Journal of Membrane Science 436 (2013) 28–35

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Journal of Membrane Science

journal homepage: www.elsevier.com/locate/memsci

Comparative analysis of physical cleaning operations for fouling control

of hollow fiber membranes in drinking water treatment
Nigel. P. De Souza, Onita D. Basu n
Department of Civil and Environmental Engineering, Carleton University, 1125 Colonel By Drive, Ottawa, ON, K1S 5B6, Canada

a r t i c l e i n f o a b s t r a c t

Article history: The combined effect of air scouring, backwashing and relaxation on the fouling reduction of a hollow
Received 23 November 2012 fiber PVDF ultrafiltration membrane was investigated using factorial designs of experiments. The
Received in revised form investigation was carried out to test and compare the efficiency of three physical cleaning operational
7 February 2013
regimes, specially: air scour, backwashing, and relaxation. Beneficial dependencies between the
Accepted 10 February 2013
Available online 17 February 2013
operations for fouling reduction were identified and examined in this study.
The use of a three operation regime under continuous flow conditions was found to be more
Keywords: effective for fouling reduction compared air assisted backwashing and air assisted relaxation with
Hollow fiber membrane fouling reductions 2.5 and 3 times lower, respectively. While the use of a short backwash duration
Backwashing
showed negligible impact on fouling reduction, a longer backwash duration was found to work in
Air scouring
synergy with a high air flow rate and a short relaxation duration for the reduction of fouling. The use of
Relaxation
Factorial design a regime involving long backwash duration (20 s), short relaxation duration (5 min.) and high air flow
rate (15 LPM) was identified as the optimal regime for fouling reduction while minimizing permeate
production losses due to backwash and relaxation operations in this study.
& 2013 Elsevier B.V. All rights reserved.

1. Introduction microstraining [3,6] or through membrane cleaning operations.

Advancements in membrane technology over the past decade
have led to the emergence of hollow fiber membrane ultrafiltra-
tion as a sound alternative to conventional methods of drinking
water treatment [1,2]. The use of ultrafiltration (UF) in the
production of drinking water has shown great promise due to
its ability to remove contaminants such as turbidity, organic
matter and pathogenic organisms (protozoa, bacteria and some
viruses) from source waters [1–3].
While the removal of these contaminants ensures a higher
quality of drinking water, studies have identified turbidity causing
particles and natural organic matter (NOM) in source waters as key
contributors to the phenomenon of membrane fouling [3,4]. Fouling
occurs due to the clogging of membrane pores and/or the buildup of
a cake layer on the membrane surface. This fouling results in an
increase in the transmembrane pressure (TMP) with a correspond-
ing decrease in membrane productivity either through increased
energy requirements or an associated decrease in permeate out-
put [5]. Consequently, fouling is highly unfavourable and continues
to be a major focus of membrane research.
Membrane fouling is controlled in two main ways: pre-
treatment techniques such as coagulation, filtration, and
n
Corresponding author. Tel.: þ1 613 520 2600x2231; fax: þ1 613 520 3951.
E-mail address: onita_basu@carleton.ca (O.D. Basu).
Cleaning operations are categorized into physical and chemical
cleaning operations and target different levels and types of
fouling. Physical cleaning operations are used to target fouling
which is easily removed from the membrane surface and pores
and employ physical processes like backwashing, air scouring and
relaxation to remove foulants off the membrane surface [7,8].
Chemical cleaning targets fouling that have a strong adhesion to
the membrane surface or in the membrane pores and makes use
of various chemicals (acids and alkalis) [3,6,7,9]. Both types of
membrane cleaning are aimed at recovering membrane perme-
ability. Physical cleaning slows down the loss of membrane
permeability overtime but eventually chemical cleaning is
required to restore a greater amount of the initial permeability.
Excess use of chemical cleaning is detrimental to the well being of
the membrane and can be costly. For instance a study by Wang
et al. [10] found that sodium hypochlorite was responsible for
weakening the membrane as well as changing membrane proper-
ties by removing surface modifications. Studies have also shown
that the use of sodium hypochlorite causes an increase in the
effective pore size of the membrane [11,12]. Since physical
cleaning precedes chemical cleaning, the proper optimization of
physical cleaning operations can prove to be beneficial for the
purpose of reducing the frequency of chemical cleaning thus
lowering costs while maintaining the wellbeing of the membrane.
The physical cleaning operations of backwashing, air scouring
and relaxation are fundamental operational strategies incorporated

