REMOVAL OF FLUORIDE FROM GROUND WATER BY USING TREATED BARK OF PHYLLANTHUS EMBLICA (AMLA) TREE

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1 International Journal of Civil Engineering and Technology (IJCIET) Volume 7, Issue 6, November-December 216, pp. 11 2, Article ID: IJCIET_7_6_2 Available online at ISSN Print: and ISSN Online: IAEME Publication REMOVAL OF FLUORIDE FROM GROUND WATER BY USING TREATED BARK OF PHYLLANTHUS EMBLICA (AMLA) TREE Ranjit N. Patil Research Scholar, G. H. Raisoni College of Engineering, Nagpur, Maharashtra, India Dr. P. B. Nagarnaik Dean Academics, G. H. Raisoni College of Engineering, Nagpur, Maharashtra, India Dr. D. K. Agrawal Professor, B.D. College of Engineering, Sevagram, Maharashtra, India ABSTRACT Fluoride is the essential element for dental health and growth of bones as well whereas excess quantity of fluoride creates a problem of human health. It is very much essential to control the excess level of fluoride concentration (WHO) <1.5 mg/l. Several methods and techniques were used by researchers throughout the decades for the control of fluoride ion. This research paper addresses Phyllanthus Emblica (Amla) bark for the estimation of fluoride. The Physico chemical characterization followed SEM, FTIR, CHN analysis etc. The batch experimental study followed the adsorption parameters, ph (6-8), dose (.5-5 mg/l), initial concentration (5mg/L), particle size (75-3μm) and time of contact (6-72 Min.). It follows Langmuir & Freundlich. Key words: Fluoride, Water, Langmuir, Freundlich. Cite this Article: Ranjit N. Patil, Dr. P. B. Nagarnaik and Dr. D. K. Agrawal, Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree. International Journal of Civil Engineering and Technology, 7(6), 216, pp INTRODUCTION India is one of the country were millions of people lack access to clean and safe water and some are drinks contaminated water (Giridharadas, 25). Many people s are faced the problem of dental fluorosis. Around 2 million peoples are under the risk of dental fluorosis. (Mohan et al., 212).From the study, the Fluoride ions is essential in some concentration for the dental health and excess is dangerous for the human health. In case of dental health and bone improvement.8 mg/l to 1. mg/l is beneficial. (N.C.R. Rao) It is necessary to control the level of fluoride ions to avoid many problems occurs due to its excess presence. In the earth crust fluoride has observed 13 th most abundant element [1]. Worldwide 32 % prevalence of fluorosis is reported [2]. Skeletal fluorosis is commonly observed symptoms of fluoride; it affects and can lead towards permanent damage of bone and joint deformations and also cause dental fluorosis. According to the directions of various authorities 1 mg/l is the permissible safe limits of fluoride in drinking water 11 editor@iaeme.com

