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, 3, 19, 2010
Drinking Water
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Author(s) 2010. This work is distributed under Engineering and Science
the Creative Commons Attribution 3.0 License.
Abstract. The paper gives an overview of the methods for removal of natural organic matter (NOM) in wa-
ter, particularly humic substances (HS), with focus on the Norwegian experiences. It is demonstrated that
humic substances may be removed by a variety of methods, such as; molecular sieving through nanofiltration
membranes, coagulation with subsequent floc separation (including granular media or membrane filtration),
oxidation followed by biofiltration and sorption processes including chemisorption (ion exchange) and physi-
cal adsorption (activated carbon). All these processes are in use in Norway and the paper gives an overview of
the operational experiences.
Fig.
Figure 1. Typical
1. Typical flow and
flow diagram diagram
picture ofand picture of
a nanofiltration a nanofiltration
plant for NOM removal. plant for NOM removal
Since
Since thethe
colourreduction
of the water ofiscalcium and bicarbonate
a major concern for users concentration
In order to prevent through
capacitythe membrane
reduction over time filter is
as a result
about 15-30
in Norway, emphasis %,willanbealkaline
given to filter
colour(calcium
(mg Pt/l) ascarbonate)
a is often
of membrane included
fouling, in ordercleaned
the membranes to increaseby two the
differ-
NOM level of calcium and bicarbonate in the typically soft and corrosive Norwegian water.
characterization parameter in this paper. Typical re- ent cleaning procedures: a frequent (daily) cleaning (chem-
lationships between colour, DOC and UV-absorption for the ical rinse) and a main cleaning that is carried out once or
Norwegian raw waters referred to in this paper are: twice a year. In the daily cleaning, that normally lasts for
In order to prevent capacity reduction over time as a result of membrane fouling, the
about an hour and takes place during night, a chemical solu-
DOC (mg C/l) = 0.120 Colour (mg Pt/l) + 1.0 (R =0.935)
membranes cleaned by two 2
different cleaning procedures:
tion, also containing an a oxidant
frequent (daily)
(normally chlorine)cleaning
for disin-
DOC (mg C/l) = rinse)
(chemical 0.241 UVabs. main+ 0.4
and a (1/m) (R =0.997)
cleaning
2 that is carried out onceis pumped
fection purposes, or twice intoathe
year. In the
membrane dailyand
module
cleaning, that normally lasts for about an hour and takes place during night, a chemicalout.
circulated here for 2030 min after which it is pumped
solution, also containing Raw water is then lead through the membrane module for
2 Membrane (nano) filtration an oxidant (normally chlorine) for disinfection purposes, is pumped
rinsing for 2040 min before the plant is again put into op-
into the membrane module and circulated here for 20-30The
eration. minutes
plants areafter
fullywhich
automatedit isandpumped
the operatorout.has
Research on membrane filtration (nano/ultra-filtration)
Raw water is then lead through the membrane module for
only to seefor rinsing
to that there arefor 20-40amounts
sufficient minutes beforeso-
of washing
the removal of humic substances was started at the university
the plant is again put into operation.
in Trondheim around 1975 (degaard and Kootatep, 1982)
The plants are fully
lutions and automated
that the pressuresand inthe operator
the plant has
are as intended.onlyThe
and tothesee
first to that there
full-scale plant wasare put
sufficient amounts
into operation in 1990. of washing solutions and that the pressures in theper
main cleaning is normally carried out a couple of times
year coupled to a general service of the plant by the contrac-
Sinceplant
then are as intended.
membrane filtration hasThebecome
mainvery cleaning
popular is in normally carried out a couple of times per year
tor. The washing chemicals may contain wetting agents (ten-
Norway
coupledand moreto than 100 nanofiltration
a general service (NF) of theplants are inby the contractor. The washing chemicals may
plant sides, phosphates etc.), sequesters (phosphates, EDTA etc.),
operation at this time. Most of the plants are small, the largest
contain wetting agents (tensides, phosphates oxidation
etc), sequesters (phosphates,
chemicals (peroxides, EDTA
chlorine etc.) etc),
and enzymes
plant having a design flow of 16 000 m /d. 3
oxidation chemicals (peroxides,
All the Norwegian NF plants are based on spiral wound chlorine etc) and enzymes
(degaard et (degaard
al., 2000). et al, 2000).
