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Water Desalination Using Carbon-Nanotube-Enhanced Membrane Distillation

Water Desalination Using Carbon-Nanotube-Enhanced Membrane Distillation

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Published:
December 28, 2010
r
2010 American Chemical Society
110
dx.doi.org/10.1021/am100981s
|
 ACS Appl. Mater. Interfaces
2011, 3, 110
114
LETTERwww.acsami.org
Water Desalination Using Carbon-Nanotube-EnhancedMembrane Distillation
Ken Gethard, Ornthida Sae-Khow, and Somenath Mitra*
Department of Chemistry and Environmental Science, New Jersey Institute of Technology, Newark, New Jersey 07102, United States
 ABSTRACT:
Carbon nanotube (CNT) enhanced membrane distillation is presented for water desalination. It is demonstrated that the immobilization of the CNTs in thepores of a hydrophobic membrane favorably alters the water
-
membrane interac-tions to promote vapor permeability while preventing liquid penetration into themembrane pores. For a salt concentration of 34 000 mg L
-
1
and at 80
°
C, thenanotube incorporation led to 1.85 and 15 times increase in
ux and salt reduction,respectively.
KEYWORDS:
desalination, membrane distillation, carbone nanotubes, membraneseparation
INTRODUCTION
Membranedistillation(MD)isawaterpuri
cationprocesswherea heated aqueous solution is passed through the lumen of a poroushydrophobic hollow 
 ber. While preventing the transport of theliquidphase,MDreliesonthenet
uxofwatervaporfromthewarmto the cool side of the membrane. Typically, MD is carried out at60
-
90
°
C,whichissigni
cantlylowerthanconventionaldistillation.Therefore,ithasthepotentialtogeneratehigh-qualitydrinkingwaterusing only low-temperature heat sources such as waste heat fromindustrial processes and solar energy. In general, MD has receivedmuch attention as an alternative to thermal, chemical and reverseosmosisdesalinationofseaandbrackishwaters.
1
-
6
ThedrivingforceformasstransportinMDisprovidedbythevaporpressuredi
ff 
erenceacross the membrane.
7
 A key component in such a process is themembraneitselfbecauseitdeterminesboth
uxandselectivity.Asof now the throughput of MD processes are relatively low, and thedevelopmentof novelmembrane architecture isof greatimportanceto enhance desalination via MD.Recently, we have demonstrated that immobilizing CNTs indi
ff 
erenttypesofmembranesalterthesolute-membraneinteractions, which is one of the major physicochemical factors a
ff 
ecting thepermeability and selectivity of a membrane. Referred to as carbonnanotube immobilized membrane (CNIM), herethe CNTsserve asa sorbent and provide an additional pathway for solute transport.Thesemembraneshavebeenusedinsolventextractionandpervapo-ration
8
and havedemonstrated superiorperformance.
9
Theobjectiveofthisresearchistostudythee
ff 
ectofCNTsontheenhancementindesalination e
ciency via membrane distillation (MD).
EXPERIMENTAL DETAILS
The membranemodules for MD were constructed in a shell andtube format using 1/4 in. tubing and threaded brass pipe
ttings.Thirty-six, 6-in. long hollow 
 ber strands were used in the module.Each module contained approximately 0.21 cm
2
of e
ff 
ective mem- brane contact area (based on
 ber internal diameter). The ends were then sealed with epoxy to prevent leakage into the shell side. Vacuumwasappliedtoonedrainporttodrawairthroughtheotherport, which created a higher pressure di
ff 
erential and provided asweep air. Air
ow wasregulated atarateof1 L min
-
1
. TheCNIM was prepared using Celgard type X-50 (Celgard, LLC, Charlotte,NC, USA) hollow 
 ber as the starting material. The process was asfollows: ten milligrams of multiwall nanotubes (Cheap Tubes, Inc.,Brattleboro, VT, USA) were dispersed in a solution containing0.1mgofpolyvinylidene
uoridein15mLofacetonebysonicatingforanhour.ThePVDF/CNTsdispersionwasforcedundervacuumintotheporestructureofthepolypropylenemembrane.TheCNIM wasproducedduringthisstepandthePVDFservedasgluethatheldthe CNTs in place. The membrane was
ushed with acetone toremove excess CNTs and PVDF. Membrane morphology wasstudied using scanning electron microscopy (Leo, model 1550)and thermo gravimetric analysis (TGA) was performed using aPerkin-Elmer Pyris instrument.Theexperimentalsystemisshown in Figure2.Thesaltmixtureused in these experiments contained 88% NaCl and 12% MgSO
4
.Thesolutionstested rangedfrom10 to34000 mgL
-
1
. The waterto be treated was pumped through the module using a HPLCpump. The solution traveled through a heat exchanger whichallowed itto beheated to the desired temperature. Asthe solutiontraveled up the module, the permeate was discharged through thedrainportandcollectedinavacuumtrap.Theionicstrengthoftheoriginalsolution,thepermeateandtheconcentrateweremeasuredusing an Oakton EC Testr 11
þ
multi range conductivity meter. All experiments were repeated in triplicate and the relative
Received:
October 12, 2010
 Accepted:
December 13, 2010
 