2 Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree [3]. Fluoride contamination observed in some part of Asia, Africa, America and Europe. The range of contamination was observed from 1 35 mg/l in ground water and.1 to 3 mg/l in fresh water [4]. Adsorption analysis is a process used by the investigators effectively for the fluoride removal from water and waste water also. Activated carbon is one of the important medium used widely because of its versatile adsorption uptake capacity for the organic compound at the same time the available commercial based activated carbon is very much costly medium used in the process of adsorption and its regeneration is also very difficult [5]. Adsorption is an effective medium for the control of fluoride contamination observed by the researchers. The low cost efficient adsorbent is still difficult and this is the reason, the researchers targeted on easily available but economically feasible low cost single or composites bioadsorbents such as babool bark [6],mango, java plum and neem tree barks[7], neem [8] seed coat of tur [9], Camellia sinensis [1],corn cob [11], orange peel [12], turkish red pine [13], gooseberry seeds [14], Guava bark [15], Khaya senegalensis fruits[16] etc. Somehow the bio-adsorbents have a good affinity of fluoride removal observed in drinking water however some of are not very high adsorptive capacity but found very much low cost. So the demands of new economically feasible adsorbent are still remain. Many bio adsorbents were studied for the removal of toxic compounds not only from drinking water but also used for the industrial waste water purposes. In this study, Phyllanthus Emblica (Amla) modified Tree Bark (TBP) is used as a low cost bio adsorbent which is one of the alternatives for commercially available activated carbon. The objective of the study is to remove the unwanted excess contamination of fluoride ions from drinking water and to make it drinkable. The selected TBP has a good efficiency of removal of fluoride and due to the easy availability it can be feasible for the future used for the removal of other metal ions. 2. MATERIAL AND METHODS 2.1. Preparation of Adsorbent Defluoridation was studied using the bark of Phyllanthus Emblica (Amla) as an adsorbent. The bark was collected from near the forest area of Chandrapur District, Maharashtra State, India. Collected bark was washed with tap water so that the mud, trash etc. removed easily and sun dried for three days. Completely dried bark was cut in to small pieces and washed with double distilled water. Washed bark was again sun dried for a day. The cut pieces of bark were grounded and sieved through required sieve sizes of 75,15,3,425 & 6 µm [17] Modification of Bark The grounded bark was modified by providing the treatment of Aluminium sulphate AR grade (4.5 g) was added in deionized water (2 ml). Phyllanthus Emblica (Amla) powder 2.5 g was added in this mixture and allowed to agitate for 3 hrs. at 15 rpm. The mixed was dried at 15 C for 2.5 hrs. and kept in muffle furnace for calcinations at 75 C for 3 hrs. The calcined material was washed with 1 (Material): 2 (deionized water) [18] shaking at 15 rpm for 24 hrs continuously and then extra washed of distilled water provide and dried in oven at 15 C for 24 hrs. Treated material kept in air tight plastic container for further experimentation used Adsorbate and Experimentation Fluoride stock solution was prepared by dissolving 2.21 g of anhydrous sodium fluoride of AR grade in l ml of deionized water in volumetric flask. Experimentations conducted in batch adsorption analysis in the laboratory for the initial concentration of fluoride ion of 5 mg/l [19]. Test solution volume of 1 ml used in 25 ml capacity plastic bottles. These bottles were agitated at a constant rate of 15 rpm in a temperature controlled orbital shaker incubator. The ph of test solution was adjusted by.1 N HCl or.1 N NaOH aqueous solutions. The samples were withdrawn at different time of intervals to observe the time of equilibrium. Removal of fluoride ion was found by using UV beam Spectrophotometer editor@iaeme.com

3 Ranjit N. Patil, Dr. P. B. Nagarnaik and Dr. D. K. Agrawal 2.4. Plant Description The tree of Phyllanthus Emblica (Amla) is generally found in small and medium in size and found in all around the districts of Maharashtra. It is also found in all parts of India and also located in Sri Lanka, Pakistan, China, Malaysia Uzbekistan and South East Asia. It has a height of about 8-18m with thin light grey bark, simple leaves in light green colour (figure1). [Swetha Dasaroju, Krishna Mohan Gottumukkala] 3. RESULTS AND DISCUSSION Figure 1 http: :homeremediess.com/amla-medicinal-plant-uses-p pictures 3.1. Physical Characterization of TBP Table 1 Chemical compositions of Phyllanthus Emblica (Amla) % MC % VM % AC % FC % H % N The chemical composition shows the good percentage of fixed carbon with less moisture content. The treated bark of Phyllanthus Emblica (Amla) has good physical characteristics required for the adsorption of fluoride ions from ground water (figure 2). 1 Charecerization of TBP 8 Values in % % MC % VM % AC % FC % H % N % Content Figure 2 Proximate and Ultimate analysis of Phyllanthus Emblica (Amla) 13 editor@iaeme.com

4 Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree 3.2. XRD Analysis XRD of treated bark of Phyllanthus Emblica (TBP) were performed to predict changes in the crystal structure of the TBP. From few decades, X-ray diffraction (XRD) analyses were one of the most prominent techniques in the scientist era for the identification of a crystal study and the nature of material [2]. XRD patterns of before and after the adsorption of fluoride ions of Phyllanthus Emblica (Amla) bark. Figure 2 (a) shows the TBP before the fluoride ion adsorption showing symmetric, sharp peaks. These peaks show the nature of crystalline, while the figure (b) shows the position and nature of peaks after fluoride ions adsorption and found no formation of peaks, which resembles about that it s an amorphous structure (figure 3). Figure 3 XRD Image of PTB (Loaded and Un-loaded) The XRD analysis of the powdered samples of loaded and unloaded of PTB were recorded and scanned for diffraction angle of 2θ ranging up to Scanning Electron Microscopy (SEM) Figure 4 [A] Unloaded [B] Loaded To study the effect of degradation process the surface morphology of loaded and unloaded adsorbent of PTB were recorded as shown in figure (4 A & B). SEM observations of loaded and unloaded adsorbent obtained from thermal degradation and aluminium sulphate treatment to natural Phyllanthus Emblica (Amla) bark. Materials recordedd its complex and porous surface texture. SEM images show porous morphology of PTB and grainy surface. These may contribute to the relatively high surface area of the 14 editor@iaeme.com

