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Membrane Fouling - A Mini Review: April 2016
Membrane Fouling - A Mini Review: April 2016
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1.0 INTRODUCTION
“Water, water, everywhere, but not a drop to drink” this was a famous line from Coleridge’s
Rime of the Ancient Mariner; a situation depicting a stranded sailor at sea surrounded by saline
water. Inaccessibility to clean and safe water is an abstract concept to many and a glaring reality
for others. Its occurrence is mostly influenced by innumerable political, economic, environmental
and social forces.
The United Nation estimates that 1.8 billion people will be residents of areas plagued by water
shortage, while two-thirds of the world's population will probably live under water stressed
conditions by 2025 (UN 2013).
A growing fresh water scarcity has compelled the use of desalination and membrane technology
for the purification of sea and ocean water.
The 21st century has seen the increased use of membranes not only for desalination but as one of
the most promising water and wastewater treatment technology. Membranes are efficient in
reducing contaminant concentration levels in water and wastewater. The use of membranes in
water and wastewater treatment has grown in popularity when compared to other conventional
water treatment technologies. This comparative advantage stern from membranes low space
requirement, no chemical use, ease of operation, reduced operation units and selective separation.
However, the major limitation to the efficient use of membranes is its inability to maintain filtration
flux for a long period of time as a result of membrane fouling. This situation creates a challenge
as it results in increased salt passage and decreased water flux across membranes, thereby
hindering its development and application.
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Membrane Fouling – A Mini Review
Membrane fouling can be characterized as reversible or irreversible fouling based on the strength
of materials being attached to the membrane surface. Reversible fouling occurs when there is no
permanent permeate flux loss and fouling can be removed by backwashing or a strong shear force.
Irreversible fouling is caused by permanent permeate flux loss and fouling is removed by chemical
cleaning3.
Fouling can also be characterized based on the type and nature of material removed as5;
Colloidal fouling: Colloids such as clay, silica, aluminum, and iron are common in natural waters.
They range in different sizes (µm to nm) and mostly carry a negative surface charge. They can
deposit and accumulate within the pores and surface of membranes causing an adverse effect on
membrane performance and water quality.
Organic fouling: This is the adsorption of NOM or DOM to membrane surfaces. Several factors
such as hydrophobicity, molecular weight, ionic strength, calcium concentration and electrostatic
charge have been suggested to contribute to organic fouling in membranes.
2
Membrane Fouling – A Mini Review
Scaling fouling: This is the precipitation of salts, hydroxides and oxides from solutions and is
dependent on the concentration and temperature, they include ions such as calcium, magnesium,
bicarbonate, sulfate, silica, iron and barium.
Biofouling: This is the loss of membrane performance as a result of interactions between
membrane material, feed water and microorganisms leading to formation of biofilms.
The reason for characterization of membrane fouling is because each type of fouling and foulants
has its effect on membrane performance and also has its own distinct mitigation/cleanup approach.
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Membrane Fouling – A Mini Review
absent in the presence of Mg2+. The effect of initial flux and crossflow velocity on fouling was
also observed, as initial flux increased, fouling was enhanced, while an increase in crossflow
velocity led to a reduction in fouling. These effects were also seen evident in Li et al.8 study where
fouling by sodium alginate (SA) was seen to be more severe than bovine serum albumin (BSA) as
a result of formation of calcium alginate gel on membrane surface8. Also, membrane surface
morphology was seen to play an important role in fouling, as rough surface membrane led to
increased fouling.
With BSA, it was observed that increasing ionic strength, decreasing pH and the presence of Ca2+
led to a decline in permeate flux.9 However, there was a small decline in flux in the presence of
Mg2+ which was attributed to salting out effect as Mg+ exhibits greater salting effect than Ca2+ as
a result of its higher charge density. It was also observed that as temperature increased, flux
decreased, which might be a result of BSA denaturation and exposure to the surrounding, this
increased its adsorption to membrane surface thus increasing the rate of fouling.9
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Membrane Fouling – A Mini Review
acts as centers for precipitation. Similar trends with organic fouling in NF membranes have also
been reported.17,18
It has been stipulated that water affinity of membranes should not be the sole factor for determining
fouling in NF membrane but rather its surface chemistry.19 A study on native (TiO2) and grafted
ceramic NF membranes, in fouling by HA without Ca2+ showed that very hydrophilic membranes
(native membrane) exhibited severe fouling while hydrophobic membranes (grafted membranes)
showed little or no fouling.19 Degree of fouling was dependent on surface chemistry of membranes
rather than Ca2+ ions, as native membranes showed decrease in fouling with the presence of
Ca2+ ions while grafted ceramics showed increase in fouling.19 Same trend was observed with and
without fulvic acid which was attributed to the interactions between the functional groups of DOM
(COOH and OH) and OH groups of the native membranes unlike the grafted membranes which
had different functional groups (aromatic and –CH3).19 Figure 2 shows the changes in foulant-
membrane interactions with and without Ca2+, arrow thickness signifies the strength of potential
interactions.