modules and the majority on cellulose acetate (CA) mem- The NF process is often selected when the NOM-
Thewith
branes, NF aprocess
few exceptionsis often selected
based when (PA)
on polyamide the NOM-content/color
content/color is highis (>30 highmg(>Pt/l)30 andmg turbidity
Pt/l) andlow
membranes.
turbidityThelow typical
(< pore size of the
1 NTU). Themembranes
most typical is 1 problems
(<1 NTU). encountered
The most typicalare problems
thoseencountered
connected are those
to
5 nm (10002000 Da) operated at a pressure of 48 bar (de- connected to capacity loss caused by fouling. In most cases
capacity loss caused by fouling. In most cases this is either caused by too high design flux
gaard et al., 2000). The typical flow diagram of a membrane this is either caused by too high design flux relative to the
relative
filtration plantto the characteristics
is shown in Fig. 1. The raw ofwater
the water
passes firstin question, especially
characteristics of thetoowaterhigh flux forespecially
in question, waters too with high
higha pre-treatment
through particle concentration
unit, normally aand high NOM-content.
micro-sieve with a flux for Model
waters with calculations
high particlemade by Thorsen
concentration and high
sieve(1999)
openingindicated
of typicallythat 50 m.
particles
After theinsieve,
the size range ofNOM-content.
the pres- about 0.1 Model 3 mcalculations
are particularly
made by critical for
Thorsen (1999)
surefouling.
is raised up to the operating pressure of the membrane indicated
Thorsen and Flgstad (2006) demonstrated when using a lab scale plant (flux that particles in the size range of about 24m
0.13
unit by a 2circulation pump. Cross-flow filtration takes place are particularly critical for fouling. Thorsen and Flgstad
L/m h) on a colored surface water that the permeability decline was 31 % over a 700 hrs
in the membrane unit resulting in a cleaned water stream (the (2006) demonstrated when using a lab scale plant (flux 24
periodthatwhen
permeate) usingthrough
has passed a 100them pre-filter
membrane and before
a dirty the L/mspiral
2
h) onwound
a coloredNF membrane
surface water thatand almost thede-
the permeability
watersamestreamwhen using a 5 that
(the concentrate) mpasses
prefilter, whilevalve
a reduction it wascline
close wasto31%0% overwhen
a 700 husing
periodawhen
0.1 using
m aprefilter.
100 m pre-
This demonstrates the importance of correct design relative to the water characteristics.
bringing the pressure in the concentrate back to that of the filter before the spiral wound NF membrane and almost the
atmosphere. Some of the concentrate is recycled to the inlet same when using a 5 m prefilter, while it was close to 0%
in order to increase the recovery. when using a 0.1 m prefilter. This demonstrates the im-
Since the reduction of calcium and bicarbonate concentra- portance of correct design relative to the water characteris-
tion through the membrane filter is about 1530%, an alka- tics. Practical full-scale experiences show that the best spiral 4
line filter (calcium carbonate) is often included in order to wound membranes can be operated for weeks with an almost
increase the level of calcium and bicarbonate in the typically constant flux up to 20 L/m2 h (Thorsen and Flgstad, 2006)
soft and corrosive Norwegian water. and the design flux recommended is therefore in the range of
Table 1. Recommended pH and dose using alum (ALG), iron (JKL) or chitosan (Chi) in contact filtration of raw waters at color levels of 15,
ION/FILTRATION
30 and 50 mg Pt/L (Eikebrokk, 2001).
Raw water colour Raw water SUVA Recommended specific coagulant dosage and
coagulation/floc separation L/mg methodCm (see Figure
pH mmol Me2)or is globally
mmol probably
Chi/gTOC; (g the
Me or g Chi/mgPt)
ALG pH 5.86.6 JKL pH 4.05.5 PAX pH 5.76.7 CHI pH 5.06.0
sed method for NOM substance removal. Principally it is constructed in a
RW15 3.8 16 (78) 16 (162) 14 (67)
nts for turbidity removal.