5 Ranjit N. Patil, Dr. P. B. Nagarnaik and Dr. D. K. Agrawal PTB. The research suggests that these pores represent the active sites for adsorption of organic and inorganic pollutants from aqueous solution [21] Effect of Adsorbent Dose Effects of adsorbent dose.5g/l- 5. g/l were studied in batch adsorption analysis of test solution volume 1 ml for an initial fluoride concentration of 5 mg/l. Figure 5 shows the removal of fluoride ions for increasing the dose of TBP and the optimum value of dose was obtained 1.5 g/l. The removal efficiency of amla bark was observed % for bring down the fluoride level.8-1. mg/l. The optimized doze of 1.5g/L was used for further study. Dose Vs. qe Dose (g/l) Figure 5 Dose of adsorbent Vs. % removal Initial fluoride concentration 5 mg/l; ph 7; agitation 15 rpm; temp.3c; Volume of sample 1 ml 3.5. Effect of ph The effect of ph study was performed in laboratory for the ph range of 2 to 1. From the ph data observations the graph has plots which shown in figure 6. The fluoride removal efficiency increased with increasing ph up to 8 for a optimum dose of 1.5 g/l and then sudden falls down due to the adsorption sites accumulation in the process of adsorbent [22]. The maximum adsorption was found for the ph range of 6. and ph Vs ph Figure 6 ph Vs. % removal Initial fluoride concentration 5 mg/l; agitation 15 rpm; temp.3 C; Dose 15 g/l; Volume of sample 1 ml 15 editor@iaeme.com

6 Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree 3.6. Effect of Contact Time The contact time is an important parameter in the process of adsorption. The optimized quantity of PTB was added in the laboratory test sample plastic bottles of 25 ml capacity of volume 1 ml containing 5 mg/l of initial fluoride concentration and allowed for agitation in incubator for a time of period intervals 15 min to 144 min. at a speed of agitation 15 rpm and degree of temperature is 27 ± 3 C. The test solutions were checked at the particular time of intervals and a time Vs. % removal graph was plotted and the time of equilibrium recorded 3 min. shown in fig. 7. The adsorption capacity was obtained more in the initial stage and changing with time increases up to some extents and then after decreases and observed significant change in the adsorption. During the adsorption, it was happened because of the diffusion occurred in the PTB surface adsorption pores [23]. 1 Time of contact Vs Time (Min) Figure 7 Time Vs. Initial fluoride concentration 5 mg/l ; ph 8 ; agitation 15 rpm ; temp.3 C ; Dose 15 g/l; Volume of sample 1 ml 3.7. Effect of Initial Metal Ion Concentration Different initial concentrations 3 mg/l, 5mg/L, 7 mg/l, 1 mg/l and 15 mg/l was studied. With increase in the initial fluoride concentration, adsorbent material exhausted slowly shown in Figure 8. Higher capacity of adsorption found in lower concentrations of fluoride. 1 Initial concentration Vs Initial concentration (mg/l) Figure 8 Initial Concentration Vs. Conditions: Initial fluoride conc. 5 mg/l; ph 8; agitation 15 rpm; temp.3c; Dose 15 g/l; Volume of sample 1 ml 16 editor@iaeme.com