0376-7388/$ - see front matter & 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.memsci.2013.02.014
 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35
into membrane bioreactor designs for the treatment of wastewater
[13]. However literature on the application and effects of these
operations in membrane filtration for drinking water purposes is
sparse. While studies have shown that periodic backwashing is
effective in removing the gel/cake foulant layer off the membrane
surface and thus reduce fouling [14,15], a recent study by Ye et al.
[13] showed that periodic backwashing only loosens foulants while
another mechanism is required to actually move the foulants off the
surface of membranes. Yigit et al. [16] and Remize et al. [17] showed
that backwashing was effective in removing surface fouling when
assisted by air scouring which played the major role of pushing the
loosened foulants off the membrane surface. While air assisted
backwashing has proved helpful in reducing fouling and restoring
membrane permeability, Metzger et al. [18] found that the constant
removal of the cake layer by air assisted backwashing promoted
irreversible fouling via pore blocking due to continuous adsorption
of smaller particles on the membrane surface in the absence of a
cake layer [15,22]. As such, the efficiency of backwashing as a
cleaning operation is dependent on the duration, interval and even
strength of the operation [19].
As in the case of backwashing, studies have shown that
relaxation is helpful in reducing surface fouling [2,13,19]. Relaxa-
tion is where permeate production is halted for brief time
intervals versus backwashing where the flow is reversed through
the membrane system. While Tian et al. [2] found that relaxation
alone removed foulants off the membrane surface; Ye et al. [13]
found that air scouring was required to remove surface foulants
loosened by relaxation. Ye et al. [13] also found that air assisted
relaxation was less effective than air assisted backwashing which
contradicted findings by Wu et al.[19].
Previous studies have taken into consideration the effects of
combining relaxation and air scouring [13] as well as backwash-
ing and air scouring [12,13] in drinking water treatment. In both
cases, air is responsible for moving foulants loosened by relaxa-
tion and backwashing away from the membrane surface and thus
plays an important role in the physical cleaning of the membrane.
The efficiency of air scouring is dependent on the air flow rate as
well as the frequency of air flow [2,20]. While continuous air
scouring was found to be more efficient at controlling fouling
than intermittent air scouring [2], the use of intermittent fouling
is more cost effective [21].
Studies examining the effect of all three physical cleaning
operations on fouling reduction appear to be limited. In this
research, the effects of a physical cleaning regime incorporating
air scouring, backwashing and relaxation on the reduction of
fouling in a bench scaled hollow fiber ultrafiltration membrane
system is investigated. Factorial designs of experiments were
employed to investigate the effects of relaxation duration and
frequency on fouling reduction as well as to identify benefits of
air scouring, backwashing and relaxation in a cleaning regime.
2. Materials and methods
2.1. Experimental apparatus
A ZW-1 hollow fiber ultrafiltration membrane (Zenon/GE,
Oakville, Canada) with a nominal pore size of 0.04 mm was used
at a flux of 38 LMH (permeate flow of 30 mL/min). The system
was operated under vacuum with a pressure range between 0 to
8.7 psi (0 to 0.6 bar); pressure was monitored using a Cole
Parmer high accuracy pressure transducer (Model No. EW-68075-02).
A schematic of the bench scaled apparatus can be seen in Fig. 1.
The air scour rate was set at 5 or 15 standard LPM and was
monitored with an AALBORG GFM37 flow meter (0–15 LPM). The
air was passed through a filter before passing by the membrane
29
module. Both the pressure transducer data and the air flow-rate
data was continuously logged over time using a data logger. The
entire set up was built in duplicate. Membranes were chemically
cleaned in place between each experiment following manufacture
recommended protocols. Membrane permeability was checked at
the start of every experiment and membranes were replaced once
the initial permeability was at 85% of the original value. The
membranes were rinsed with distilled water before being placed
back in operation. The membrane system was either operated in
dead-end mode (100% recovery of feed flow in permeate stream)
or continuous flow mode (80% recovery of feed flow in permeate
stream). A system schematic is shown in Fig. 1.
2.2. Feed water
Synthetic surface water was prepared in distilled water with
the following conditions: pH of 7–8 (adjusted with sodium
hydroxide as necessary); organic carbon comprised of Sigma
Aldrich Technical Grade Humic Acid (3 mg/L TOC) and Sigma
Aldrich 20 mm cellulose (3 mg/L TOC) intended to mimic a
challenging surface water source; kaolin clay was added to the
feed water for a final turbidity of 20 NTU. Water hardness was
simulated as 150 mg/L CaCO3 to mimic a moderately hard source
water, and was comprised of reagent grade sodium bicarbonate
(67 mg/L) and calcium sulphate (129 mg/L).
2.3. Experimental design
2.3.1. Relaxation parameter effects
The impacts of relaxation parameters on continuous versus
dead-end flow operation were examined with respect to relaxa-
tion duration and frequency. The operational conditions can be
seen in Table 1. For each experiment, fouling was measured in
terms of TMP (mbar) every 15 s during filtration and relaxation
periods and at every second during periodic backwashes over a
24 h experimental run. Line 170: Air was supplied continuously in
this experiment at 5 LPM. A fixed flux of 38 LMH was used for
both filtration and backwash conditions. Relaxation duration and
frequency parameters were based on values reported in literature
[19,20].
2.3.2. Cleaning operation effects
The effects of air flow rates, backwash durations and relaxation
durations on fouling minimization were studied using a 23
factorial designs. The factorial design experiments can be seen
in Table 2 along with the cleaning operational parameters
involved. The 23 factorial experiments made use of continuous
flow operation with 80% recovery and were performed over a five-
day period. TMP was recorded at regular intervals during each
flow and relaxation operation.
2.3.3. Cleaning operation exclusion test
A fractional 23 factorial experimental design was employed to
investigate the impact of cleaning parameter exclusion on mem-
brane fouling (see Table 3). Continuous flow operations with 80%
recovery and 38 LMH forward flux were used for the experiments
and as in all previous factorial design of experiments, fouling was
measured in terms of TMP (mbar) at regular time intervals over a
two-day experiment period.
30 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35