RW30
Since 4.3
Norwegian 20 (63)
lake water 20 (128)
commonly 17 (54)
is low0.6 in(110)
0.7 (80)
e compact flow diagrams RW50 (direct-
4.8 or contact
26 (61) filtration),
26 (100) are dominating
20 (49) in(70)
0.8
ventional processsulphate,
ALG-aluminium is JKL-ferric
used only when aluminium
chloride; PAX-poly turbiditychloride;is higher than normal.
Chi-Chitosan.
For Me-coagulants: Dose levels needed to obtain <0.1 mg residual Me/L, >90% and 5060% colour and TOC reduction Absolute minimum
n units (flotation and microsand ballasted lamella sedimentation) before the
doses are 25% lower than the given practical minimum doses.
when theForconventional
Chitosan: Dose levelsprocess is >60%
needed to obtain used. and 2035% colour and TOC reduction, resp.
Ca(OH)2
c- Settling/ Filtration
on flotation
CO2
Raw water
Anthracite,d60=1,5 mm 50cm
Flocculant (Polymer)
Sand, 1-2mm Sand,d60=0,6 mm 30cm Treated water
Gravel, 2-5mm 3x10cm
Coagulant Gravel, 5-10mm
support
(Al or Fe) Chlorine
Introduction
Figure 3. Typical flow scheme for a contact filtration plant for NOM removal in Norway.
n/floc separation Fig. 3. Typical flow scheme for a contact filtration
plant dose:
Minimum required coagulant for NOM
Dose (mg removal
Me/L) = A in3.1
Norway
Alternative filter configurations
Raw water Colour (mg Pt/L) + B where A and B are constants
depending on the coagulant and operational conditions. For The two-media anthracite/sand filter is most commonly used
rmally carried
alum A was out found byto be the
0.043 addition of aluminium
and for iron 0.107, while B filter sulfate,
configuration,prepolymerised
as shown in Fig. 3. An alternative two-
de of iron chloride as coagulants. The primary NOM-coagulation
was found to be 0.30 for alum and 0.58 for iron. The practical media configuration is the one based on, Filtralite (Fig. 4),
minimum dose was recommended to be 25% higher than this. a lightweight expanded clay media produced in Norway. By
) complexation of NOM with dissolved metal
Sludge production at optimum coagulation: SS
coagulant
using Filtralitespecies (Al or
of two different grainFe),
sizes and densities, a
precipitation
(mg/L) = of
SSRWa+ kMe-NOM
Dose where SSRW solid phase, solid
is the suspended coarse-to-fine media
b) complexation of NOM with filter is established.
concentration in the raw water including the contribution Saltnes et al. (2001, 2002) demonstrated in a Filtralite filter
ant species, leading
from additional processestolikeadsorption
pH- and corrosion of this
control, k complexed
with coarse grains (see material onto high sludge
Fig. 4) and consequently
H)3 solids, and c)
is a constant directonadsorption
depending of NOM
the type of coagulant and Dose isontostorage
the surface
capacity/longof precipitated
filter runs, that bigger grain sizes could
the coagulant dose (mg Me/L). For alum and ferric chloride be compensated for by increasing filter depth, especially
he coagulation
as coagulant,of k iswaters
found to becontaining both particles
4.2 and 2.5 respectively when and
usingNOM
a polymerbecomes
as filter aid. more
ving several important
Filter run time to break factors: a) thecoagulation:
through at optimum dissolved coagulant species
Because of the need present
for corrosion control, an alternative
tBT = a (vf SS)b where tBT is time of filtration until break- filter configuration has become popular in Norway, where
ddition, through
b) the presence of precipitated metalcalcium
(h), vf is rate of filtration (m/hr), SS is the suspended
hydroxide solids, c) the
carbonate is used as the bottom media in a down-
articles solids
andconcentration
NOM, d) the chemical
in coagulated properties
water, i.e. sludge produc- of these
flow contaminants
three media andanthracite/sand as
filter with conventional
tion (mg SS/L), and a and b are constants specific to the filter the upper media (Fig. 5) (degaard, et al., 1999). Floc sepa-
th dissolved coagulant species, and e) the pHration
and coagulant. For alum without any polymer as filter aid
of takes
coagulation, which is
place in the anthracite/sand part of the filter while
mistry ofand the
SSRWcoagulant
= 0, the time ofand thehas
filtration water alkalinity
been found to be: (Eikebrokk et al,
the calcium carbonate part2006).
