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Buddharatna.J.Godboley* et al. / (IJAEST) INTERNATIONAL JOURNAL OF ADVANCED ENGINEERING SCIENCES AND TECHNOLOGIES Vol No. 7, Issue No. 1, 054 - 064

Removal of As (III) From Groundwater by Iron Impregnated Potato Peels (IIPP): Batch Study Buddharatna.J.Godboley M.Tech. student, IV sem. Environmental Engg. G.H.Raisoni College of Engg. Nagpur India. E mail:- godboley619@gmail.com

R.M. Dhoble Associate Prof. Civil Engg. G. H. Raisoni College of Engg. Nagpur India E mail:- rmdhoble@ rediffmil.com

Abstract:

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The presence of arsenic in ground water is major problem as it causes adverse effects on human body if the concentration is more than 10Âľg/L and drink arsenic contaminated water for longer period. In present study the efforts have been taken to remove As (III) from drinking water using Iron Impregnated Potato Peels (IIPP). From the experimental data of batch study it was found that at 1.0 mg/L concentration of As (III) the Langmuir adsorption capacity in batch study was found 0.1039 mg/g at the adsorbent dose (IIPP) of 20 g/L at pH 7.0. The adsorption process is exothermic in nature. The IIPP was also used in field water with the same conditions of simulated water and found that all the physicochemical parameters of drinking water were in the permissible limits. No leaching of iron was found in the water after treatment. Kinetic study was also carried out and found that the values

of correlation coefficient (R2) for the pseudo-second-order kinetic model fitted well as compared to pseudo first-order model. The cost of IIPP was found Rs. 69 /Kg. Key word:: Arsenic (III) removal, adsorption, iron impregnated potato peel -------------------------------------------------------------------------------------------------------------------------

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1.0 Introduction Arsenic (As) is considered a contaminant of major concern due to its high toxicity at small concentrations and its ability to go undetected (L.M.Camacho et al., 2011). It is naturally present in the environment due to geological formations, such as lacustre sediments and volcanic rocks. The highest arsenic concentrations (20-200 mg/kg) are typically found in organic-rich and sulphide-rich shale’s, sedimentary ironstones, phosphatic rocks, and some coals (D, Chakraborti et al., 2002). The common valencies of geogenic arsenic in ground water sources are As(III) (arsenite) and As(V)(arsenate).The inorganic hydrolysed species are present as H3AsO3, H2AsO3--, HAsO32-, AsO33-- and H3AsO4, H2AsO4-- HAsO42-- andAsO43- (A.Gupta, et al., 1997). Under reducing conditions, Arsenite As( (III)) is the dominant form; arsenate (As (V)) is generally the stable form in oxygenated environments. Arsenic and its compounds

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occur in crystalline, powder, amorphous or vitreous forms. They usually occur in trace quantities in all rock, soil, water and air. However, concentrations may be higher in certain areas as a result of weathering and anthropogenic activities including metal mining and smelting, fossil fuel combustion and pesticide use. Arsenic is a geogenic water menace affecting millions of people all over the world and is regarded as the largest mass poisoning in history. Permanent arsenic intake leads to chronic intoxication, and prolonged arsenic exposure can damage the central nervous system, liver, skin and results in the appearance of diverse types of cancer, such as hyperkeratosis, lung and skin cancer (D. Mohan, et al., 2007). In India after West-Bengal and the bordering districts of Bangladesh, arsenic in groundwater was detected in part of Assam, Arunachal Pradesh, Manipur, Nagaland and Tripura, Jharkhand, Bihar

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Buddharatna.J.Godboley* et al. / (IJAEST) INTERNATIONAL JOURNAL OF ADVANCED ENGINEERING SCIENCES AND TECHNOLOGIES Vol No. 7, Issue No. 1, 054 - 064

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In West Bengal most frequent arsenic concentration value range from 0.3 to 0.7 mg/L with occasionally higher value of 1.86 and 5.0 mg/L reported from two places in the district of Murshidabad (A.Gupta et al., 1997). High concentration of arsenic (10 - 3200 µg/L) in groundwater of West Bengal has been encountered in Nadia, Murshidabad, Malda, Barddhaman, Hooghly, North & South 24- Paragnas districts of West Bengal. According to a survey conducted by WHO in 2006, the number of people poisoned by arsenic in India and Bangladesh alone were 70 million (C.Niu et al., 2007). WHO provisional guideline value for arsenic in drinking water is 10 µg/l (WHO, 2004). Permissible limit of arsenic in drinking water is less than 10µg/L (WHO. 1993).

