Desalination 424 (2017) 140–148

Contents lists available at ScienceDirect

Desalination
journal homepage: www.elsevier.com/locate/desal

Laminated PTFE membranes to enhance the performance in direct contact MARK

membrane distillation for high salinity solution
Ying Chena, Rui Zhenga, Jin Wanga, Yongjie Liua,b, Yanqiang Wangc, Xue-Mei Lia,⁎, Tao Hea,b,⁎⁎
a
Laboratory for Membrane Materials and Separation Technology, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, China
b
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
c
The Walt Disney (China) Co., Ltd. Disney Research China, Shanghai 200031, China

G RA P H I C A L AB S T R A C T

A R T I C L E I N F O A B S T R A C T

Keywords: Due to the excellent performance in treating high salinity brines, membrane distillation (MD) has been widely
Membrane distillation employed in desalination, brine treatment and wastewater purification. Commercial hydrophobic membranes
Lamination were limited by wetting and fouling over time. Herein, we reported a simple and practicable method to improve
High salinity the stability performance of thin polytetrafluoroethylene (PTFE) membranes by laminating PTFE flat sheet
Air pockets
membranes. A NaCl solution with a concentration of 3.26 mol/L was utilized as a model high salinity brines.
Desalination
Results indicated that single-layered PTFE flat membrane did show high flux, but salt leakage occurred in a few
days caused by the contaminants leached from the tubing and connections. By simply laminating two pieces of
PTFE membranes, a double-layered membrane showed a very stable performance for nearly one month at a
rather high flux of 30 kg/m2 ∙ h. Air pockets between two sheets of PTFE membranes were observed during
operation resulting in flux fluctuation. Interestingly, these air pockets coincidently avoided the close contact of
the flat sheets, thus reduced overlapped pores which causing extra mass transfer resistance. Experimental ver-
ification of the reduced pore size and flux due to layer overlap. Proper module design would realize this la-
minated membrane as a potential stable MD membrane for treating high salinity water.

⁎
Corresponding author.
⁎⁎
Corresponding author at: Laboratory for Membrane Materials and Separation Technology, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203,
China.
E-mail address: het@sari.ac.cn (T. He).

