and colloidal particles responsible for haze
(Takács et al., 2007). Microfiltration of beer can ensure microbiological stability in a
single operation. In the milk and dairy industry, membranes can be used to control
microbial growth instead of heat treatment. Membrane filtration is used for globular
milk fat fractionation (Daufin et al., 2001). Microfiltration is used in an integrated
protein extraction process for the manufacture of micelle casein products and whey
protein isolates. Membranes are also used in the treatment of dairy effluents and waste
stream. Membrane processes should contribute to process simplification, improve
competitiveness, and be environmentally beneficial.
In juice production, use of membranes leads to better process economics and product
quality. Enzymatic membrane reactor is used for the clarification and maceration of
juice, reverse osmosis for concentration, and pervaporation for recovery of aromas
(Girard and Fukumoto, 2000). By choosing a suitable membrane configuration, it is
also possible to achieve direct pulping and clarification in one step. Membranes are
also used for agrowaste treatment. Membranes are used in processes especially devel-
oped for the treatment of persistent compounds like chlorobenzene, tetrachloroethyl-
ene, and trichloroethylene. In water these components are mostly present at a very
low concentrations, which makes conventional processing inefficient.
Membrane systems are extensively used throughout the various biological and
chemical industries to control variety of products (Pal et al., 2009). These membrane
processes are successful because they are effective and economically implemented at
the very large scale required for industrial application. A combination of different
membrane processes gives interesting benefits not achieved by single operation. On
an industrial scale, the integration of various membrane operations can be beneficial
because it leads to low environmental impacts, low energy consumption, and high-
quality products. Dairy proteins, food additives, nutraceuticals and therapeutics
processing by membrane integration can be advantegous. An example is shown in
Figure 27.8.

Conclusions

Most of the membrane technology used in the food industry originated in the dairy
industry. Ultrafiltration is the most widely used process in the dairy industry.
Microfiltration is used for removing microorganisms and casein micelles. Membranes
play an important role in the fractionation of milk. Current membrane processes are
limited by their low capacity due to fouling. Microfiltration reduces the amount of
bacteria and spores without affecting the taste and flavors of milk. It can be used for
the pretreatment of skim milk for production of raw milk cheeses. Ultrafiltration has
found major application in the production of cheese. Whey contains dissolved salts,
 Membrane Separation and Design 787

Raw juice

Figure 27.8 Integration of various membrane systems for fruit juice processing.

sugars and 25% of the original protein, and thus ultrafiltration of whey allows these
additional foods to be recovered. Another role of membrane separation is in fractiona-
tion of buttermilk, an application where both ultrafiltration and microfiltration can
be used. In the food and beverage industry, safety, microbiological quality, functional-
ity, texture, and flavors can be improved by membrane processes. Clarification of fruit
juices can be done by microfiltration or ultrafiltration and deacidification by electro-
dialysis. Significant developments have been made in membrane technology in the
last decade but the potential is limitless and there is a great need for research in all
these aspects. Lower cost, lower fouling rates, and lower energy consumption will
improve commercialization.

References

Bailey, A.F.G., Barbe, A.M., Hogan, P.A., Johnson, R.A. and Sheng, J. (2000) The effect
of ultrafiltration on the subsequent concentration of grape juice by osmotic distil-
lation. Journal of Membrane Science 164: 195–204.
Bruschke, H. (1995) Industrial application of membrane separation processes. Pure and
Applied Chemistry 67: 993–1002.
Cuperus, F.P. (1998) Membrane process in agro-food: state of the art and new oppor-
tunities. Separation and Purification Technology 14: 233–239.
Daufin, G., Escudier, J.P., Carrère, H., Bérot, S., Fillaudeau, L. and Decloux, M. (2001)
Recent and emerging application of membrane processes in food and dairy industry.
Transactions IChemE 79A: 1–14.
788 Handbook of Food Process Design: Volume II

Earle, R.L. and Earle, M.D. (2004) Unit Operations in Food Processing, 4th edn. New
Zealand Institute of Food Science and Technology. Available at [Link]/
unitoperations
Ghosh, R. (2006) Principles of bioseparations engineering. World Scientific, Singapore:
pp 199–242.
Girard, B. and Fukumoto, R.L. (2000) Membrane processing of fruit juices and bever-
ages: a review. Critical Reviews in Biotechnology 20: 109–175.
Ibraz A., and Barbosa-Cánovas, G.V. (2002) Unit operations in food engineering. CRC
Press, Boca Raton, FL.
Le, M.S. (1987) Recovery of beer from tank bottoms with membranes. Journal of
Chemical Technology and Biotechnology 37: 59–66.
Marriott, J.I., Sørensen, E. and Bogle, I.D.L. (2001) Detailed mathematical modelling
of membrane modules. Computers and Chemical Engineering 25: 693–700.
Memtec Ltd (1998) The use of cross flow membranes to clarify and stabilize beer.
Filtration and Separation 35: 860–861.
Nagarale, R.K., Gohil, G.S. and Shahi, V.K. (2006) Recent developments on ion-
exchange membranes and electro-membrane processes. Advances in Colloid and
Interface Science 119: 97–130.
Pal, P., Sikder, J., Roy, S. and Giorno, L. (2009) Process intensification in lactic acid
production: a review of membrane based processes. Chemical Engineering and
Processing 48: 1549–1559.
Pinelo, M., Jonsson, G., Anne, S. and Meyer, A.S. (2009) Membrane technology for
purification of enzymatically produced oligosaccharides: molecular and operational
features affecting performance. Separation and Purification Technology 70: 1–11.
Reis, R.V. and Zydney, A. (2007) Bioprocess membrane technology. Journal of
Membrane Science 297: 16–50.
Saboya, V.L. and Maubois, J.-L. (2000) Current developments of microfiltration tech-
nology in the dairy industry. Lait 80: 541–553.
Saxena, A., Tripathi, B.P., Kumar, M. and Shahi, V.K. (2009) Membrane-based tech-
niques for the separation and purification of proteins: an overview. Advances in
Colloid and Interface Science 145: 1–22.
Slater, C.S. (1989) Instruction in membrane separation processes. Journal of Membrane
Science 44: 265–272.
Strathmann, H. (1981) Membrane separation processes. Journal of Membrane Science
9: 121–189.
Takács, L., Vatai, G. and Korány, K. (2007) Production of alcohol free wine by per-
vaporation. Journal of Food Engineering 78: 118–125.