2.2 Methods The synthesized material was subjected to detailed characterization by using different techniques like X-ray diffraction, scanning electron microscopy (SEM) and Wave length energy dispersive analysis of X-ray (WDAX). XRD patterns have been recorded at Vishwesharaya National institute of Technology (VNIT), Nagpur using X- Ray diffractometer, (Model Phillips: PW-1830). The SEM analysis of the synthesized adsorbents was carried out at VNIT, Nagpur using Scanning Electron Microscopy (Jeol, JXA-840 A, Electron probe micro-analyzer, Japan) with different magnification. Chemical composition of the adsorption materials was carried on Wave length Dispersive X-Ray Fluorescence Spectrophotometer (WDXRFS) equipment from Indian Bureau of Mines at Nagpur (PW 2403 magix, Philips Netherlands).

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Chhattisgarh, and Utter Pradesh. Elevated arsenic concentration has been found in Taiwan, Argentina, Mexico, Chile, Chin, Thailand, USA, South Africa, New Zealand Bangladesh and India (R.M. Dhoble et al., 2010; S. Bang et al., 2005). Arsenic concentration in rural area averaged between 0.6 and 0.9 mg/L and in between 3.2 and 5.6 mg/L for the rivers influenced by industrial discharges (C. Neal et al., 2000).

3.0 Characterisation of Material. 3.1 X-ray Powder Diffraction (XRD) In this test samples were scanned for 2ø range from 5 to 60°.The X-ray diffraction spectrum pattern of the IIPP did not show any significant change in sharp peak ((Fig.1 Fig.1 thereby indicating the amorphous (Fig.1), nature of the product.

2.0 Materials and Methods 2.1 Materials

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All the chemicals used in the present study were analytical grade. Standards for calibration were prepared from As (III) standard reference sodium (Meta) arsenite. Stock solution (1000mg/L) was prepared from sodium (Meta) arsenite (Merck India) A.R.grade and frozen to prevent oxidation. Solutions of As (III) of 100 mg/L were prepared in every fortnight and working solutions of As (III) were prepared according to experiment requirements. pH was adjusted by standard acid and base solutions of 0.1 N HCl and 0.1 N NaOH respectively.

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Fig 1: - Characterisation of IIPP by XRD 3.2 Scanning Electrons Microscopes (SEM) Scanning electrons microscopes analysis was performed to understand the morphology of IIPP.From Fig.2. it is observed that the pore size of adsorbent is bigger before adsorption and then filled by the arsenic ions after adsorption.

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b) Af Aft After ter adsorption

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a) Before adsorption

Fig 2:: Characterisation of IIPP by SEM

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3.3 Chemical composition of IIPP was carried out on WDAX. Table 1 shows the composition of material (IIPP) Table 1: Chemical composition of IIPP Element

Fe

Percentage

61.7

Mg

Al

P

Ca

2.28

0.77

0.73

0.55

0.27

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4.0 Batch study

Si

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In the adsorption study a temperature controlled orbital shaker (Remi Instruments, Mumbai), was used for the batch adsorption study. The temperature range for the studies was from 293 to 313K. All the batch studies were performed at the shaking rate of 150 revolutions per minute (rpm). For each experimental run, 50 ml aqueous solution of the known concentration of arsenic (III) was taken in 100 ml capacity plastic bottles containing 50 ml of arsenic (III) solution and known mass of the adsorbent. These bottles were agitated at a constant shaking rate of 150 rpm in a temperature controlled orbital shaker maintained at a constant temperature. The pH of the adsorbate solution was adjusted using 0.1 N HCl or 0.1 N NaOH aqueous solutions without any further adjustment during the

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sorption process. To check whether the equilibrium has been attained, the samples were withdrawn from the flasks at different time intervals. Remaining Arsenic (III) was measured by Atomic absorption spectrometer (Hydride Vapors Generator, HVGAAS). The comparison was made between synthesis and field water. 5.0 Adsorption model 5.1 Langmuir Isotherm Langmuir isotherm is based on the assumption that points of valency exist on the surface of the adsorbent and that each of these sites is capable of adsorbing one molecule; thus, the adsorbed layer will be one molecule thick. Furthermore, it is assumed that all the adsorption sites have equal affinities for molecules of the adsorbate and that the presence of

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adsorbed molecules at one site will not affect the adsorption of molecules at an adjacent site. The Langmuir equation is commonly written as follows (I. Langmuir.1916).