http://dx.doi.org/10.1016/j.desal.2017.10.007
Received 19 August 2017; Received in revised form 4 October 2017; Accepted 4 October 2017
0011-9164/ © 2017 Elsevier B.V. All rights reserved.
Y. Chen et al.
1. Introduction
Water is the most precious resource for life on the earth. World's
population growth and climate change result in change in water supply
and habit of water consumption [1,2]. The global changes in population
and economic development in the next few decades envision large in-
crease in water demand [1]. To release the pressure of water crisis,
reusing of unconventional water resources, such as seawater, municipal
brine, and industrial wastewater etc., has been steady growth in the
water sector [3]. Desalination of all types is a prerequisite to guarantee
the quality of water [4]. The state-of-the-art reverse osmosis (RO)
reaches relatively low rate of energy consumption [5], but disposal of
the concentrate is a major issue. The concentrated brine is a secondary
waste stream that can increase the surface water salinity, thus leading
to negative impact on the environment [6]. Further extraction of water
from the brine using hybrid technologies is one potential direction.
In a typical hybrid desalination system, the brine is further con-
centrated using high pressure RO (HPRO), and the concentrate has even
higher salinity. At this point, pressure driving processes are limited by
high osmotic pressure, potential scaling and fouling. Membrane dis-
tillation (MD), a thermally driven process, is the alternative. The
driving force of MD is vapor pressure gradient across a hydrophobic
membrane. In a MD process, the feed temperature could be as low as
40–60 °C [7,8], thus, it is possible to utilize low-grade heat from in-
dustry and alternative energy sources, such as solar and geothermal
energy. MD provides an attractive solution for water and wastewater
treatment by membrane technology with a small footprint and low ef-
fective cost. By integration MD with RO or other process in a hybrid
system, high water recovery rate can be achieved [9–11].
MD is less sensitive to membrane fouling and feed salinity, therefore
suitable for treating high salinity brine and achieving high water re-
covery [12–14]. MD has been also reported for recovery of valuable
salts from effluents or brine from desalination operations [15,16].
Moreover, salt rejection is independent of feed salinity in treating high
salinity brines since, in theory, only water vapor is allowed to diffuse
through the membrane [17]. MD was recognized as one of the most
effective techniques for treatment of highly concentrated brines
[11,13,18,19], especially in places where low-grade heat, solar or
geothermal sources are available [20].
The key of MD is the hydrophobic membranes, which are readily
commercially available. MD membranes need to be specially designed
to exhibit high hydrophobicity [21], good thermal stability [22], ex-
cellent chemical resistance, and mechanical rigidity to ensure higher
permeation flux and better stability in long-term operation [22–26].
However, treating real water streams were limited by wetting and
fouling over time [27].
To overcome these challenges, special hydrophobic, super-
hydrophobic and omniphobic surfaces has been designed and devel-
oped for MD application in recent years [28,29]. High performance
superhydrophobic polyvinylidene fluoride (PVDF) flat sheet mem-
branes for MD were prepared via CF4 plasma surface modification
[27,30]. It was found that superhydrophobic PVDF membranes ex-
hibited stable MD performance in concentrating the anionic surfactant
emulsified waste water. A hybrid PDMS/PVDF electrospun membrane
with superhydrophobic surface was used in MD [31]. Novel dual-layer
in-air superamphiphilic and underwater superoleophobic membrane
surface was achieved via plasma induced grafting of polyethylene
glycol and subsequent TiO2 particles deposition onto membrane surface
with improved anti-fouling properties [32]. Porous PVDF membranes
were coated with TiO2 and fluoro-silane compounds to create super-
hydrophobic surfaces for membrane distillation and crystallization
showed a good performance under aggressive fouling conditions [33].
An omniphobic microporous membrane was fabricated by modifying a
hydrophilic glass fiber membrane with silica nanoparticles followed by
surface fluorination and polymer coating. The omniphobic membrane
exhibits an antiwetting property not only against water but also against
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Desalination 424 (2017) 140–148
low surface tension organic solvents [34,35].
The new development in MD membranes involved multiple fabri-
cation steps. Nevertheless, these specially designed membranes still
need long time technological development before being accepted as
affordable membranes. Evaluations were conducted in present works to
evaluate the suitability of low cost commercial hydrophobic in
sweeping gas MD process [36]. Some of the membranes demonstrated
reasonable long term stable operation without a deterioration of its
efficiency [22,37]. However, challenge of these membranes in high
salinity water for extended time has not yet been the focal of research
and systematically investigated. To obtain a relatively high water flux
can be achieved by selecting thin MD membranes, e.g. polytetra-
fluoroethylene (PTFE) membranes [25,38–40]; however, the membrane
with high flux tends to be fouled or scaled at a quicker rate. Desirably a
long time stable MD operation is necessary while maintaining reason-
able flux. One of the core criteria for such application of MD system in
concentrating highly saline water is to build a MD membrane module
with high flux to reduce the footprint, but without sacrificing the
permeate quality by maintaining a high rejection (or low permeate
conductivity). The other important parameter is to reduce the re-
placement cost or chemical cleaning of the MD membrane (or module).
Currently PTFE thin porous membrane has been widely utilized in
sealing, fabrics, air-filter, breathing mask, vapor-breathing membrane
for automotive lighting, etc.; thin PTFE membrane (about 10–20 μm)
has been mass produced at a very low cost (mostly purchased in weight
not in square meters, and a few percent of other commercial hydro-
phobic membranes). Thus, PTFE membrane was one of the first im-
portant candidates for MD module. It is known that the hydrophobic
membrane, once fouled, loses the MD flux and salt rejection. A new
module concept was adopted by laminating the thin PTFE membranes
into a module manifold; the top layer acted as the protecting layer to
the sub-layer; once fouled, the top layer or both could be replaced at a
low cost.
In this work, we presented a fundamental analysis of the perfor-
mance and interesting observation of the laminated PTFE flat sheet
membranes in a bench scale direct contact membrane distillation
(DCMD). The DCMD performance were studied using a model
3.26 mol/L NaCl solution as the feed; at this concentration range, the
conventional reverse osmosis technology is not applicable due to very
high osmotic pressure. The flux and salt leakage were tracked during
the long term DCMD operation. Membrane failures were analyzed using
scanning electron microscopy. The different lamination layers were
studied in the flux and mass transfer resistance. The potential of such
MD module configuration was discussed.
2. Experimental section
2.1. Materials and chemicals
Sodium chloride (AR grade) was supplied by Sinopharm Chemical
Reagent Co. Ltd. and used as received. Deionized water (DI water) was
used in the experiments. Properties of commercial PTFE membranes
were listed in Table 1.
2.2. Characterizations
The pore size (the bubble point, the mean flow, and the smallest
pore size) and gas permeability were measured using a capillary flow
porometry (Porolux 1000) following our previous work [41,42]. The
gas permeability of the membrane was tested at 0.1 bar. The porosity
was assessed gravimetrically. The water contact angle was measured by
a contact angle goniometer (Maist Drop Meter A-100P) using ultrapure
water (5 μL). The morphology of the membrane top and bottom sur-
faces and cross-section was characterized by scanning electron micro-
scopy (SEM) (HITACHI TM-1000). The cross-section samples were
prepared by wetting samples in ethanol and then cryogenically
Y. Chen et al. Desalination 424 (2017) 140–148