Fig. 1. Schematic of experimental setup.

Table 1 Table 2
Operational parameters for relaxation duration and frequency analysis on fouling 23 factorial design used to evaluate the effect of air flow rate, relaxation duration
reduction. and backwash durations on membrane fouling.

Filtration flux 38.3 LMH (30 ml/min) for 15 min Experiment # Factors
Backwash flux 38.3 LMH (30 ml/min) for 10 s
Air flow rate 5 LPM Air flow Relaxation Backwash
Relaxation conditions rate duration duration
Operation mode Duration (min) Frequency (h)
Exp 1 (dead-end) 5 2 Exp 9   
Exp 2 (dead-end) 15 2 Exp 10 þ  
Exp 3 (dead-end) 5 4 Exp 11  þ 
Exp 4 (dead-end) 15 4 Exp 12 þ þ 
Exp 5 (continuous) 5 2 Exp 13   þ
Exp 6 (continuous) 15 2 Exp 14 þ  þ
Exp 7 (continuous) 5 4 Exp 15  þ þ
Exp 8 (continuous) 15 4 Exp 16 þ þ þ
Operational Parameters
Air flow rate (continuous) 5 LPM ( ), 15 LPM (þ )
3. Results and discussion Relaxation duration 5 min (  ), 15 min (þ )
(interval: 4 hn)
3.1. Relaxation duration vs. frequency Backwash duration (flux: 10 s (  ), 20 s (þ )
19 LMH)
Filtration flux (15 min cycle) 38 LMH (30 mL/min)
Relaxation duration (5 or 15 min) and frequency (2 or 4 h)
were tested in both dead-end and continuous flow modes with n
Relaxation once every 16 cycles; 1 cycle ¼ forward flow þbackwash
the hollow fiber membranes. Interestingly the greater specific flux
value for the dead-end flow mode (Table 4) was at opposing under all conditions tested. In order to help validate experimental
conditions to that observed for the continuous flow mode. results a randomized set of replicate experiments was conducted
Specifically, the highest specific flux in dead-end mode for experiments 2, 6 and 16. The general observed trend lines
(3.94 LMH/mbar) was observed at a relaxation duration of 5 min fitted closely and the final TMP values for these tests were within
and a frequency of 4 h; while the highest specific flux in 5% of the original values.
continuous flow mode (3.61 LMH/mbar) was observed at a The fouling trends in Figs. 2 and 3 show that the shorter and
relaxation duration of 15 min and a frequency of 2 h. Overall, the less frequent relaxation operation produced the least fouling for
continuous mode had a slightly higher average specific flux the dead-end flow mode while the longer and more frequent
(2.78 LMH/mbar) compared to the dead-end mode (2.60 LMH/mbar) relaxation operation was beneficial for the continuous flow mode.
 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35 31

It is speculated that the longer relaxation durations during the Taking into account the highest specific flux and daily permeate
dead-end flow mode were thought to be responsible for increas- production achieved during this investigation an operational regime
ing the homogeneity of the reactor solution over time, circulating using a combination of high air flow rate, long backwash and short
smaller particles known to cause irreversible pore blocking [6,22] relaxation duration was found to be most effective for fouling
across the membrane surface, due to the continuous air scour, reduction.
thus increasing the rate of fouling. It is possible that an even Interestingly, the most severe fouling occurred (  50 mbar)
shorter relaxation duration may be preferred than the ones tested occurred under the following two conditions low air scour
in this study. Future studies will examine this in more detail. In (5 LPM), low relaxation duration (5 min), and either backwash
the case of the continuous flow mode, the longer relaxation duration (10 or 20 s) (see Figs. 4 and 5). Indicating that backwash
duration of 15 min assisted in decreasing the retentate concen- duration under low air scour and short relaxation was not
tration in the reactor which clearly contributed to the decrease in dominant in minimizing fouling. In the experiments where the
fouling observed. However longer relaxation times result in lowest fouling occurred air scour was high, while either low or