111
dx.doi.org/10.1021/am100981s |
 ACS Appl. Mater. Interfaces
2011, 3,
110–114
ACS Applied Materials & Interfaces
LETTER
standard deviation of these measurements was found to be lessthan 5%.
RESULTS AND DISCUSSION
Scanning electron micrographs of the original membrane andCNIMareshowninimagesaandbinFigure1.Theincorporationof CNTs is clearly evident, and the CNTs were found to be uniformly distributed. The TGA is presented in Figure 1c. This indicated thatthe CNIM contained approximately 0.5% CNTs by weight. It wasalso observed the presence of CNTs enhanced the thermal stability of the membrane by increasing the onset of thermal degradation by as much as 29
°
C. This is an important factor for MD, where theelevated temperatures can a
ff 
ect the membrane material.The proposed mechanisms of permeation in the presence of CNTs are shown in Figure 3. Immobilizing the CNTs in thepores alters the water
-
membrane interactions, which is one of the major physicochemical factors a
ff 
ecting the permeability andselectivity of the membrane.
10
Because CNTs are highly hydro-phobic, they decrease the tendency of a pore to become wet withliquid, so higher transport of pure vapor can occur. It is well-known that gas
ow across a membrane pore follows Knudsen,Fickian, or molecular di
ff 
usion
11
-
13
. Because CNTs are knowntohaverapid sorption anddesorptioncapacity,
14
-
16
itispossiblethey allow thewater vapor molecules to follow asurfacedi
ff 
usionpattern, in which the solute hops from one site to another by interacting with the surfaces. This action may increase overall vapor transport. The CNTs can also provide an alternate routefor fast mass transport via di
ff 
usion along their smoothsurface
17,18
. The water vapor may also be transported directly through the inner tubes of the CNTs, which are known toenhance vapor transport.
19
It is also well-established that CNTs have high thermalconductivity, which is a signi
cant factor.
20
The higher thermalconductivity of the CNTs reduces the temperature gradient inthe membranes, thus reducing condensation and allowing more
Figure 1.
(a, b) SEM images of the original membrane and the CNIM. (c) Thermal gravitational analysis of the plain membrane and CNIM.
Figure 2.
Schematic diagram of the experimental setup.
 
