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Wat. Res. Vol. 31, No. 5, pp. 991-996.

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Department of Chemical Engineering, University of Patras and Institute of Chemical Engineering and
High Temperature Chemical Processes, P.O. Box 1414, GR- 26500 Patras, Greece

(Received October 1994; accepted in revisedform October 1996)

Abstract--A trickling filter for iron removal from potable water has been constructed and tested. Iron
removal was found to be caused by both biological and physico-chemical iron oxidation. The extent of
each oxidation type was assessed. In addition, iron concentration profiles were taken along the filter depth,
for both biological and physico-chemical iron oxidation, under the same operating conditions. Significant
quantities of iron precipitated, mandating a periodic filter backwash. The possible duration of the filter
operating cycles was studied as a function of the inlet iron concentration and the volumetric flow-rate.
The limits of feed iron concentration and hydraulic loadings on the filter were determined and appropriate
operating diagrams were constructed. © 1997 Elsevier Science Ltd

Key words---biofilm, biological oxidation, iron removal, physico-chemical oxidation, potable water,
trickling filter

I!NTRODUCTION at a pH under 6 and reduced forms may persist for

some time in aerated waters (Sawyer and McCarty,
When iron is present in a water supply, at 1978). The rates may be increased by the presence
concentrations exceeding the secondary drinking of certain inorganic catalysts or through the action
water standards of 0.2mg/l (EEC, 1980), it is of micro-organisms. There are several genus of
undesirable for the following reasons (Kontari, 1988): bacteria that oxidize dissolved iron with different
(a) iron precipitates give water a reddish colour when mechanisms. Gallionella sp, Leptothrix ochracea and
exposed to air; (b) iron gives water a metallic taste; Crenothrix polyspora cause primary intracellular
(c) home softeners become clogged by iron precipi- oxidation by enzymatic action, while secondary
tates; (d) deposition of iron precipitates in the extracellular oxidation is caused by the catalytic
distribution system can reduce the effective pipe action of polymers excreted by the filaments
diameter and eventually clog the pipe; and (e) iron is comprising the stalks produced by Gallionella sp.,
a substrate for growth of bacteria in the water mains. the sheaths from Leptothrix sp., Crenothrix sp.,
When iron bacteria die and slough off, bad odours Clonothrix sp. and Sphaerotilus sp. Also, secondary
and unpleasant tastes may be caused. extracellular oxidation is caused by the catalytic
Surface water iron is generally found in its action of polymers, excreted by the microscopic
precipitated ferric form. It is found in its ferrous state filaments of capillary appearance that are aban-
in the deeper layers of some water reserves lacking doned by the gliding trichomes of Toxothrix
oxygen, or in groundwater, in which case it is in a trichogenes and extracellular polymers that are
reduced dissolved form (Fe 2+) and often chelated. excreted by various Siderocapsaceae (Mouchet,
The state of iron in water depends above all on the 1992).
pH and the redox potential. A dissolved form of iron Aeration followed by solid-liquid separation is the
(FC ÷ or FeOH +) can be changed to a precipitated most commonly used physico-chemical treatment
form (FeCO3, Fe (OH)2 or Fe (OH)3) by increasing method for iron removal. Aeration is generally
either the oxidation potential, the pH, or both (Hem, recommended for oxidizing ferrous iron for water
1961). with high iron concentrations ( > 5 mg/l) so that
The rates of ferrous iron oxidation by air increase costs for chemicals can be avoided (Wong, 1984).
with the pH and ;about 90% conversion may be Sedimentation and/or filtration (sand or dual-media
achieved in 10-20 rain at a pH of 7 (Sundstrom and filtration) are applied for the solid-liquid separation.
Klei, 1979). Iron oxidation is substantially slower If necessary, other treatments may be added, such as
pH correction (lime softening), chemical oxidation
*Author to whom all ~-orrespondence should be addressed. (with chlorine, potassium permanganate or ozone)