Table 1 calculated based on the mass of water transported from feed to

Properties of PTFE flat sheet membranes used in this research.
Property Parameter
Membrane PTFE
Mean flow pore size (μm) 0.248 ± 0.027
Thickness (μm) 11 ± 3
Contact angle (°) 151.7 ± 6.5
LEPw (bar) 3.38 ± 0.21
Porosity (%) 92.3 ± 4.5
Young's modulus (MPa) 0.347 ± 0.203
Tensile strain at breakage (MPa) 21.1 ± 0.6
Elongation at break (%) 280 ± 40
Supplier Sano, China
breaking in liquid nitrogen. All the samples were coated with a thin
layer of gold.
2.3. DCMD experiments
MD performance was evaluated by a bench-scale DCMD and a
schematic diagram of the experimental setup and the membrane mod-
ules is shown in Fig. 1. The effective membrane area was 30 cm2. The
spacer was used to support the membrane and to promote the flow
turbulence (Fig. 1b). Detailed module characteristics used for the MD
process were described in our previous papers [27]. In the DCMD
process, the feed solution and permeate solution were circulated co-
currently. Both feed and permeate solutions were circulated at a flow
rate of 600 mL/min. Feed temperature and the permeate temperature
were maintained constant. DI water and 3.26 mol/L NaCl solution were
used as feed and DI water were used in permeate sides to measure the
fluxes of each membrane at different experimental conditions. To
maintain a constant feed concentration, additional DI water was added
based on the amount of water transferred across the membrane. In case
only one piece of PTFE membrane was used, it was labelled as “single-
layered”. In case two or more layers of membranes were laminated, the
membrane was labelled as “double-layered”, “triple-layered” or
“quadruple-layered”. Multilayered membranes were manually over-
lapped together and mounted into the test module (Fig. 1b).
In some experiments, an over pressure in the feed side was applied.
Referring to Fig. 1a, an extra water tank lifted up 500 mm above the
feed tank was coupled to the system to add an extra pressure between
feed and permeate. The extra pressure acted on the feed side of the
membrane as the external force to prevent formation of air/vapor
pockets between two PTFE layers.
The conductivity and permeate weight were monitored by a trans-
mitter and collected by a computer. The permeate flux (J, kg/m2·h) was
permeate (Δ m, kg) divided by time interval (Δ t, h) and membrane area
(A, m2), as
∆m
J=
A∆t (1)
3. Results and discussion
3.1. Characterization of the membranes
As listed in Table 1, the mean flow pore size and porosity of PTFE is
0.248 μm and 92.3%. LEPw value is 3.38 bar. The contact angle of PTFE
membranes is above 150°, mainly attributed to the open top surface
consisting of nanofibrous-like structure. The PTFE membrane is very
thin, about 11 μm. Thus, very high flux is expected in MD due to low
mass transfer resistance. However, the membrane shows Young's
modulus of 0.347 MPa, tensile strain at breakage of 21.1 MPa, and
elongation at break of 280%. Fig. 2 shows that the membrane is basi-
cally a three-dimensional network structure consisting of knots-threads,
which is typical for stretched membrane.
3.2. Performance of single-layered membrane
Fig. 3 shows the performance of the PTFE membrane in MD using a
3.26 mol/L NaCl solution as the feed. The feed concentration was
maintained constant to avoid the effect of concentration (or possible
formation of scaling). In each cycle, the membrane was tested for
10–12 h and rinsed overnight to simulate the day time when solar
power was available and night time when heating was not available.
For a single PTFE membrane, very stable flux was observed for initial
six cycles: the flux was maintained at 41–42 kg/m2 ∙ h; the permeate
conductivity declined in each cycle, meaning the water permeating
across the membrane contained less salt than the original. This is a
unique characteristic of MD if the membrane is of very high rejection
ratio. In the 5th cycle, slight increase of permeate conductivity was
observed. It was apparent that from the feed channel, part of membrane
became semitransparent (as shown in the inlet picture of Fig. 3a). At
Cycle 7, MD flux dropped to 37 kg/m2 ∙h and black spots were identified
on the membrane surface (Fig. 3b), due to deposition of impurity from
the system during multiple MD operation.
The membrane was taken out of the test cell and rinsed in water to
remove the impurity. After that, the flux was recovered slightly as
shown in the next two cycles. At cycle 11, the quick decline in the flux
was obtained followed by increases in the permeate conductivity. This
may be ascribed to salt deposition on the surface and/or in the pores,