Where, K F and n are the constants. Ce = the concentration of adsorbate solution at equilibrium by taking logarithm on both sides, this equation is converted into a linear form: (S.Kandu et al., 2006)

qe=

log qe= log kf +1/n log Ce

Where qe is the amount adsorbed (mg/g); Ce is the equilibrium concentration of adsorbate (mg/l); qmax indicates the monolayer adsorption capacity of adsorbent (mg/g) and the Langmuir constant b (L/mg) is related to the energy of adsorption. The linear form of the Langmuir isotherm can be expressed as equation 2.

When

(

---- (2)

is plotted against , a straight

with slope

is obtained which shows

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the adsorption dsorption follow the Langmuir isotherm. The Langmuir constants b and qmax are calculated from the slope and intercept with Y- axis. The essential characteristics of a Langmuir isotherm can be expressed in terms of a dimensionless separation factor, r (T.Weber et al., 1974) which describes the type of isotherm and is defined by r=

---- (3)

Where b and Co are the terms appearing in the Langmuir isotherm. The parameter indicates the shape of the isotherm accordingly. 5.2 Freundlich Isotherm The equation that describes such isotherm is the Freundlich Isotherm, given as 1

Qe = K FCen

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Thus a plot between ln q e and ln Ce is a straight line. The Freundlich equation is most useful for dilute solutions over small concentration ranges. The values of the constants ‘n’and ‘kf’ can be determined from the plot. Larger Kf indicates larger the adsorption capacity. The intercept is roughly an indicator of sorption capacity and the slope, 1/n, of adsorption capacity. The parameter 1/n measures the strength of adsorption. A high KF and high ‘ n’ value is an indication of high adsorption throughout the concentration range. A low KF and high ‘n’ indicates a low adsorption throughout the concentration range. A low ‘n’ value indicates high adsorption at strong solute concentration.

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=

---- (5)

T

---- (1)

--- (4)

if 1/n < 1, bond energies increases with surface density 1/n > 1, bond energies decreases with surface density 1/n = 1, all surface sites are equivalent 6.0 Kinetic study In order to estimate equilibrium adsorption rate for the uptake of As (III) by impregnated potato peels (IIPP), time dependent sorption studies were conducted. Adsorption kinetics was monitored by adding known weight of IIPP into 50 ml of at 1mg/L arsenic solution at 293 K, 303K and 313K stirred at 150 rpm. A portion of solution was withdrawn from the vessel at predetermined time intervals was filtered and analyzed for residual concentration of As (III) using Atomic absorption spectrophotometer hydride vapour generator.

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where qe and qt (mg/g) are the amounts of As adsorbed at equilibrium (mg/g) and t (min), respectively, while K1 is the rate constant of the equation (min−1). The Lagergren second-order rate model is given by the following expression [ Baig etal., 2010]: =

----- (7)

Fig.3 : Effect of dose of adsorbent for As (III) removal on adsorption by IIPP Condition: Co- 1mg/L, pH -7.0, Temp. 303K. rpm – 150.

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whereK2 (g/mol/min) is the rate constant of the second-order equation, qt (mol/g) is the amount of adsorption at time t (min) and qe is the amount of adsorption equilibrium (mol/g). In order to be able to estimate maximum capacities of adsorbents, it is necessary to know the quantity of adsorbed metal as a function of metal concentration in solution.

finalized and used for further study. This is also noted that as the dose of adsorbent increased the adsorption capacity also increased. This may be due to the more number of active sites available.