decreased water production per unit time therefore a balance high values for relaxation or backwash duration were present. At
between relaxation and system productivity must be taken into first glance this may imply that backwash duration did not
consideration. This work demonstrates the importance of taking influence the overall fouling in these studies. However, as
both relaxation duration and relaxation frequency into considera- previously mentioned, a positive effect of backwash duration on
tion when optimizing a hollow fiber membrane system. fouling reduction was noted. Interaction plots (Fig. 6) were thus
employed to verify this effect.
3.2. Three way combination—Air scouring, relaxation and Interaction plots are a visual graphical representation of the
backwashing relationship between independent and dependent factors. For
instance, the factors (air, backwash, relaxation) are the indepen-
An examination of the impacts on fouling reduction by dent variables while TMP represents the dependent variable.
combining air scour, backwash, and relaxation were undertaken When factors increase or decrease in uniform fashion the TMP
in these experiments. The observed final TMP changes and the change is independent of any interaction between the factors.
corresponding specific fluxes from the 23 factorial experiments However if slopes change in a non-uniform fashion then the TMP
investigating these effects are presented in Table 5. The low air change is dependent, at least partially, on the interaction between
flow rate (5 LPM) coupled with the short relaxation duration the factors. Fig. 6b and c shows that the effect of backwashing
(5 min.) resulted in higher fouling regardless of the backwash duration on fouling reduction is dependent on the air flow rate
duration (10 or 20 s). However, a positive effect of increasing the and the relaxation duration. While an increase in backwash
backwash duration to 20 s was noted when using regimes with duration when using a low air flow rate or long relaxation
combinations of low air flow rate and long relaxation duration duration did not result in any decrease in fouling, the use of a
(Table 5—Exp. 10 and 14) and vice versa (Table 5—Exp. 11 and 15). longer backwash duration when employing either a high air flow
rate or short relaxation duration maybe beneficial for fouling
Table 3 reduction.
Fractional 23 factorial design used to investigate the impact of cleaning para- The data also demonstrates the benefit of relaxation on
meters exclusion on membrane fouling. controlling fouling. When a short backwash duration was
employed (Fig. 4), the two lowest fouling curves occurred at the
Experiment # Factors
high relaxation duration. In the case of the longer backwash
Air flow rate Backwash Relaxation duration (Fig. 5), the fouling was similar whether a high air flow
duration duration rate or high relaxation duration was used. However it was also
observed that the results for the high air flow/low relaxation
Exp 17 þ þ 
duration and vice versa were not identical under both the short
Exp 18 þ  þ
Exp 19  þ þ and long backwash durations which also indicates a synergistic
Exp 20 þ þ þ type relationship between all three parameters when using a long
Operational parameters backwash duration. With regards to the relationship between air
Air flow rate 0 LPM ( ), 5 LPM (þ) flow rate and relaxation duration (Fig. 6a), a high air flow rate
(continuous) coupled with a short relaxation duration was found to have
Backwash duration 0 s ( ), 10 s (þ ) similar effects as low air flow rate coupled with a long relaxation
(flux: 19 LMH)
duration. Of these two combinations the use of a short relaxation
Relaxation duration 0 min (  ), 5 min (þ )
(interval: 4 h) duration ideal for higher permeate production along with a high
air flow rate was found to be ideal for fouling reduction in
nRelaxation once every 16 cycles; 1 cycle ¼ forward flow þbackwash this study.