Fig. 1. (a) Schematic illustration of the direct contact membrane distillation process and (b) the flat sheet module and spacer with the dimensions of the test cell [41,43].

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Fig. 2. SEM images of PTFE flat sheet membranes: (a) top and (b) bottom surface of PTFE membrane.

which reduced the overall flux and increased the salt concentration in
the permeate solution. This was a clear indication of membrane wet-
ting, which most probably caused by fouling of the membrane. Results
indicated that single-layered PTFE flat membrane did show high flux,
but unavoidable fouling and wetting limited operation time, although
the feed water was only a NaCl solution.
Deformation of the membrane was observed on the surface. The
membrane was cut into three sections as shown in Fig. 4a. Salt crystals
were observed on the membrane surface, as shown in Fig. 4b–e and Fig.
S1. The water contact angle of 110° was much lower than that of initial
PTFE membrane (151.7°). It was obviously that the salt deposition on
the surface and/or in the pores, leading to the reduction of the overall
flux.
Pore size of pristine PTFE membrane and different parts of single-
layered PTFE membrane after experiment was shown in Fig. 4f. The
pore size of used membrane appeared to be much bigger than that of
pristine PTFE membrane. For example, the bubble point increased from
the initial 0.359 μm to 0.471 μm, 0.530 μm, 0.405 μm in part 1, 2 and 3,
respectively. The same occurred for the mean flow pore size and the
smallest pore size of the three parts on membrane. Table 1 showed that
the Young's modulus of pristine PTFE membrane was low, 0.347 MPa;
this meant that the membrane could yield to the extra force. In the test
module, flow of both feed and permeate was maintained at 600 mL/
min; consequently, turbulence was visualized at the narrow inlet and
the outlet orifice; there the membrane followed a repetitive stretch due
to the external force exerted by the liquid flow. The membrane de-
formation occurred after an extended period of time, consequently re-
sulting in larger pores. The deformation in combination of the thin
membrane and scaling/fouling resulted in wetting of membrane and
losing the MD performance. Thin flexible PTFE membranes showed
advantage in low mass transfer resistance, but disadvantage in yield to
external force.
3.3. Performance of double-layered membrane
The results in Figs. 3 and 4 showed that single-layered membrane
was indeed not yet stable enough in MD even for treating a NaCl salt
solution. Fig. 4 showed that trace contaminants in saline feed might
have strong impact on the membrane wetting and fouling. Fortunately,
the current PTFE membrane was thin and the MD flux was rather high.
Intuitively, if one membrane acts as a protecting layer and the other as
the separating layer, a double-layered membrane would result in more
stable performance. Fig. 5 shows the MD performance of a double-
layered membrane in treating a 3.26 mol/L NaCl solution. A stable
performance was observed with relatively high flux (28–32 kg/m2 ∙ h)
and conductivity of permeate side was in each cycle. Decline in con-
ductivity was an indication that the MD membrane was intact because
the permeate across the membrane was even purer. Results indicated
that double-layered PTFE flat membrane did show quite stable MD
performance, especially compared to single-layered membrane. On the
29th and 30th day, permeate flux declined considerably and con-
ductivity increased sharply.
The membranes were taken out of test cell for autopsy. Fig. 6a
showed that only small part of membrane near the outlet had slight
deformation (in part A). Attempt to separate two membranes was not
easy because the double-layered membranes attached tightly to each

Fig. 3. Permeate flux and conductivity of DCMD at different time for single-layered PTFE flat membrane. Feed and permeate inlet temperature were 60.2 ± 0.5 and 20.9 ± 0.5 °C,
respectively; feed was 3.26 mol/L NaCl solution, and constant concentration was maintained; both feed and permeate inlet velocity were 600 mL/min. Peristaltic pumps were used to
cycle feed and permeate. For each cycle, the membrane module was tested for 10–12 h and rinsed with DI water overnight.

