FLUORIDE REMOVAL FROM DRINKING WATER BY

ELECTROCOAGULATION PROCESS
Bhaskar Sharma
M.tech (15MT000371)
Under the guidance
of
Prof. I.M. Mishra & Dr. D. K. Sandilya

Department of Chemical Engineering

Indian Institute Of Technology (ISM), Dhanbad
Jharkhand - 826004
 CONTENT
 Introduction

 Objective

 Electrocoagulation Technique

 Electrocoagulation : Experimental

 Electrocoagulation: Results and Discussion

 Conclusions

 References
1. INTRODUCTION
Fluoride is widely distributed in nature and is present in rock minerals, soil, water,
plants, foods and even in the atmosphere.

It enters into human body through a variety of sources like water, food, air, medicine
and cosmetics. Among these, drinking water is the most common source which
makes fluoride available to human beings.

Fluoride within the permissible limit of 0.5 ~ 1.5 mg/L (WHO limit) is necessary for
bone formation and the prevention of tooth decay.

Whereas excessive intake of fluoride has harmful effects on human health, causing
dental fluorosis, muscular-skeletal fluorosis, osteoporosis, arthritis, and brittle bones.
 F- Concentration (mg/L) Health Outcome
<0.5 Dental caries
0.5–1.5 Optimum dental health
1.5–4.0 Dental fluorosis
4.0–10 Dental and skeletal fluorosis
>10.0 Crippling fluorosis

Effect of prolonged use of drinking water on human health, related to fluoride content
(Dissanayake, 1991).
• In India ,nearly 117 million people including 6 million children in the country in
200 districts in 15 states are affected with dental, skeletal fluorosis.

• Higher concentration (>50 mg/l) of fluoride in ground water are common in some
of the areas of the Rajasthan, Southern Punjab, Gujrat, Karnataka, Tamilanadu,
M.P and Southern Haryana.

• The extent of fluoride concentration in ground water varies from 1.0 to 50 mg/L.
Fig 1.1: Top 10 Indian States affected with fluorosis
• The desirable or permissible limits set by various authorities are given below:

Name of Authority Desiable limit, (mg/L)

1. BIS (Bureu of Indian Standard) 0.6-1.2

2. ICMR (Indian Council of Medical Research) 1.0

3. WHO (World Health Organisation) 1.5

2. Objective
The objectives of this work can broadly be categorized as,

• To develop a process involving electrocoagulation followed by filtration and apply this

in the treatment of drinking water with the aim of separating fluoride.

• To study the effect of various process parameters(initial fluoride concentration, current

density, interelectrode distance etc.) in electrocoagulation using aqueous synthetic
solution of fluoride.
3. ElectrocoagulAtion Technique
 3.1 Electrocoagulation
• Electrocoagulation uses an electrochemical cell to treat polluted water.
Sacrificial anodes corrode to release active coagulant cations, usually
aluminium or iron, to solution.
• Accompanying electrochemical reactions are dependent on species present
and usually evolve electrolytic gases.
• The coagulant’s delivery and its nature influence the coagulation and
separation processes. Electrocoagulation is a technique for applying direct
current to sacrificial electrodes that are underwater in an aqueous solution.
• Electro-coagulation is a direct and efficient technique to remove the
flocculating agent produced by electro-oxidation of a sacrificial anode and
generally made of iron or aluminum.
• The treatment is performed without including any chemical coagulant or
flocculants, which diminishes the amount of sludge which must be disposed.
 3.2 Electrochemistry
• Equation shows the dissolution of aluminium in the anode.
Al3+ + 3e− ↔ Al
• Oxygen evolution is also possible at the anode
4 OH- ⎯⎯→ O2 + 2H2O +4e-
• Simultaneously, an associated cathodic reaction, usually the evolution of hydrogen,
occurs. The reaction occurring at the cathode is dependent on pH.
• At neutral or alkaline pH, hydrogen is produced via Equation:
2H2O + 2e- ⎯⎯→ 2OH- + H2
while under acidic conditions, following equation best describes the hydrogen
evolution at the cathode :
2H+ + 2e- ⎯⎯→ H2
 3.3 Electrocoagulation and chemical coagulation