5
Membrane Fouling – A Mini Review
Fouling for feedwater with high ionic strength was represented by cake formation due to reduced
charge repulsion between positively and negatively charged natural organic matter (NOM), while
for feedwater with inorganic scalants (CO32−, SO42−, and PO43−) was via pore blocking as a result
of precipitation on membrane surface and pores.
6
Membrane Fouling – A Mini Review
might be as a result of acid dissociation. However, this is in contrast with another study29 where
fouling was seen to occur in both acidic and alkaline solutions, where acidic pH promoted gel layer
formation and alkaline pH promoted pore blockage with humic foulants.29 Increased Ca2+ and
pressure enhanced fouling and fouling was said to occur via three mechanisms internal pore
adsorption, pore blockage and cake formation.29
4.0 DISCUSSION
Membrane fouling is common to all types of membrane and its mostly dependent on the membrane
properties, feedwater properties and concentration, operating conditions and solution chemistry of
feed water. foulants are seen to differ and have varying effects across different types of
membranes. For example, in NF and RO, biofouling and inorganic (scaling) are said to be the
dominant form of fouling occurring in these processes due to precipitation occurring on membrane
surface because of hydrolysis and oxidation of foulants where salts are seen exceeding their
solubility. However, Mustafa et al.19 observed a decline in fouling upon addition of Ca2+ to native
NF membranes when compared to grafted membranes showing the case where fouling was
dependent on the surface chemistry of the membrane rather than the foulant. This varying effect
was also seen in Li et al.17 where increased ionic strength had no effect on fouling while
studies8,9,16,22,30 observed enhanced fouling with increased pH, ionic strength and initial flux.
In MF and UF, there are no salt concentration in the reject stream so inorganic fouling are less
dominant, rather organic fouling by NOM and its different components are mostly responsible for
fouling in these two processes. Duclos-Orsello et al.24 observed negligible fouling when changes
were made to pH and concentration and foulants were found to adsorb differently on membranes
made from different materials (membrane morphology) while Mohammad et al.28 observed a
decline in fouling with increasing pH. Ca2+ was also seen to increase fouling.
Based on the above, it is seen that there are no important or specific foulants for all membrane
type, rather it is a function of the foulants characteristics, membrane properties, solution chemistry,
operating conditions and understanding the fouling process and phenomena.
7
Membrane Fouling – A Mini Review
Chemical cleaning is used for irreversible fouling and restoration of permeability in membranes
and includes processes such as hydrolysis, solubilisation, and chelation. The most applied chemical
cleaning processes in water treatment plants are cleaning in place (CIP) which is conducted less
frequently and incorporates the use of sodium hypochlorite and citric acid for removal of organic
matter and inorganic substances respectively and chemically enhanced backwash (CEB) which is
conducted frequently by the use of oxidants such as chlorine and ozone.54,55 However, consistent
chemical cleaning can reduce the life span of membranes leading to membrane replacement which
means more cost.56 The effectiveness of membrane cleaning can be influenced by temperature in
that temperature can lead to change in chemical reaction equilibrium, reaction kinetics and
solubility of foulants57.