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Fig. 4. (a) The photo of the membrane surface facing feed side after experiment. (b)–(e) SEM images of single-layered PTFE surface after experiment: feed side membrane surface of (b)
Part 1A, (c) Part 1B, (d) Part 2 and (e) Part 3. The insert pictures showed the contact angles of the membrane surfaces. (f) Pore size of pristine PTFE membrane and different parts of
single-layered PTFE membrane after experiment.

other. Salt crystals were observed on the membrane surface, as shown
in Fig. 6b and c. The contact angle of membrane in feed side after test
declined to slightly above 90°, much lower than that of initial PTFE
membrane (151.7°). Deposited foulant matter could be identified in the
surface of the top membrane layer, Fig. S1c, similar to the top surface of
the single-layered membrane; but the top surface of the supporting
layer (Fig. S1e) appeared to be intact. Penetration of foulant across the
PTFE membrane was observed as shown in the bottom surface side of
the single layer membrane (Fig. S1b), which was most probably related
to the wetting and salt diffusion (Fig. 3). Aggregates of foulant matters
were also found in the bottom side of the first layer PTFE membrane
(Fig. S1d), at a significantly much lower scale than that in the single
layer membranes (Fig. S1b). However, almost no salt could be observed
on supporting layer of the double-layered PTFE membrane (Fig. S1e
and S1f).
The double-layered membranes did show significantly improved
performance in test with a relatively high and stable flux. Although
contact angle decreased and scaling appeared on the membrane sur-
face, the membrane facing permeate side still remain intact; therefore,
by replacing the first layer (facing feed side) with a new one, it is ex-
pected to restore the MD performance. Module design for easily
handling is required.
3.4. Air pockets
Interestingly, the flux fluctuated in each cycle (highlighted by red
arrows in Fig. 5). Close observation identified air pockets between two
membranes in operation as shown in Fig. 6e. One of the water drops

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40 25
Flux
Conductivity
20

Conductivity (μS/cm)
30
Flux (kg/m ⋅h)
2

15
20

10

10
5

1 3 5 7 9 11 13 15 17 19 21 23 25 27 29
Cycle
Fig. 5. Permeate flux and conductivity of DCMD at different cycles for double-layered PTFE membrane. Feed and permeate inlet temperature were 60.2 ± 0.5 °C and 20.9 ± 0.5 °C,
respectively; feed was 3.26 mol/L NaCl solution, constant concentration; both feed and permeate inlet velocity were 600 mL/min. Peristaltic pumps were used to cycle feed and permeate.
For each cycle, the membrane module was tested for 10–12 h (whole day), and then was rinsed with DI water overnight.

collected between the two membrane layers after test was about 7 mm.
In the double-layered PTFE membrane, undetermined gap existed be-
tween two membranes due to the high membrane flexibility [44]. When
vapor entries the gap across the top membrane, some would diffuse
across the second and condenses in the permeate, and some would re-
main [45,46]. The gap in the air pockets would create a resistance to
heat transfer, thus it was possible that the temperature gradient in the
area lead to condensation of vapor into liquid. Obviously, the collected
water drops were the result of the condensed water vapor. If the liquid
formed progressively during the experiment, reduction in the MD flux
would be observed due to the blockage of effective membrane area for
vapor transport. This issue is of key importance for large MD modules.
However, at a scale of small test module, we did not observe yet con-
densed liquid between the membrane. If liquid was condensed in the
membranes, the resistance for the vapor diffusion increased due to re-
duced effective membrane area; however, we found that these air
pockets actually assisted the vapor transport. The formation of liquid in
between two membranes did not likely occur. But, it could be due to
limited experimental time or the small module size. The formation of
liquid between laminated membranes would be investigated in the near
future.
Intuitively, this gap between two membranes would lead to extra
resistance because the water vapor would diffuse much longer distance
than across the double thin PTFE membrane. Therefore, an additional
experiment was designed to apply an extra pressure (as the insert pic-
ture shown in Fig. 1a) to the feed so that two PTFE membranes attached
to each other and no air/vapor pockets were seen on the membranes.
Fig. 7a shows that the MD flux of double-layered PTFE membrane
without air pockets was about 14 kg/m2∙ h, half as that of double-
layered PTFE membrane with air pockets (around 30 kg/m2∙ h) under
the same DCMD test conditions.
Fig. 7b illustrated schematically the vapor diffusing in a single-