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For adsorption, simplified approach given by Lagergren can often be applied with success especially in the first phase of the sorption. The Lagergren first-order rate model is given by the following expression. (J. Baig et al., 2010) Log (qe-qt) = log qe – t ----- (6)

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7.0 Results and discussion 7.1 Optimum dose of adsorbent The optimum dose experiments were carried by adding different amount of adsorbent doses 1.0, 2.0, 3.0, 5.0, 10.0, 20.0 and 25 g/L into the 1.0 mg/l known amount of As (III) concentration. This was put inside the 100 ml capacity glass bottles containing 50 ml of Arsenic (III) solution. The bottles with arsenic mixture were then being put into the incubator shaker which operated at 150 rpm and with constant temperature 303K up to 24 hrs.From Fig. 3 shows that as the dose of adsorbent increased the adsorption of as (III) also increased upto from 1 to 20 g/L and found at the dose of 20 g/L the remaining As (III) was less than 10 µg/L ( less than permissible limit WHO 2007).After this removal was not significantly reduced. Hence the IIPP dose of 20g/L was

7.2 Effect of pH The sorption of As (III) by the adsorbent was studied over a pH of 2-12 at 303K and over a contact time of 24 h. concentration of 1.0 mg/L As (III) was used. From the Fig. 4 it is observed that the adsorption of As (III) was less in acidic zone and increased as the pH increased upto 7.0 pH and then decreased. For the drinking purpose the pH should be in the range of 6.5-8.5 (BIS 10500-1991) and in the present study it was found that pH is in permissible limit

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Fig.4: Effect of pH for As (III) removal on adsorption by IIPP. (Condition: Co- 1mg/L, Dose of adsorbent: 20 g/L., Temp. 303K. rpm – 150.)

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Fig.6 E Effect ffect of time of contact of As (III) removal on adsorption by IIPP. (Condition: Dose of adsorbent – 20 g/L, pH -7.0, Temp. 303K. rpm – 150.)

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The study of different initial concentrations containing optimum dose 20.0gm/l of adsorbent (IIPP ) was carried into the known amount of different As (III) concentration in the range of 0.5 – 4.0 mg/L put in bottles containing 50 ml of arsenic (III) solution. The bottles were then put into the incubator shaker which operated at 150 rpm and with constant temperature 303K up to 24hrs. (i.e. time of contact). It is evident from the Fig. 5 that adsorption of As (III) decreased with the increased in As (III) concentration. This may be due to the insufficient number of active sites than the number of As (III) ions present in solution.

concentration in water after treatment was less than permissible limit (10µg/L). This may be due to the saturation of adsorbent capacity of IIPP. Hence 24 hrs was selected the time of contact at 303K.

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7.3 Effect of Initial concentration

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Fig.5: Effect ffect of initial concentrationof As(III) removal on adsorption by IIPP. (Condition: Dose of adsorbent – 20 g/L, pH -7.0, Temp. 303K. rpm – 150.)

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7.4 Effect of Time of Contact

The time of equilibrium study experiments were carried by adding fixed amount of adsorbent (20g/L).The arsenic (III) standard solution of 50 ml was put in the 100 ml capacity plastic bottles at optimum pH7.0.The bottles with Arsenic (III) mixture were then being put into the incubator shaker which operated at 150 rpm and with constant temperature 303K.The bottles were take out from the incubator shaker after 15, 30, 60, 120, 240, 360, 480, 600, 720, and 1440 min intervals. From Fig. 6 it is found that as the time of contact increased the adsorption of as (III) also increased. After 22 hrs. The adsorption was almost constant and found the As (III)

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8.0 Adsorption model In this Langmuir and Freundlich model were used for best fitting. From Fig. 7 & 8 it is observed that the experimental data is fitted in Langmuir model and in Freundlich model. From Table 2 it is observed that the adsorption capacity increased as the temperature increased this indicated that the process is exothermic. The maximum adsorption capacity on Langmuir adsorption model at temperature was found 0.1039 mg/g at 303K and from Table 3 Freundlich maximum adsorption capacities it was found 0.3859 mg/g. This indicates the Freundlich model was best fitted then Langmuir model. (Ref.Table 2 & 3).

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Fig.8: Freundlich model fit for adsorption of As (III) at 303K (Condition: Co- 1mg/L, Dose of adsorbent -20g/L., pH -7.0, rpm – 150.)

9.0 Kinetic adsorption model It is apparent from the values of correlation coefficients that the pseudosecond-order kinetic model fitted well as compared to pseudo first-order model (Ref. Fig.9 &10).Table 4 shows the various kinetic and diffusion parameters for As (III) adsorption by IIPP.