Table 4
Effect of relaxation parameters (duration and frequency) on fouling reduction for dead-end or continuous flow.

Flow Experiment Relaxation duration Relaxation frequency Final DTMP (þ / Daily permeate produced Specific flux (LMH/
Operation # (min) (h)  2.6 mbar) (L) mbar)

Dead-end flow 1 5 2  17.2 40.6 2.23

2 15 2  17.9 37.6 2.14
3 5 4  9.72 41.4 3.94
4 15 4  18.2 39.8 2.10
Continuous 5 5 2  14.5 40.6 2.64
flow 6 15 2  10.6 37.6 3.61
7 5 4  19.3 41.4 1.98
8 15 4  13.3 39.8 2.88
32 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35

Fig. 2. Effect of relaxation parameters when employing a dead-end flow operation (Filtration and backwash flux -38 LMH).

Fig. 3. Effect of relaxation parameters when employing a continuous flow (80% recovery) operation (Filtration and backwash flux -38 LMH).

Table 5
Cleaning operation evaluation and cleaning operation exclusion tests.

Flow Type Exp Exp Backwash Backwash Continuous Air Relaxation Relaxation Final DTMP (þ/ Permeate Specific Flux
# duration Flux (LMH) duration (s) flow Rate (LPM) Duration (min) Frequency (h)  2.6 mbar) Produced (L) (LMH/mbar)
(days)

Air scouring and relaxation with short backwashes

Continuous 9 5 19 10 5 5 4  50.9 41.6 0.75
flow 10 5 19 10 5 15 4  23.9 40.0 1.60
11 5 19 10 15 5 4  32.5 41.6 1.18
12 5 19 10 15 15 4  11.2 40.0 3.42

Air scouring and relaxation with long backwashes

Continuous 13 5 19 20 5 5 4  48.7 41.0 0.79
flow 14 5 19 20 5 15 4  15.1 39.4 2.54
15 5 19 20 15 5 4  8.96 41.0 4.27
16 5 19 20 15 15 4  14.9 39.4 2.57