Fig. 6. (a) The photo of the feed side membrane surface after experiment. SEM images of membrane surface in feed side after experiment: (b) Part A and (c) Part B. The insert pictures
showed the contact angles of the membrane surface. (d) Pore size of pristine double-layered PTFE membranes and Part A of double-layered PTFE membranes after experiment. (e) Droplet
condensed in gap between the double-layered membranes, the diameter is approximately 7 mm.

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Y. Chen et al.
Fig. 7. (a) MD performance of double-layered PTFE membranes in different conditions: with air pockets and without air pockets. Feed and permeate inlet temperature were 60.2 ± 0.5
and 20.9 ± 0.5 °C, respectively; feed was 3.26 mol/L NaCl solution, constant concentration; both feed and permeate inlet velocity were 600 mL/min. Peristaltic pumps were used to
cycle feed and permeate. (b) Schematic diagrams of paths of vapor across the membranes. (c) Different pore sizes of multi-layered membranes.
layered, double-layered (air pockets) and double-layered (closely at-
tached) membrane configuration. Vapor diffused freely across a single-
layered membrane at a high flux (around 40 kg/m2 ∙h, Fig. 3). When
double-layered PTFE membranes were fully overlapped together
(Fig. 7b, the third), overlapping of pore in one membrane to the
polymer in the other membrane is highly probable. This would reduce
the passage for water vapor. However, with air pockets between layers,
a certain amount of air or vapor were collected between the layers,
which helpful to avoid thin sheet closely attached and reduce the ef-
fective transport channels. Moreover, with the existence of air pockets,
pore sizes decreased and might cause the increase of membrane mass
transfer resistance. The mass transfer resistance of the double-layered
membranes with/without air pockets was discussed below:
1) In case of double-layered membrane with air pockets; the dia-
meters of air pockets were in the range of few millimeters, at least 3
orders of magnitude of the thickness of the PTFE membranes. This
means that the vapor had to travel a long distance to go through the air
pockets than through the double-layered membrane without air
pockets. Thus, in average, the water vapor molecules diffuse longer
distance. This was an extra resistance in the membranes with air
pockets.
However, air pockets between two layers constantly shifted and
vibrated with the flow; or the vapor (air) in the pockets were not static,
but moving. This meant extra turbulence existed between the two
layers, which was beneficial to the mass transfer of vapor across the
porous membranes.
2) In case two layers were closed attached; Fig. 7c showed that the
effective pore size decreased. As seen in Eq. 2, the mass transfer re-
sistance (Rm) increased [43,47,48]
1 −1
1 ε ⎡ 3 ⎛ πRTavg ⎞ 2 P RTavg ⎤
= + a
τδ ⎢ 2r ⎝ 8M ⎠ PD M ⎥
⎜ ⎟
Rm
⎣ ⎦
where ε is the membrane porosity, τ is the tortuosity factor, δ is the
membrane thickness, r is mean radius of pore, Tavg is the average
temperature in membrane pores, M is the molecular weight of water, R
Desalination 424 (2017) 140–148
is the gas constant, Pa and P is the air pressure and total pressure.
Since the test module was small and the inlet/outlet temperatures
were well controlled, the membrane intrinsic parameters, the pore size
and the thickness, were key to the mass transfer resistance. The closely
laminated double layer membrane showed low MD flux, most probably
due to the decrease in the membrane pores and increased thickness. For
membrane with air pockets, the membrane intrinsic parameters (por-
osity, tortuosity and thickness) were all changed, even though the same
pore size could be assumed. A quantitative comparison of the mass
transfer resistance of the two cases was not yet available.
Besides, air or vapor showed lower heat conductivity coefficient
than that of polymer membrane [49]. The air pockets between two
layers membrane may help to remain the temperature of hot side and
cooling side, respectively, and keep certain temperature difference
across the feed side and permeate side help to remain a higher driving
force. This might be one possible reason for high flux of double-layered
PTFE membranes with air pockets between two sheets of membranes as
well.
To further verify the hypothesis, pore sizes of single-layered and
double-layered membranes without air pockets were investigated as
shown in (Fig. 7c). In the measurement of the pore sizes, the laminated
membranes were laminated under pressure, thus membrane layers were
closely attached. The bubble point, the mean flow and the smallest pore
size of double-layered membranes were 0.285 μm, 0.222 μm and
