m. pontié*, a. thekkedath, s. plantier, j.b. castaing, a. massé, p. jaouen new seawater...
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M. Pontié*, A. Thekkedath, S. Plantier,
J.B. Castaing, A. Massé, P. Jaouen
New seawater pre-treatment by ultrafiltration (UF) operation
intensification
Laboratory GEPEA, UMR CNRS 6144, 37 bd. de l’Université, 44602 Saint-Nazaire, France
Session : l-6 Product related filtration and separation. Water
EUROPEAN CONFERENCE ON FLUID PARTICLE SEPARATION (ECFPS) 5 - 7 october 2010, Lyon - FRANCE
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One of the critical issues in the successful application of
membrane systems for water treatment is the adhesion of
foulants to the membrane surface following by a cake
elaboration*.
The dramatic wellknown consequence is a decline in permeate
flow followed by an increase in operational and maintenance
costs.
Main aim : investigate the possibilities of de-organized
the cake by insertion of large size clays particles.
*A. THEKKEDATH, M. PONTIE, C.R. Chimie 10 (2007) 803- 812.2/17
General introduction
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3/17
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M. Pontié et al. Desalination 204 (2007) 155-160
UF less susceptible to fouling than MF
4/17
Why Ultrafiltration ?? J
/J0
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Membranes
(Millipore)
Material MWCO
YM 100,
30, 10
Regenerated cellulose,
Flat sheet
100 kDa
30 kDa and 10 kDa
5/17
200 nm
SEM image of the 100 kDa surface morphology (2D-FD :1.90)
N2
Permeate
manometers
Membrane
Filtration cell
+ -Millivoltmeter
Ag/AgClelectrode
Ag/AgClelectrode
N2
Permeate
manometers
Membrane
Filtration cell
N2
Permeate
manometers
Membrane
Filtration cell
N2
Permeate
manometers
Membrane
Filtration cell
Membrane
Filtration cell
Membrane
Filtration cell
+ -Millivoltmeter
Ag/AgClelectrode
Ag/AgClelectrode
Dead-End filtration cell in a bench scale
lab. pilot (membrane area 29 cm2)
Experimentals Membranes and bench scale unit
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Humics characteristics
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
Mea
npar
ticl
esiz
e(nm
)
(mV
)
0
Mean particle size (nm)
Zeta potential
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
(mV
)
0
(mV)
Zet
apote
nti
al
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
Mea
npar
ticl
esiz
e(nm
)
(mV
)
0
Mean particle size (nm)
Zeta potential
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
(mV
)
0
(mV)
Zet
apote
nti
al
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
Mea
npar
ticl
esiz
e(nm
)
(mV
)
0
Mean particle size (nm)
Zeta potential
-20
-40
20
40
-60
0
3 4 5 6 7 8 9 10 11 12 1321
pH
500
1000
1500
2000
2500
(mV
)
0
(mV)
Zet
apote
nti
al
Acrôs
The distribution of mean particle size (nm) and zeta potential (mV) for Acros humic acid (5 mg/L) at pH=6.2 (Zetasizer Malvern Co.) :
• Average particle size (250 nm)• Charge (-30 mV)
6/17
O
O
N
O
O O
H
HN
CO
NR
N O
OH
O
OH
OO
HO CO2H
CO2H
OH
OH
OH
CO2H
CO2H
OH
R
CO2H
humic acid model structure (Stevenson, 1982)
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pillared clay Inorgano clay
Montm-Na Natural clay (BENTONITE)
Na.xH2O
INTERCALATIONCALCINATION
Pillars Micropore
Mont-CTAB
CTAB ADSORPTION
SEM images of Mont-Al -CTAB (2 nm C deposition, beam
energy 3 keV, and the magnifications x500 and x10,000)
Relative elementary composition analysis of Mont-Al(C) from EDX (excluded C) Na Mg Al Si Cl K Ca Fe
% 1.31 2.56 34.26 56.51 ----- 2.31 ------ 3.31
SEM images show microporous surface with aggregates (average size of 3 m±2)
Mont-CTAB preparation steps
M.W. NACEUR et al. Desalination 168 (2004) 253-258 7/17
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Modified fouling index for ultrafiltration (MFI-UF)
V (L)
t/V
(s/
L)
SCHIPPERS J. C., VERDOW J, Desalination 32 (1980) 137
t/V vs. V graph to determine MFI-UF and a humic acid cake formed on a PES membrane
Purely based on cake formation Fouling potential of the feed solution Directly dependent on the concentration of particles More reliable than SDI (silt density index)
VSPI
Vt .
.2.
P.SR.
2m
+
= µµ
MFI
8/17
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• Image J software is used to determine the fractal dimension from SEM images• From the original image, a threshold (binary) image is generated• Fractal box count method is applied• The slope of the log N (count) vs. log (size) plot is used to get fractal dimension of the image. The absolute value is taken as the FD.