992 G. Dimitrakos Michalakos et al.

ion exchange processes, settling and biological during start-up through the use of an air pump. After 10 d,
microscopic observations (x 1200) revealed the presence of
oxidation. two types of microbes; cylindrically shaped (probably genus
As mentioned above, numerous bacteria are Leptothrix and Crenothrix Cohn), and bean shaped
capable of provoking the biological oxidation of iron (probably genus Gallionella Ehrenberg). The filter was then
inside or Outside their sheaths. The extent to which switched to continuous operation. During continuous
an observed iron removal may be attributed to operation, water was added with feed iron concentrations
ranging between 1 and 17 mg/l. This covers the range of
physico-chemical and/or biological iron oxidation possible concentrations encountered in drinking water
may vary depending on the particular treatment supplies. The feed solution resulted after mixing a
environment employed. In this communication, the concentrated iron solution (containing small amounts of
use of a pilot-scale trickling filter for iron removal ammonia and phosphorus) with water from the water
from drinking water is presented. The limits between supply network (containing nonmeasurable iron amounts)
at a mixing chamber located at the top of the filter. The
physico-chemical and biological iron removal are concentrated iron solution was always kept in a refrigerator
identified. Experimental profiles of total iron located close to the filter, in order to prevent bacterial
concentration are given in both cases (only physico- growth in the feed medium.
chemical and combined physico-chemical and bio- In order to study the extent of physico-chemical iron
oxidation, the filter was disinfected, with commercial bleach
logical) and the limits of the filter for iron of chlorine (NaOCI 5%), to exclude bacterial growth. The
concentration and hydraulic loadings were assessed filter was disinfected every 2 d by adding chlorine to the filter
and used to generate an operating diagram, useful for for half an hour and then passing network water through the
the design of appropriate trickling filters. filter, before starting to feed with the iron concentrated
solution. Under these conditions, only physico-chemical
iron oxidation was possible.
During all experiments, pH, temperature and total iron
MATERIALS AND METHODS concentration were measured on a daily basis. Iron
The pilot-scale trickling filter consisted of a 1.8 m high concentration measurements were done according to the
Plexiglas tube with an inside diameter of 9 cm. This Standard Methods for the Examination of Water and
pilot-filter height is typical of a full scale industrial filter Wastewater (APHA et al., 1989) using an atomic absorption
(Metcalf and Eddy, 1991). Since it is the loadings (hydraulic spectrophotometer (model SpectrAA-10 Plus, VARIAN).
and iron) per unit cross-sectional area that count, no
scale-up is necessary. The filter was externally covered in EXPERIMENTAL RESULTS
order to avoid algal growth on the walls. The support media
was gravel with a mean diameter of 0.5cm and a The experiments aimed at determining the limits of
~ 1330 m2/m3 specific surface area, while the depth of the hydraulic and iron concentration loadings, under
support media was 1.6 m and the filter porosity was 0.35
(Vayenas and Lyberatos, 1995, 1994). At the top of the filter, which the filter efficiency is satisfactory (total iron
there was a fixed nozzle which distributed the incoming concentration at the filter outlet less than 0.2 mg/l).
water evenly to the whole filter surface. An underdrain The experiments also aimed at determining the extent
system collected the treated water and any biological solids of biological vs physico-chemical iron oxidation
that would detach from the media. Along the filter depth since, as mentioned earlier, both take place under the
there were 15 sampling ports for iron concentration
measurements in the bulk liquid. Thus it was possible to operating conditions used.
have an experimental assessment of the total iron Once continuous operation was established, the
concentration profiles along the filter depth (Figs 3-5). volumetric flow rate (VFR) was progressively raised
Throughout all experiments the temperature was fairly to 1000 ml/min (corresponding to a retention time o f
constant at about 28°C, the pH ranged from 7.0 to 7.3 and
the concentration of the dissolved oxygen in the liquid phase 3 min). At this V F R , various feed iron concentrations
was about 8 mg/l (saturation concentration). The above were tested. Figure 1 presents the required duration
measurements were made using the U-10 Water Quality of operating cycles (time intervals in days, between
Checker (HORIBA). With these operating conditions and two successive backwashes of the filter) for total
since the redox potential ranged from 0.3 to 0.4V (as iron concentrations in the range of 1-17 mg/1. At
measured with a redox potential electrode), according to
Hem (1961), we could have both physico-chemical and 1 mg/l, no backwash was required. It seems that a
biological iron oxidation taking place. steady-state was reached. For higher iron concen-
The use of a trickling filter has the advantage of not trations the duration of operating cycles had to be
requiring an external air supply, since air is naturally decreased. At 17 mg/1, an operating cycle duration of
convected through the filter due to the temperature
difference between the interior and exterior of the filter. A 1 d was found sufficient, while the outlet iron
similar filter referred to as a contact filter (filter media was concentration was about 0.2 mg/l (limited operation).
crushed rocks to 30-70 mm) has been mentioned by Carlson Generally, as investigated, for higher concentrations
and Schwertmann (1987). In our filter however, complete and VFRs, an increase in the inlet iron concentration
aeration and very good filtration may be effected at the same or in the V F R , decreases the required duration of the
time, since the mean gravel diameter was only 5 ram.
Inoculum was taken from the wastewater treatment plant operating cycles. During an operating cycle, only
of the University of Patras and added to the filter, with a minimal suspended solids or iron precipitates could
concentrated iron solution (FeSO4-7H20) which also be observed at the filter outlet, while at the end o f
contained small quantities of ammonia (NH~CI) and each cycle an increase of the suspended solids and
phosphorus (KH2PO,), to ensure bacterial growth. A
start-up time of approximately 10 d was necessary for the precipitates was apparent. This was used as a
biological oxidation to begin. During this period, the filter criterion for starting filter backwash.
was operated as a batch reactor. The filter was aerated Once the feed iron concentration limit (17 mg/1) of
Trickling filter for iron removal from water 993




v 14-
0 12-


0 4 6 8 1'0 1'2 1'4 l's 1'8 20
Fig. 1. Required backwash frequency (cycle duration) as a function of inlet iron concentration.

the filter for a VFR of 1000 ml/min was determined, operating cycles were of the order of only hours and
we searched for the feed concentration limits for the filter outlet concentration was above 0.2 mg/1.
higher VFRs. Figure 2 presents the curve (upper Below this curve, the filter had excellent performance.
curve, which resulted after fitting the experimental We also found that the absolute upper VFR limit for
data) of iron oxidation. Above this curve the this filter was 3000 ml/min, since for higher VFRs the


-m-Biological and Physicochemical oxidation

1 El
-&- Physicochemical o x i d a t i o n

1 zl.