10.0 Com Comparison Co mparison parison of simulated and field water The adsorption experiments were carried on simulated and field tap water containing arsenic (III) of 1mg/L, at optimum pH-7.0, by adding optimum dose of adsorbent (20 g/L) which was put inside the bottles in 50 ml. which operated at 150 rpm and with constant temperature 30ºC ± 1 up to 24hrs. (time of equilibrium). The samples were taken out and analysed for As (III) remaining. From Fig. 11 the removal of As (III) was more in simulated water than the As (III) spiked in field tap water. This may be due to the presence of cations and anions present in field tap water. Table 5 shows that the effect on adsorption before and after treatment. All the parameters after treatment was within permissible limit (BIS 10500-1991). It is also observed that the iron leaching was not observed as the iron content before treatment was 0.1637 and after adsorption was 0.1174. Similarly chloride content was not increased after treatment and found within permissible limit.

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Fig.7: Langmuir model fit for adsorption of As (III) at 293K, 303K and 313K. (Condition: Co- 1mg/L, Dose of adsorbent -20g/L., pH -7.0, rpm – 150.)

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Fig.9: Pseudo-first kinetic model for arsenic removal by IIPP

Fig10: Pseudo-second kinetic model for arsenic removal by IIPP

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arsenic removal by IIPP10

Fig.11: Comparision of simulated and field water on adsorption of As (III) by IIPP @ 2011 http://www.ijaest.iserp.org. All rights Reserved. Page 60


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Table 2: Langmuir Adsorption isotherm parameters for As (III) adsorption by IIPP Temperature 293K 303K 313K

qmax ( mg/g) 0.1177 0.1039 0.0798

R2 0.951 0.947 0.919

r 0.007 0.010 0.0062

Table 3: Freundlich adsorption isotherm parameters for As (III) adsorption by IIPP Kf ( mg/g) 0.4172 0.3859 0.345

R2 0.909 0.926 0.979

n 0.0396 0.0367 0.0330

T

Temp 293K 303K 313K

Table 4: Various kinetic and diffusion parameters for As (III) adsorption by IIPP

T (K)

K1 (min-1)

293

0.03086

303

0.003224

313

0.000691

Pseudo-second-order parameters

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Lagergren en parameters R2

h k min (g mg-1 min-1) (mg g--11 m in-1)

R2

25.67

0.06361

1.0

0.960

2.88

0.0071

0.999

0.975

0.1028

0.000284

0.949

A

0.957

Table 5: Physicochemical parameters of field water before and after treatment with IIPP

1 2 3 4 5

pH Turbidity TDS Chloride Sulphate

NTU mg/L mg/L mg/L

Before Treatment 7.18 BDL 440 153 219.86

6

Conductivity

Âľs/cm

325

278

--

7 8 9 10

Total Hardness Total Alkalinity Fe Arsenic

mg/L mg/L mg/L ppb

310 140 0.1637 992.08

219 189 0.1174 8.76

<300 <200 <0.3 <10

Parameter

Unit

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Sr.No

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After Treatment 7.33 BDL 460 142 165.07

Permissible limit BIS 10500-1991 6.5-8. 5 <5.0 <500 <250 <200

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Buddharatna.J.Godboley* et al. / (IJAEST) INTERNATIONAL JOURNAL OF ADVANCED ENGINEERING SCIENCES AND TECHNOLOGIES Vol No. 7, Issue No. 1, 054 - 064

Table 6: Comparison of IIPP with existing adsorbents reported in literature

Adsorbent

pH

Concent ration

Removal efficiency of

(mg/L)

( As III ) in %

5-9

1.0

20-30

Lignite

7.5

1.0

6-14

crush coconut shell,

7.5

1.0

15-33

Illite

7.5

1.0

7-12

Kaolinite clay,

7.5

1.0

5-8 5-8

Rice husk,

7.5

1.0

Fly ash

7.5

1.0

Not detectable Not

Charcoal

7.5

1.0

5-18 5-18

7.5

1.0

26-29 26-29

6.2

1.0

72

Partially activated coconut shell

0-19 0-19

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Yamuna sand

S.Guha eet al., 1990

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Giridih bituminouscoal (GBC).