• Coagulation is a key feature of all electrocoagulation reactors, describing the

interaction between the coagulant and any pollutant material.
• The coagulant’s role here is to destabilise the colloidal suspension by reducing any
attractive forces, thereby lowering the energy barrier and enabling particles to
aggregate.
• . Chemical dosing delivers the coagulant as a salt that dissociates in solution with
hydrolysis of the aluminium cation (and associated anions) determining solution
speciation and pH.
• Alum (i.e. aluminium sulphate) addition, for example, acidifies the water. By
contrast, aluminium added via electrocoagulation does not bring with it any
associated salt anions, with the result that the pH typically stabilises in the alkaline
range.
 3.4 Coagulation mechanism for the removal of fluoride

• The electrode reactions are summarized as follows:

At Anode:
Al ⇒ Al3+ +3e-

At Cathode:
3H2O + 3e- ⇒ 3/2 H2↑ + 3OH-
• Al (III) and OH- ions generated by electrode reactions react to form various
monomeric species such as Al (OH)+2, Al(OH)+2, Al2(OH)24+ , Al(OH)4 - and
polymeric species such asAl6(OH)153+, Al7(OH)174+, Al8(OH)204+, Al13O4(OH)7+24,
Al13(OH)345+, which transform finally into Al (OH)3(S) according to complex
precipitation kinetics.
Al3+ + 3H2O ⇒Al(OH)3 + 3H+

• This Al(OH)3 complex is believed to have strong fluoride adsorption capacity as

Al(OH)3 + xF- ⇔ Al(OH)3-X Fx + xOH-
3.5 Floatation

• The production of electrolytic gases is an inevitable by-product of

electrocoagulation. These gases lift pollutant particles and coagulant
aggregates to the surface by a flotation like process, while
encouraging contact between pollutant particles and coagulant by
providing a certain amount of mixing action.

• Electrochemistry, coagulation and flotation thus form the three

foundation stones for electrocoagulation.
4. Electrocoagulation: Experimental
 4.1 Electrocoagulation bath & electrode
• Perspex made tank of working volume around 1.2 L and dimensions of
0.12 m × 0.10 m × 0.10 m was considered for the electrocoagulation
bath.
• Aluminium was reported to be very effective and successful in fluoride
removal at favorable operating conditions. Hence, aluminum sheets of
0.104 m × 0.084 m × 0.002 m were used as electrodes and the effective
surface area of each electrode was 80 × 10−4 m2.
• Dc power supply (Scientech 4180) of 0-30 V and 0-5 A and magnetic
stirrer at 300 rpm were used for experimental purpose.
• Two types of electrode connection (monopolar and bipolar) were
investigated during the EC of fluoride present in drinking water.
 Parameters Experimental
Conditions
Initial concentration (mg L-1) 4, 6, 8, 10
Interelectrode distance (m) 0.005, 0.01, 0.015
Current density (A/m2) 250, 375, 500, 625
Experiment time (min) 45
Temperature (° C) 35
Electrode connection Monopolar and bipolar

Fig 2.1 Photograph of electrocoagulation Setup Table 4.2.1 Experimental conditions

• Mono-polar electrode connection
In monopolar electrode connection, one end of the electrode was
connected to the positive terminal of the power source whereas the other
end of the electrode was connected to the negative terminal of the same
power source, thus completed the formation of a primary cell which
under the application of potential in contact with the contaminant
solution initiated the electrocoagulation process.