I-'- 1 0
0 8 -
0 El x x


1000 1500 2000 2500 3000

Fig. 2. Operating curves which showing the limits when: (a) simultaneous biological and physico-chemical
iron oxidation take place; and (b) only physico-chemicaloxidation takes place.
994 G. Dimitrakos Michalakos et al.

filter flooded, regardless of what the feed iron resulted in a better exploitation of the total filter
concentration was. height. The outlet iron concentrations for biological
In order to assess the filter performance with oxidation still remained within the allowable limits,
physico-chemical iron oxidation alone, the same whereas physico-chemical oxidation would be insuffi-
experiments were repeated after the filter was cient again. Also, comparison between Figs 3 and 4
disinfected. Iron oxidation was possible only shows that for the same inlet iron concentration the
physico-chemically, using the air which flowed biological activity is significant only for the lower
physically through the filter. The lower curve of VFR (Fig. 3).
Fig. 2 represents the physico-chemical iron oxidation
limiting curve, under which the filter had excellent
performance. It is obvious that the existence of
bacteria in the filter can dramatically improve the
filter efficiency under the same operating conditions. In this work the use of a trickling filter for iron
Figures 3-5 present total iron concentration removal from drinking water was examined and
profiles along the filter depth for both biological verified. The filter had excellent performance under
and physico-chemical oxidation. As seen in Fig. 3 various flow rates and inlet iron concentrations. The
(inlet iron concentration: 4.1 mg/l, VFR: 2000 ml/ use of the trickling filter for iron removal confirmed
min) the biological oxidation profile is, as expected, that natural air convection through the filter secures
below the physico-chemical one, all along the filter oxygen saturation conditions at the bulk liquid. Thus,
depth. We can also observe that the outlet iron there was no need for extra aeration. In addition,
concentration with physico-chemical oxidation alone since large quantities of iron precipitates were
is above the upper permitted limit of 0.2 mg/1 while, remaining in the filter, oxidation and filtration were
with biological oxidation allowed, the outlet iron probably taking place simultaneously within the same
concentration is less than 0.1 mg/l. treatment unit. The required frequency of filter
Figures 4 (inlet iron concentration: 4.0 mg/1, VFR: backwashing was found to depend on the inlet iron
2500ml/min) and 5 (inlet iron concentration: concentration and the volumetric flow rate. The
3.0 rag/l, VFR: 3000 ml/min) show that differences in higher the setting of these operating parameters were,
the concentration profiles for the two types of the more frequent was the required backwash.
oxidation are more pronounced at the lower part of Operating diagrams were constructed showing the
the filter, suggesting that bacterial oxidation naturally allowable limits in hydraulic loading and inlet iron
takes place in that part of the filter. Under these concentration so that the filter performs adequately.
operating conditions the flow rates were high and Such limiting curves were given also for the case

Biological and Physicoehemical oxidation

Physicochemical oxidation
z 3.5-
O 2
O l
O l
n- 1
m •

0 2'0 6'0 go 1 ,0 16c
Fig. 3. Iron concentration profiles along the filter depth for: (a) simultaneous biological and
physico-chemical iron oxidation (inlet iron concentration: 4.1 mg/l, VFR: 2000ml/min); and (b) only
physico-chemical oxidation.
Trickling filter for iron removal from water 995

Biological and Physiooehemical oxidation

Physi¢ochemical oxidation

z 3. -
< 3-
Z 2.5-
CO 2-
0 !1
co 1.5-
n" 1

o 2o 4'0 6'0 8'o 160 1;~0 lz;O 160
Fig. 4. Iron concentration profiles along the filter depth for: (a) simultaneous biological and
physico-chemical iron oxidation (inlet iron concentration: 4.0 •g/l, VFR: 2500 ml/min); and (b) only
physico-chemical oxidation.

of physico-chemical oxidation alone. For the The advantages of biological iron removal of the
same VFRs, biological oxidation allows treatment presented trickling filter, are numerous: (a) rapid
of almost double the iron concentration than oxidation and no need for an external air supply;
physico-chemical oxidation alone. (b) iron oxidation and filtration taking place in the

Biological and Physicochemical oxidation
Physicochemical oxidation


Z 2-
Orr IB

0.5 L

0 2'0 4'0 60 ab 160 1~0 1~,0 160
Fig. 5. Iron concentration profiles along the filter depth for: (a) simultaneous biological and
physico-chemical iron oxidation (inlet iron concentration: 3.0 mg/I, VFR: 3000 mi/min); and (b) only
physico.chemical oxidation.
996 G. Dimitrakos Michalakos et al.

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