Reference

S.Prasad et al., 1995

1.0

90-94

K. Pallamreddy et al., 1996

7.1-8.0

1.0

95

J. Lackovic etal., 2000

12

1.1

96.7

S. Kuriakose etal.,2004

Iron oxide coated sand

7.5

0.1

99

V. Gupta et al.,2005

Activated charcoal

8.0

0.05,0.1, 0.5 &1.0

72.71, 68 & 63.

7.0-8.0

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Powder activated alumina (PAA)) and kimberlite tailing Zero- Valent iron

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Iron oxide impregnated activated vated alumina

Activated tea waste

8.0

IIPP

7.0

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0.05,0.1, 0.5 &1.0 1.0

48, 47, 45 & 43. 99.27

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A. Quaff et al., 2005 Present study

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Comparison was made with few reported adsorbents on percentage removal basis and found that IIPP has good percentage removal capacity of As (III) than others. (Ref. Table 6) 13.0 Cost analysis Cost of IIPP was worked out by considering loss and impurities in batch and found Rs. 68.67/kg (Rs.69/kg) which could be low cost of adsorbent to remove as As(III) from drinking water.

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Conclusion • Pre-treatment was required to raw material before using for removal of As (III). • Optimum dose of IIPP was found 20g/L for removal of As (III) of 1 mg/L concentration. • Adsorption capacity was more in the pH range of 6-8. • Optimum time of contact was found 24 hrs. • Adsorption capacity of IIPP on Langmuir model and Freundlich model was 0.1039 mg/g and 0.385 mg/g respectively at 303K. • Freundlich model was best fitted then Langmuir model. • It is apparent from the values of correlation coefficients fort the pseudosecond-order kinetic model fitted well as compared to pseudo first-order model. • All the physicochemical parameter of drinking water was within permissible limits (BIS 10500 -1991) after treatment. • The cost of IIPP was found Rs 69/Kg.

Journal of Hazardous Materials, 189, 286–293, (2011). 2. D.Chakraborti, M.M Rahman, K Paul, U.K.Chowdhury,M.K., Sengupta, D. Lodh , C.R. Chanda, K.C Saha, and S.C.Mukherjee “Arsenic calamity in the Indian subcontinent —What lessons have been learned?” Talanta, 58, 3–22, (2002). 3. Anirban Gupta, Amal Datta and P.Bandopadhyay “Technologies and options for arsenic removal”, IWWA, Annual Convention, Calcutta, 1-9. (1997). 4. D. Mohan and C.U. Pittman. “Arsenic removal from water/wastewater using adsorbents—a critical review.” J. Hazard. Materials, 142, 1–53, (2007). 5. R.M.Dhoble,A.G.Bhole and Sadhana Rayalu. “Adsorption a versatile method for removal of As (III) from water: A state of art:, International Journal of Environmental Engg. and Management, 1, 91-99, ( 2010). 6. Sunbaek Bang, Manish,Patel Lee Lippincott and X.Meng. “Removal of arsenic from groundwater by granular titanium dioxide adsorbent”, Chemosphere, 60,.389-397. (2005). 7. C.Neal and A.J.Robson. “A summary of river water quality data collected within the land ocean interaction study: core data for eastern UK rivers draining to North-Sea,” Sci., Total Enviro., 251/252, 585-665, (2000). 8. C.H., Niu, B Volesky. and D. Cleiman “Bisorption of arsenic (V) with acidwashed crab shell”. Water Research, 41, (11), 2473-2478, (2007). 9. I. Langmuir. “The constitution and fundamental properties of solids and liquids”, J.9 Am. Chem. Soc. 38, 22212295, (1916). 10. T.W. Weber and R.K. Chakraborti “Pore and solid diffusion models for fixed bed adsorbers”. J. American Inst. Chem. Engg., (20), 28-36, (1974). 11. S. Kundu and A.K. Gupta “Adsorptive removal of As (III) from aqueous solution using iron oxide coated

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12.0 Comparison of IIPP with already existing adsorbents.

References 1. Lucy M. Camacho, R. Parra Ramona and Deng Shuguang “Arsenic removal from groundwater by MnO2-modified natural clinoptilolite zeolite: Effects of pH and initial feed concentration”,

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