has the function of carbonation.
tBT = 298 (vf DoseAl )
1.29
. Most of these plants use iron chloride as coagulant (typical
portant Drink.
factorsWaterin
Eng.order to 2010
Sci., 3, 19, achieve optimal coagulation, flocculation and
www.drink-water-eng-sci.net/3/1/2010/
tachment and retainment on the filter grains, are the coagulant dosage and
H (see Table 1).
nded clay media produced in Norway. By using Filtralite of two different
Specific ozone dose (mgO mgPt ) -1
F/F+
178
ensity, AS anthracite/sand,
sity F/F Filtralite/Filtralite
FL NC Filtralite normal density,
FL NC
F/F FL HC Filtralite high density
1,6-2,5 FL NC
mm A/S F/F
1,6-2,5
Filter depth (cm)
95 mm
FL NC
1,6-2,5 FL NC
mm 60 Anthracite
1,6-2,5
0,8-1,6 mm
FL HC
mm
FL HC 47
0,8-1,6 FL HC
0,8-1,6 35 mm Sand FL HC
0,8-1,6
mm
0,4-0,8 0,8-1,6 mm
mm mm
Support 0 Support
layer layer
Support Support Support
layer layer layer
-30
Figure6 Figure 6. The continuous, uplow (Dynasand) filter.
-multi Filtralite Fig. 5 The three media filter Fig. 6 The continuous,
Figure 4. The mono-multi Filtralite filter.
Fig. 4 The mono-multi Filtralite Fig. 5 The three media filter Fig. 6 The con
for coagulation/carbonatisation
washinguplow (Dynasand)
in order to ensure the properfilter
grain grading at the
filter forstart
coagulation/carbonatisation uplow (Dynasa
of a new filtration cycle. In the three media filters a typ-
ical back-washing routine is composed of 3 min water back-
01, 2002) demonstrated in a Filtralite filter withwash
coarse
at 6080grains (see
m/h, 3 min Figure
backwash 4)(together with
with air
Saltnes et al (2001, 2002) demonstrated in
water) a Filtralite
and finally 6.5 min filter with
water backwash. coarse grains
Overall this re- (see
y high sludge storage capacity/long filter runs, that bigger grain sizes could be
and consequently high sludge storage capacity/long filterwater
sults in quite high backwash runs, that bigger
consumption, grain size
in the range
by increasing filter depth, especially when usingofa611%
polymer(degaardasetfilter aid.
al., 1999).
compensated for by increasing filter depth, especially when using a polymer as filter
Another filter that is much used in Norway in contact fil-
tration plants for NOM-removal is the continuously operated
need for corrosion control, an alternative filter filterconfiguration
the so-called Dynasand hasfilterbecome
(see Fig. 6).
Because of the need for corrosion control, an alternative filter configuration ha
way, wherepopular
calciumincarbonate is used
Norway, where calcium carbonate
as the bottom media in a down-flow
is used as the bottom media in a d
3.2 Coagulation/membrane filtration
r with conventional anthracite/sand as the
three media filter with conventional anthracite/sand upper media (Figure as 5)the (degaard,
upper media (Figure 5) (
c separation takes place in the
et al, 1999). Floc separation takes placeanthracite/sand part
There is nowof anthe
in theafter filter
increasing while
interest
anthracite/sand the
in replacing the granular
part (ultra-
of the
media filtration coagulation with membrane or filter
e part hascalcium
the function of carbonation.
carbonate part has the functiononof Most of these
micro-) plants
filtration.