• Bipolar electrode connection

In bipolar connection, more than two electrodes were used to make such
arrangement in order to reduce the effective corrosion of the electrode
and improve the process performance.
Fig. 2.2 Schematic diagram of electrochemical cell for the EC experiments. (a)
Monopolar connection; and (b) bipolar connection. (1) Al electrodes; (2) fluoride
contaminated drinking water; (3) electrode support; and (4) DC power source.
 4.2 Solution preparation
• Sodium fluoride (NaF, supplied by Sd Fine-Chem Limited, Mumbai,
Mol. wt.: 41.99, Product no. 40139) was used in this work for the
preparation of fluoride solution.
• Measured quantity of salts of Na (i.e.2.21mg ) was added in tap water
(1 L).pH of tap water 7.5. Initial fluoride concentration varied from 4 to
10 mg L-1.
• 4ppm,6ppm, 8 ppm and 10 ppm fluoride solutions are prepared.
• The measurement of fluoride in the samples, taken at different time
interval (0-45 min) during the EC run are done by ion selective
electrode (Multi- 9420).
5. RESULT AND DISCUSSION
 5.1 Effect of initial fluoride concentration
Time F F F
(min.) concn. concn. concn.
9
(ppm) (ppm) (ppm) 8

Fluoride Conc(ppm)
7
6
0 4 6 8
5
5 2.754 4.597 6.213 4
10 2.665 3.871 4.824 3
15 2.383 3.218 4.009 2
20 1.836 2.854 3.217 1
0
25 1.409 2.492 3.000 0 10 20 30 40 50
30 1.321 2.274 2.831 Time(min)
35 1.000 2.056 2.374
4ppm 6ppm 8ppm
40 0.973 1.766 2.181
45 0.884 1.330 1.772
Fig. 5.1: Variation of fluoride concentration in the EC bath with
Table 5.1 Experimental reading for effect of initial F Conc. time. Interelectrode distance: 0.005 m; current density: 250 A m-
2; temperature: 35 °C, Electrode connection: Monopolar.
 5.2 Effect of bipolar connection of electrode
F F Current density=250 Am-2
conc.(mg/L) conc.(mg/L) 12
Time(min) (Monopolar) (Bipolar)

Fluoride Conc.(ppm)
10
0 10 10
8
5 7.383 6.989
6
10 6.485 5.752
15 6.206 4.797 4

20 5.786 4.208 2
25 5.225 3.704 0
30 4.58 3.003 0 10 20 30 40 50
35 3.823 2.611 Time (min)

40 3.008 1.994 Monopolar Bipolar

45 2.194 1.744 Fig. 5.2: Variation of fluoride concentration in the EC bath with
Table 5.2 Experimental readings for bipolar electrode time. Interelectrode distance: 0.005 m; current density: 250 A m-
2; temperature: 35 °C, Initial fluoride concentration: 10 mg L-1
connection Electrode connection: bipolar and monopolar.
 5.3 Effect of interelectrode distance
F FConc.(mg
FConc.(m/L Conc.(mg/ /L) current density: 625 A/m2
) L) (interelectr Interelectrode distance (m)
(inter (inter ode 12

Fluoride Conc(ppm)
Time(min) electrode electrode dist=0.015) 10
dist=0.005) dist=0.010)
8

6
0 10 10 10 4
5 6.397 7.259 7.644
10 5.705 6.627 7.054 2
15 5.212 6.162 6.432 0
20 4.652 5.697 5.974 0 10 20 30 40 50
25 3.926 5.165 5.451 Time(min)
30 2.936 4.467 4.861
0.005 0.015 0.01
35 1.779 3.534 4.041
40 1.021 2.802 3.682 Fig. 5.3: Effects of inter electrode distance on the fluoride
45 0.758 2.036 3.158 concentration in the EC bath with time. Initial fluoride
Table 5.3 Experimental readings for effect of inter concentration 10 mg L-1, current density: 625 A m-2, inter
electrode distance: 0.005 m, temperature 35 °C, electrode
electrode distance connection: monopolar
 5.4 Fluoride removal with varying current density
F F F F
Conc.(p Conc.(p Conc.(p Conc.(p Current density (A/m2)
pm) pm) pm) pm)
12
Time(mi (250 (375 (500 (625

Fluoride Conc(ppm)
10
n) A/m2 ) A/m2 ) A/m2 ) A/m2 )
8
0 10 10 10 10
5 7.421 7.125 6.895 6.403 6