112
dx.doi.org/10.1021/am100981s |
 ACS Appl. Mater. Interfaces
2011, 3,
110–114
ACS Applied Materials & Interfaces
LETTER
 vapor to permeatethrough the pores. Thecondensation of wateris known to reduce the hydrophobicity of the membrane leadingto the attraction of more water molecules, which may eventually lead to pore clogging. The presence of CNTs reduces thesee
ff 
ects. The relatively uniform temperature distribution leads tohigher temperature in the permeate side of the membrane andlowers the surface tension
21
in the pores, thus allowing easiertransport of water vapors.MD experiments were carried out in the range of 60
-
100
°
C.For both membrane types, the salt reduction and
ux increased with temperature up to 80
°
C. There was a leveling o
ff 
and evenslight reduction at higher temperatures. This data is shown isFigure 4a. The absolutelevel of salt reduction and
ux per cm
2
of membrane was higher for CNIM at all temperatures. Theincorporation of CNTs generated higher salt reduction and
ux at signi
cantly lower temperatures. The e
ff 
ect was most pro-nounced at lower temperatures. For example, at 60
°
C and 0.5mL min
-
1
feed
ow, the salt reduction using CNIM was 6 timeshigher and was nearly the same as that accomplished at 90
°
Cusing the conventional membrane. Both salt reduction and
ux reached their peaks at 80
°
C when the CNIM was used. The datademonstrate that CNIM can provide signi
cantly higher eco-e
ciency,becausemorepurewatergenerationcanbecarriedoutat a signi
cantly lower temperature.Desalination as a function of 
ow rate is shown in Figure 4b when feed solution temperature was at 80
°
C. In the
ow raterangestudied,inbothcases,thesaltreductionand
uxpercm
2
of membrane decreased with
ow rate. Compared to the conven-tional membrane, the CNIM demonstrated signi
cantly higher
uxandsaltreductionatallfeed
owrates.Fluxdoubledintheinthe presence of CNTs and salt reduction increased
 ve times.This is attributed to some of the reasons mentioned above,especially the fact that the CNTs serve as sorbent sites for vaportransport while rejecting the liquid water because of its highhydrophobicity. Improvement in salt reduction was observed atall
ow rates, which ranged from 1.4 to 4.7 times higher. TheionicradiusofNa
þ
andCl
-
are1.02and1.81Å,respectively.
22
Itis well-known that during reverse osmosis, water clusters exceed-ing four molecules can transport salt ions through the polymericmembrane.
23
Becausetheporesherearesigni
cantlylarger(0.04
 μ
m), the salt permeation inthe membranes occurs mainly due tothe entrainment of 
ne liquid droplets in the vapor phase.Therefore, itisconcluded that theenhancement insalt reductionin the presence of the CNTs is due to the relatively higher vapor
ux and the rejection of water molecules due to higher hydro-phobicity. The higher
ux and salt reduction have practicalrami
cations because they lead to signi
cantly higher e
ciency processes. Higher salt reduction can be attained at higher
ow rates, thus requiring less membrane material and energy per unitof water treated.It is well-known that salt reduction in membrane processesdecreases with increased salt concentration.
24,25
This wasmeasured as a function of salt concentration and the data ispresented in Table 1. The measurements were carried out at a
ow rate of 0.5 mL min
-
1
and 80
°
C. These measurements weremade in triplicate and represent a relative standard deviation of less than 5%. The results showed a substantial decrease in
ux (25%) for the plain membranes as the salt concentration wasincreasedfrom10to34000mgL
-
1
.Thisphenomenonhasbeenreported before.
26,27
On the other hand, the CNIM showed noappreciable decrease in
ux, most likely due to the hydrophobicnature of the CNTs, which prevented the liquid phase penetra-tion into the membrane. Also, the salt reduction capability of CNIMwassigni
cantlyhigheratallconcentrations.Thesevariedfrom 99 to 15%, while in the plain membrane it was 71 to 1%.This indicates that the CNIM was less susceptible to salt bleed-through than the standard membrane. Once again, this isattributed to the CNIM's ability to selectively allow the passageof water vapor.
MassTransferinthePresenceofCarbonNanotubes.
The water vapor flux 
 w 
through the membrane is given by 
28
 J 
 w 
¼
ð
L
-
 V 
Þ ð
1
Þ
 where
is the mass transfer coefficient and
L
and C
 V 
are theliquidandvapor-phase concentrations.
L
istheconcentrationof the exit stream (in mg L
-
1
) after the removal of the vapor phase,
Figure 3.
Mechanisms of MD in the presence of CNTs.
Figure 4.
(a) E
ff 
ect of temperature on salt reduction and
ux at a feed
ow rate of 0.5 mL min
-
1
; (b) e
ff 
ect of 
ow rate on salt reduction and
ux at 80
°
C.

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