carbonation. use
At this iron
time only chloride
one full scale
Mostchloride)/hollow plant
of these plants based use iro
pical dosage 3.3-5 mg Fe/l) in order
as coagulant (typical dosage 3.3-5 mg (10 to reach the operating
coagulation (poly
Fe/l) in order
nm) membrane
pH of 3.5-4,0
aluminium
to reach
filtration
that
the isoperating
(Xiga, Norit)
fibre UF
in operation inpH of 3.
ure sufficient dissolution
is 5.required tofilter of
ensure the CaCO 3 . In
sufficient dissolution some of
Norway. these
It has aplants CO
stable operation
of the CaCO3. In 2 atis added
a flux of 80 L/m2 h at 90%
some of these plants CO
Figure The three media for coagulation/carbonatisation. recovery on a raw water with color 40 mg Pt/L. The plant is
y 6-15 mg/l) in order to minimize the
as well (typically 6-15 mg/l) in order backwashed iron dosage. pH,
to minimize grain size
the(and
with treated iron as well water
dosage.
chlorinated)
as pH, grain size
and chem-
uence the contact
dissolution of the marble in order to arrive
ical cleaningat(75%the
time influence the dissolution of the marble in order to arrive at the comb combination
phosphoric acid, soakingof for 20 min and
dosage 3.35 mg Fe/l) in order to reach the operating pH of 15% sodium hypochlorite, soaking for 15 min) is performed
3.54.0 that is required to ensure sufficient dissolution of the every 8th backwash.
CaCO3 . In some of these plants CO2 is added as well (typ- Research is being carried out at Norwegian University of
ically 615 mg/l) in order to minimize the iron dosage. pH, 7
Science and Technology (NTNU) both on ultra- and micro-
grain size as well as contact time influence the dissolution filtration. Two systems have been investigated for NOM re-
of the marble in order to arrive at the combination of pH, moval:
alkalinity and Ca-concentration aimed for (see above). In a
typical Norwegian situation, it is experienced that the empty 1. A system based on coagulation, flocculation and sub-
bed contact time in the marble part of the filter should be at merged, hollow fibre, outside-in UF filtration (Zenon
least 1525 min. A filter depth of the marble layer of 150 Zeeweed) (Machenbach and degaard, 2004).
250 mm at a filtration rate of 5 m/h is required (see Fig. 5).
After reaching a critical lower grain size, the smallest grains 2. A system based on coagulation, flocculation and inside-
are washed out during back-washing and new marble grains out ceramic microfiltration membranes (Metawater)
have to be supplied. New grains are supplied during back- (Meyn et al., 2007).
In both cases a water with a high color (50 mg Pt/L corre- 1.0
sponding to a TOC of 5.5 mg/l) has been investigated. It has
been shown that the optimized coagulation (pH and coagu-
lant dose) conditions for membrane filtration are pretty much 0.8
the same as for sand filtration. In the UF study (Machen- 1
C/C0 =
bach and degaard, 2004), that was carried out with operat- 0.6 1 + 20D/C0
ing fluxes in the range of 4575 L/m2 h, it was demonstrated
C/C0
that optimization of floc aggregation (flocculation) was im-
portant in order to minimize trans-membrane pressure (TMP) 0.4
build-up. A packed bed flocculator at low velocity gradients
(G-value 30 s1 ) and 5 min empty bed residence time gave 0.2
lower TMP-build-up than a high velocity gradient (G-value
'400 s1 ) and 30 s residence time pipe flocculator. In the MF
study, however, that was operated at fluxes in the range of 0.0
0.00 0.05 0.10 0.15 0.20 0.25 0.30
140220 L/m2 h, a pipe flocculator operated at varying con-
-1
ditions (G = 60 and 300 s1 and HRT 7.5 and 30 s) gave only Specific ozone dose (mgO3 mgPt )
Figure
moderately higher TMP build-up than the standard, tradi-
tional two-stage flocculation tank with 20 min HRT (Meyn Figure 7. Color reduction versus specific ozon dose.