10 6.534 6.337 6.042 5.681 4

15 6.239 5.91 5.484 5.188 2
20 5.845 5.352 4.794 4.629 0
25 5.221 4.925 4.367 3.907 0 10 20 30 40 50
Time (min)
30 4.629 4.039 3.218 2.889 250 375 500 625
35 3.842 3.284 2.627 1.773
40 3.054 2.725 1.707 0.985
Fig 5.4(a): Effects of current density on the fluoride
45 2.2 1.937 1.051 0.788
concentration in the EC bath with time. Initial fluoride
Table 5.4(a) Experimental readings for varying current density concentration 10 mg L-1, inter electrode distance: 0.005 m,
(monopolar connection) temperature: 35°C, electrode connection: monopolar
 F F Electrode connection: Bipolar
Conc(mg/ F Conc(mg/ Current density (A m-2)
L) Conc(mg/ L)
12
(375 A/m2 L) (625 A/m2
Time(min) ) (500A/m2 ) ) 10

Fluoride Conc(ppm)
0 10 10 10
8
5 6.801 6.224 5.755
10 6.032 5.276 4.122 6
15 4.617 4.039 3.391
4
20 3.992 3.705 2.479
25 3.478 2.937 1.604 2
30 2.782 2.062 0.981
0
35 2.159 1.654 0.861 0 10 20 30 40 50
40 1.571 1.139 0.743 Time(min)
45 1.308 0.984 0.588 375 500 625
Fig. 5.4.(b): Effect of current density on the fluoride
Table 5.4(b) Experimental readings for varying current
concentration in the EC bath with time. Initial fluoride
density (bipolar connection)
concentration: 10 mg L-1; interelectrode distance: 0.005 m;
electrode connection: bipolar; temperature: 35 °C.
 5.5 Variation of pH in electrocoagulation bath
pH pH pH
Time(min) (625 Am-2) (500 Am-2) (375 Am-2) Current densities (Am-2)
8
0 5.607 5.607 5.607 7

pH in EC Bath
5 6.154 5.917 5.705 6
5
10 6.235 6.007 5.795 4
15 6.399 6.293 5.925 3
2
20 6.521 6.391 5.991
1
25 6.668 6.431 6.129 0
0 10 20 30 40 50
30 6.725 6.554 6.211
35 6.839 6.611 6.358 Time(min)
625 500 375
40 6.945 6.652 6.401
45 6.994 6.717 6.481 Fig. 5.5.1: Variation of pH of fluoride containing drinking water
in the EC bath with time at different current densities. Inter
electrode distance: 0.005 m, initial fluoride concentration: 10
Table 5.5.1 Experimental readings for effect of variation of
mg L-1, electrode connection: monopolar
pH in EC bath
5.6 Variation of conductivity of treated water

• In order to examine the treated water quality by electrocoagulation, conductivity

measurement was made so that it could be permissible for the drinking purpose.

• Before each experiment using bipolar electrode connection, the conductivity of the
contaminated water was measured as 0.4, 0.6 and 0.9 mmhos for the initial fluoride
concentration of 6, 8 and 10 mg L-1, respectively.

• After the treatment, the sludge was filtered out and the clear solution was collected.
The conductivity of treated water was around 0.2 mmhos for all cases, that is, in the
range of permissible limit of drinking water.
6. Conclusion
1. Electrocoagulation (EC) technique was investigated in batch mode for
the removal of fluoride from drinking water using monopolar and bipolar
electrode connections.
2. Variation of different operating parameters such as, current density,
inter electrode distance, time of EC and initial concentration of fluoride
were investigated in detail.
3. Inter-electrode distance of 0.005 m and current density of 625 Am-2
were found to be most effective variables for the removal of fluoride
contaminants.
4. The results showed that the performance of EC in terms of percentage
removal of fluoride were increased with the increase in current density but
decreased with inter electrode distance.
5. The results also confirmed that the bipolar connection can serve better
removal than the monopolar connection.

6. Electrocoagulation was able to remove 92.12% & 94.12% fluoride

from the mixture composed of 10mgL-1 of fluoride respectively from
drinking water using monopolar & bipolar electrode connection in 45
minutes at current density 625 Am-2 and inter electrode distance of 0.005
m.
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Thank You