Operation elimination comparison

Continuous 17 2 19 10 5 5 4  32.8 41.6 1.17
flow 18 2 19 0 5 5 4  99.8 42.3 0.38
19 2 19 10 0 5 4  207 41.6 0.19
20 2 19 10 5 0 4  82.2 42.5 0.47
 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35 33

3.3. Parameter exclusion results

Limited research has examined the combination of air scour-

ing, relaxation and backwashing as a methodology for membrane
fouling reduction. The parameter exclusion results demonstrate
the dominant effect of air scouring on fouling reduction as well as
the benefit of combining relaxation, air scouring and backwashing
in a physical cleaning regime for the mitigation of membrane
fouling in drinking water treatment (Fig. 7). Visually the results of
the exclusion tests are clearly observed with the three parameter
cleaning regime resulting in a cleaner looking membrane than
any of the duo cleaning regimes (Fig. 8). Air scouring had the most
dramatic impact on the fouling in the system; with an increase in
TMP to approximately  200 mbar was observed when air

Fig. 4. Comparison of cleaning regimes employing air scouring (5 and 15 LPM),

relaxation (5 and 15 min duration) and a short backwash duration (10 s).

Fig. 7. Membrane surface conditions due to cleaning operation exclusion tests

Fig. 5. Comparison of cleaning regimes employing air scouring (5 and 15 LPM), (From left to right—with air scouring, backwashing and relaxation; without
relaxation (5 and 15 min duration) and a long backwash duration (20 s). relaxation; without backwashing; without air scouring).

Fig. 6. Dependencies between air flow rate (AF), relaxation duration (RD) and backwash duration (BD) (a) Air flow rate vs. relaxation duration, (b) air flow rate vs.
backwash duration, (c) relaxation duration vs. backwash duration.
34 N.P. De Souza, O.D. Basu / Journal of Membrane Science 436 (2013) 28–35
Fig. 8. Effect of cleaning operation exclusion under high fouling conditions (AF—air flow rate; BD—backwash duration; RD—relaxation duration).
scouring was excluded, compared to the base case of approxi-
mately  30 mbar when all three physical cleaning parameters
were employed. Excluding either backwashing or relaxation
resulted in similar increases to fouling with final TMP increases
between 80 and  100 mbar. Similar to findings reported by Ye
et al. [10], the use of air assisted backwashing was more efficient
in fouling reduction than the use of air assisted relaxation; while
incorporating all three physical cleaning methods resulted in the
lowest fouling conditions.
4. Conclusions
This research investigated the combination of three physical
cleaning operations on fouling reduction of hollow fiber mem-
branes in drinking water treatment. The impacts of relaxation
parameters on fouling reduction were found to be dependent on
the flow modes (continuous vs. dead-end) employed during
experimentation. A relatively lower fouling was observed with
the continuous flow mode compared to the dead end mode with a
longer relaxation duration (15 min) found to be beneficial for
fouling reduction.
Backwash duration was found to work in synergy with air
scouring and relaxation for the reduction of fouling. Both back-
wash duration and relaxation duration were found to have
integrated results, for instance in some cases low backwash
duration and a high relaxation duration had similar results to a
longer backwash duration and a shorter relaxation duration. Air
scouring was found to dominate membrane fouling control with
the lowest fouling observations in all instances when the air scour
rate was highest. The combination of the three operations proved
to be superior in reducing fouling compared to air assisted
backwashing and air assisted relaxation.
Full scale implications of this research would suggest that air
assisted backwash periods in combination with short durations
relaxation might be beneficial for removing reversible fouling
while minimizing net productivity losses due to backwash and
relaxation operations in the regime.
Acknowledgements
The authors would like to thank the Natural Sciences and
Engineering Research Council (NSERC) for helping fund this
research. The authors would also like to thank GE – Zenon for
providing the membranes for the research. Finally the authors
would like to thank Mr. Mohammad Al Rasheed for his assistance
during portions of the experiments.
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