et al., 2007). The difference in experience is probably caused
by the fact that conditions suitable for good flocculation exist
inside the ceramic membrane module itself. When using ozonation in humic surface water without any
The higher flux of the MF-unit was not sustainable and it pollutants, the direct oxidation reaction pathway is advanta-
seems that the recommended fluxes for UF-membranes after geous. This would imply that using an inert ozone column
coagulation of NOM is typically 5070 L/m2 h while it is the packing media is beneficial and that the pH should be neu-
range of 130160 L/m2 h in MF membranes. tral to low. At high alkalinity and NOM concentration the
efficiency of the system would be somewhat reduced,
In practice the ozone dose required for 80% colour re-
4 Oxidation/biofiltration moval that has typically been achieved in pilot- and full-scale
plants, is around 0.150.20 mg O3 /mgPt which translates to
4.1 Oxidation 1.01.5 mg O3 /mgTOC, see Fig. 7 (degaard et al., 2006).
In humic surface water where color removal and disinfection 4.2 Ozonation/biofiltration
is the main target, ozonation normally is the preferred oxi-
dation method. The oxidation of NOM by ozone can follow Ozonation is effective in colour removal from humic surface
two main pathways; 1) direct oxidation by ozon which selec- water see Fig. 7 in which the colour removal versus specific
tively targets mainly activated aromatics and double bonds, dose is shown for different waters (degaard er at, 2006).
and 2) indirect reaction where ozone is decomposed to form Ozonation of colored water, however, Figure6
also results in reac-
hydroxyl radicals which are more powerful but less selective tion products that are far more biodegradable than the orig-
oxidants than ozone. Consequently, the direct reaction path- inal
humic substances. Biofiltration is therefore required in
way results in high color removal, but little TOC removal, order to remove the easily biodegradable organic ozonation
whereas the indirect pathway removes less color and more by-products. The flow-scheme of various alternatives of an
TOC. The water matrix may determine the importance of the ozonation/biofiltration plant is shown in Fig. 8.
two pathways, and also the degree of scavenging. pH is of It is well known that activated carbon filters after ozona-
particular importance, and at high pH the indirect reaction tion of NOM-containing waters results in biological activity
pathway dominates and the ozonation may be considered as in the filter. The run-time of GAC filters is increased be-
an AOP (Advanced Oxidation Process, defined as using hy- cause of biological regeneration. In Norway we have also
droxyl radicals for oxidation). The use of an AOP may be experiences from plants with biofilters consisting of packed
advantageous if oxidation of ozone resistant compounds is bed plastic carrier (Kaldnes K1) followed by sand filters
desired (i.e. several micro-pollutants, atrazine, alachlor, etc.). for biomass separation, combined biofilters/separation filters
A disadvantage of the AOPs is that the hydroxyl radicals are with Filtralite or with three-media (anthracite/sand/calcium
very unstable, easily scavenged and have a very short life- carbonate) as filter medium (Melin et al., 2006). Besides
time. Ozonation may become an AOP when combined with the fact that granular activated carbon (GAC) filters give
H2 O2 or UV, or by using a catalytic packing media in the a quicker start-up caused by the adsorption effect, the rate
ozone column. Other AOPs may also be applied, such as of biodegradation does not seem to be strongly influenced
UV/H2 O2 , UV/TiO2 , Vacuum-UV, Fenton, etc. by the media selected, while the kinetic studies show that
CaCO 3 Biofilm
(optional) carrier
Alt. 2
GAC or Alt. 3
Filtralite Bio filter +
filter UF filter
for removal of several micro pollutants. The cost estimation downwards or upwards. The regeneration solution is typi-
has shown that the OBM process is competitive with conven- cally reused 78 times and in such a manner that about 1/8
tional treatment processes (Azrague et al., 2009). of the regeneration solution volume is substituted after each
regeneration.
Until now, the magnetic ion exchange process (MIEX) is
5 Sorption processes
not applied at Norwegian water treatment plants.
GAC adsorption as well as ion exchange may be used for
removing humic substances. 6 Conclusions
Edited by: B. Heijman Machenbach, I. and degaard, H.: Relevance of flocculation in in-
tegrated membrane processes for NOM removal, in: Chemical
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