FD = 1.57
log N = -(FD). log
Original and threshold images MANDELBROT B. B., The Fractal Geometry of Nature, Freeman, San Francisco, 1982. 9/17
Determination of cake Fractal Dimension (FD)
Particle-cluster aggregation (Diffusion-limited aggregation)
2D-FD = 1.5 to 1.75
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0,00
0,20
0,40
0,60
0,80
1,00
1,20
0 0,5 1 1,5 2 2,5
cumulated volume, V(L)
No
rmal
ized
flo
w, J
/J0
100 k Da 30 kDa 10 kDa
Acros HA, constant pressure of 2 bars pH 6.7 and 5 mg/L HA
.
Tighter membranes show lower flux decline
Role of membrane MWCO
10/17
Results and discussion
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SEM images of cakes with and without Mont-CTAB - 100 kDa
HA alone HA + Mont-CTAB
11/17
Rm x 10-12 m-1 = 0.67
R HA +Mont-CTAB x 10-12 m-1 = 0.45
RHA x 10-12 m-1 = 1.67
Rcake decreased 3 times in presence of Mont-CTAB
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Intensification of UF-100 kDa with Mont-CTAB
0,00
0,20
0,40
0,60
0,80
1,00
1,20
0 0,2 0,4 0,6 0,8 1 1,2
Cumulated volume, V(L)
Norm
aliz
ed F
lux,
J/J
0
HA HA + Bentonite
12/17
20%
Less fouling occured with Mont-CTAB particles and a GAIN IN FLOW of 20 % was observed
MFI decreased 2 times in presence of Mont-CTAB
0
500
1000
1500
2000
2500
3000
0 0,2 0,4 0,6 0,8 1 1,2
Cumulated volume, V (L)
t/V (s
/L)
HA HA + bentonite
MFI : 1358 ± 140 s/L2 594 ± 60 s/L2
THEKKEDATH A., PhD Thesis, Angers University (France), (2007)
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bentonite Humic Acid
1.57
1.45
HA alone
HA + Mont-CTAB particles
FD of cake surface imaging with and without Mont-CTAB
2D- Fractal dimension
13/17
FD decreases in presence of Mont-CTAB showing a more porous cake
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FD, MWCO and Hydraulic permeability
1,5
1,55
1,6
1,65
1,7
1,75
1,8
1,85
0 20 40 60 80 100 120 140 160 180
Permeability
FD
(L. m -2. h -1. bar -1)
1,5
1,55
1,6
1,65
1,7
1,75
1,8
1,85
0 20 40 60 80 100 120 140 160 180
Permeability
FD
(L. m -2. h -1. bar -1)
100 kDa 1.57 155
30 kDa 1.62 83
10 kDa 1.82 20
MWCOFD
(Fouled membrane)Permeability (L.h-1.m-2.bar-1)
(Fouled membrane)
FD values were in a decreasing trend with increasing MWCO Higher value of permeability corresponds to a lower value of FD or a more porous cake.
1,5
1,55
1,6
1,65
1,7
1,75
1,8
1,85
0 20 40 60 80 100 120
MWCO (k Da)
FD
14/17
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Less fouling occured in UF in presence of Mont-CTAB particles with :
- a gain in permeate flow of 20%
- a lower cake resistance and a lower MFI
- a lower FD (NEW RESULT) meaning a more porous cake
Opening interesting perspectives for the intensification of UF as seawater pre-treament before RO.
15/17
Feed tank (Sea water)
Permeate
Feed Tank (adsorption+ coagulation)
Feed pump Membrane UF
Rejection water
Feed pump
Coagulant injection by peristaltic
Lamellar settler
UF submerged Hollow Fibers + Mont-CTAB
Conclusion and perspectives
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16/17
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Acknowledgements
Lots of thanks to my young collaborators : A. THEKKEDATH, H.
DACH, F. DE NARDI, K. KECILIMERCI to Nourredine Nghaffour
(KAUST) 16
www.gepea.fr
17/17
MEDRC : Project n° 06-AS-003 (Sultate of Oman) AWWARF for funds to A. Thekkedath thesis Blida University (Algeria), M.W. Naceur LCME, Poitiers (France), B. Legube Microscopy Dept. (SCIAM), Angers university, (France), R. Filmon
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Low pHpH 3 Coiled, compact configuration Severe flux decline
Chemical conditions NOM in solution NOM on membrane surface
Role of pH
High pH Stretched, linear configurationpH 9.5
Lower flux decline
• At basic pH, a thin and loosely packed cake layer• At acidic pH, a dense and compact cake layer
HONG S. and. ELIMELECH M, J. Membr. Sci. 132 (1997) 152 A1
Annexe