0.161 μm, respectively, which were significantly smaller than those of
single-layered membranes (0.359 μm, 0.291 μm and 0.258 μm, respec-
tively). The same trend was also found for triple-layered membranes
and quadruple-layered membranes. These results provided solid sup-
port to the hypothesis in Fig. 7b. The other proof of the reduction in the
pore sizes was demonstrated by the increase in the LEPw of the double
layered membranes: the LEPw was measured to be 4.25 bar, which was
significantly higher than the single layered membrane of 3.38 bar. The
(2)
same trend is expected for the multilayered membranes.
As the number of overlapping layers increased, all of bubble point
pore size, mean flow pore size and smallest pore size of double-layered
membranes declined considerably. Similar results were detected in
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1.0 Experimental water flux
Gas flux
0.8
Normalized flux
0.6
0.4
0.2
0.0
d doi.org/10.1016/j.desal.2017.10.007.
ayered ouble-layered riple-layered druple-layere
Single-l D T Qua
Fig. 8. Normalized MD and gas flux (at 0.1 bar) for multi-layered membranes. DI water
was used as feed solution. Feed and permeate inlet temperature were 60.2 ± 0.5 and
20.9 ± 0.5 °C, respectively, and both feed and permeate flows inlet velocity were
600 mL/min. Experimental water flux and nitrogen gas flux of single-layered PTFE
membrane was 48.1 ± 0.4 kg/m2 ∙ h and 1.38 ± 0.05 L/min ∙cm2. Normalized flux was
the flux of specific layers membrane divided by single-layered water flux or gas flux.
water permeation flux and gas permeability, as shown in Fig. 8. Water
flux declined by 30% and 23% of that of single-layered membranes.
Within the range of the experiment, attempts to increase the sheet
layers would only decrease the fluxes and pore sizes against MD per-
formance. However, as demonstrated in the experiment, the double-
layered membrane showed much longer stable MD performance, it is
expected that the triple- or quadruple-layered membrane would result
in more stable operation. The relationship between the stable MD op-
eration time and the number of the layers was not straight forward.
Recently, Duong et al. [50] reported that increase the temperature
gradient, thus the flux of an air gap membrane distillation process,
resulted in a more severe membrane scaling; one of the main causes was
the increased concentration polarization effect which led to the for-
mation of CaSO4 scaling. Therefore, reduced MD flux of the multi-
layered membranes (Fig. 8) might have advantages in reduction in the
concentration polarization and significant increase in the stable MD
operation time. The negative side of the multilayered membrane is the
large membrane area and relatively large module size and high cost.
The optimal configuration would be defined after considering the MD
flux and time of operation as well as the capital and operational cost.
4. Conclusions
In this study, performance of PTFE flat sheet membrane was ex-
amined during the DCMD process of modeled high salinity brines.
Results indicated that single-layered PTFE flat membrane did show high
flux, but the performance was not stable. This may be ascribed to salt
deposition on the surface and/or in the pores, which reduced the
overall flux and increased the salt concentration in the permeate solu-
tion. By simply laminating two pieces of PTFE membranes together, a
double-layered membrane was prepared. The extra PTFE layer would
serve as a barrier for the potential defects within the membrane, and a
much longer stable MD performance was observed. The MD test results
showed a very stable performance was detected in 28 cycles (days). A
high flux of 30 kg/m2 ∙ h for the double-layered membrane was observed
which was ascribed to the formation of air pockets between two sheets
of PTFE membranes. When two layers were closed attached, the flux
declined more than 50% to 14 kg/m2 ∙h. Results of pore size measure-
ments showed that closely attached double-layered PTFE membranes
have much smaller pore sizes than the original. This explained the re-
duced flux due to the increased mass transfer resistance. Further in-
crease of the overlapping layers will only decrease the fluxes and pore
sizes against MD performance. Challenges to the current membrane
147
Desalination 424 (2017) 140–148
concept are to design an optimal module for an easy access for repla-
cing the top contaminated membrane.
Acknowledgements
The authors would like to thank the partial financial support from
the National Natural Science Foundation of China (Project nos.
U1507117, 21676290), Disney Research Funding (Contract nos.
CA1501).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
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