BSA fouled UF membranes have been effectively cleaned 58 with NaCl, NaNO3, NH4Cl and KCl
salts and it was observed that higher temperature yielded higher cleaning efficiency. Another study
also achieved effective cleaning with HCl, NaOH, and HOCl.59 CaSO4 a scalant was effectively
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Membrane Fouling – A Mini Review
cleaned using EDTA-4Na, KCOOH , citric acid, NaOH and NaCl , an order of efficiency was
obtained EDTA-4Na > NaCl > citric acid > NaOH > KCOOH which might be because EDTA
forms a chelate with CaSO4 which is highly soluble in water therefore making it easy to be
cleaned.60
However, even though cleaning has been achieved with these processes, there are also limitations
associated with them. Pretreatment (coagulation/flocculation) removes or changes the
physicochemical properties of potential foulants thereby improving membrane rejection, excess
coagulants has also seen to be potential foulants.61
Some cleaning methods are dependent on the membrane configuration, sponge balls are assumed
to be only effective for tubular membranes in the absence of internal obstructions62 while several
studies63-65 have reported that air sparging is more effective in membranes with loose modules and
they are cost intensive due to energy cost. Air bubbling can sometimes prove ineffective as there
have been cases where bubbles adsorbed on membrane surface and the internal pores leading to a
decline in flux.66 Hwang et al.67 reported that air sparging reduced deposition of particle on
membrane surface but did not show any effect on the internal fouling.
Shear force and transmembrane pressure can cause algal cell lysis resulting in highly degradable
and increased soluble proteins, sugars, neutral and negatively charged polysaccharides68 which
facilitates foulant attachment on membranes thereby aggravating fouling.
Backwashing reduces internal and surface fouling and allows longer operation of plant before shut
down for chemical cleaning.69,70 However, backwash may pave way for infiltration of
macromolecules into membrane pores due to its loosening and detaching of cake layer.71
Backwash efficiency is dependent on the duration and frequency of the backwash cycle as there is
need for temporary shutdown of filtration process and some permeate consumption.70 Studies72,73
have reported that air assisted backwash shortens the backwash cycle and improves foulant
removal, this is however in contrast with a study by Metzger et al.74 who reported that air assisted
backwash encourages irreversible fouling
Anti-scalants used in membrane cleaning are mostly phosphate based and these may aggravate
fouling. Phosphates are essential plant nutrients and promotes algae growth, also when in contact
with natural waters can lead to eutrophication so dosage applied should be monitored in order to
avoid the occurrence of such incidents.
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Membrane Fouling – A Mini Review
Oxidants such as ozone and chlorine can lead to degradation of NOM producing polar disinfection
byproducts (DBP) which may act as foulants. Some chemicals are able to restore permeate flux
however, they may cause a reduction in rejection of particles by membranes.75 Oxidants can also
lead to reduced mechanical strength of membranes76, and ageing of membranes resulting in
changes to pore sizes of membranes and a reduction in their hydrophobicity and hydraulic
resistance.77 Frequent chemical cleaning is also associated with waste production and shut down
of the membrane process reducing the plant capacity.
The issue of foulant mitigation by different processes is a complex one as it may be that membrane
materials, cleaners, and foulants chemistry are not the main factors for determining membrane
cleaning efficiency as fouling most times do not occur via a sole mechanism or material but via
combination of different mechanisms and materials. Thus much importance should be attached to
the understanding of the mechanism of combined fouling.
6.0 SUMMARY
This paper has given a review on membrane fouling based on fouling mechanism, fouling
characteristics, and common foulants as well as measures taken to mitigate fouling. A major
conclusion can be drawn at the end of this review, membrane fouling is consistent in all membrane
types. It is seen that fouling is specific to different operating conditions. As far as the issue of
fouling exists, it is important that all fouling phenomena and processes are adequately understood
and are taken into account before and during operation in order to reduce flux decline because
most membrane fouling’s that have occurred during membrane application are as a result of
inadequate understanding of processes, operating conditions and phenomena. Designing and
developing membranes with enhanced modified membrane surfaces, improved water affinity and
improved pore sizes and distribution should be considered. Feedwater conditions can also be
optimized, pre-treatment before filtration should not also be left out as it was seen that pre-
treatment of feedwater helped reduce fouling. The development of green and sustainable
techniques (less or no chemical) for cleaning membranes is also something that should/needs to
be addressed in membrane fouling.
However, an important research question that needs to be addressed in membrane fouling is “Is
there a complete understanding of fouling process and phenomena?” until this is addressed, fouling
would continue to occur in membrane application.
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Membrane Fouling – A Mini Review
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Membrane Fouling – A Mini Review
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