7 Ranjit N. Patil, Dr. P. B. Nagarnaik and Dr. D. K. Agrawal 3.8. Effect of Particle Size The effect of particle size in the process adsorption by using PTB was examined for the 5 mg/l initial concentration of fluoride ions. The analysis obtained the significant change in the adsorption uptake capacity of PTB due to change occurred in numerous of adsorption sites. The IS sieves (75-3 µm) was used to know the particle size impact over the PTB adsorption process. The analysis shows that the fluoride removal capacity more observed in smaller size of particles while less in higher particles size because of the maximum adsorption surface area available in case of smaller size particles. It also affects and reduces outer mass transfer resistance [24]. Figure 9 shows the particle size Vs.% removal of fluoride. 1 Particle Size Vs Particle Size (µm) Figure 9 Particle Size Vs. Conditions: Initial fluoride conc. 5 mg/l ; ph 8 ; agitation 15 rpm ; temp.3c ; Dose 15 g/l; Volume of sample 1 ml 4. ADSORPTION MODELS The isotherm study focused on the interaction of adsorbate with adsorbent. The data were observed in related in Langmuir and Freundlich adsorption isotherms. The Langmuir isotherm is a presumption depends that the removal due to monolayer sorption happens on a homogeneous surface of adsorbent without any collaboration between adsorbed particles were as Freundlich is equilibrium sorption based adsorption on the heterogeneous surfaces. Following are the linear equations of Langmuir and Freundlich isotherms shown in equation (a) & (b) respectively. 1 = 1 1 ( ) Equation (a) + 1 In the above equation, the fluoride adsorbed capacity is denoted by qe in mg/g and qmax is the maximum amount adsorbed in mg/g; the equilibrium fluoride concentration is denoted by Ce in mg/l; Langmuir isotherm constant is denoted by KL in L/mg. log =log + 1 log Equation (b) In equation 2, the equilibrium fluoride concentration is denoted by Ce and qe is the amount adsorbed in mg/g; KF is the empirical constant of Freundlich in mg/g and 1/n is the Freundlich exponent. The linear plot shows the Langmuir and Freundlich isotherm application in Fig.1 & editor@iaeme.com

8 Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree 1 vs. 1 The data plot in both the adsorption shows the good correlation coefficients for Freundlich isotherm as compare to Langmuir. The R 2 value obtained in Freundlich (R 2 =.976 ) is more than the Langmuir (R 2 =.986). The data followed the Freundlich isotherm than the Langmuir. Figure 1 shows the Langmuir isotherm [25]. 2.5 Langmuir y =.977x R² = /qe K Linear (33 K) /Ce Figure 1 Langmuir Isotherm The study predicted that the nature of surface adsorbent was heterogeneous and suitable for adsorption. Figure 11 shows the Freundlich isotherm..1 Freundlich y =.658x R² =.92 log qe K Linear (33 K) -.5 log Ce Figure 11 Freundlich Isotherm 5. CONCLUSION From the observations and the results, it has found that the adsorbent of Amla bark required pre-treatment for the removal of fluoride ions from ground water. The dose of PTB optimizes 1.5 g/l for the concentration of fluoride ions 5 mg/l at ph 6-8. Maximum removal recorded at minimum initial concentrations. The optimum time of contact was found 6 Min. The lower size particle sieved PTB has more resulted uptake capacity of fluoride ions. Scanning Electron Microscopy (SEM) of PTB shows enough capacity of pores to remove fluoride ions Adsorption model of PTB well fitted in Langmuir as well as in Freundlich model at 33K editor@iaeme.com

9 Ranjit N. Patil, Dr. P. B. Nagarnaik and Dr. D. K. Agrawal REFERENCE [1] Maheshwari R.C.Meenakshi, Fluoride in drinking water and its removal Journal of Hazardous Materials, Vol.B137, (26), [2] Bhargava, D.S., Killedar, D.J., Fluoride adsorption on fishbone charcoal through a moving media adsorber. Vol.26, 1992, [3] Ranjit N. Patil, DR. P. B. Nagarnaik, DR. D. K. Agrawal (215). Removal of fluoride from water by using bio-adsorbents: a state of art. International journal of pure and applied research in engineering and technology Vol. 3 (9): [4] S.P.Teotia, M. Teotia, R.K. Singh, Hydrogeo chemical aspects of endemic skeletal fluorosis in India-an epidemiological study, Fluoride 14 (1981) [5] A. K. Patil1, V. S. Shrivastava, Alternanthera bettzichiana Plant powder as Low Cost Adsorbent for Removal of Congo red from Aqueous Solution. International Journal of ChemTech Research Vol.2 (2): [6] Bhagyashree M Mamilwar, A.G.Bhole, A.M.Sudame, Removal Of Fluoride From Ground Water By Using Adsorbent, International Journal of Engineering Research and Applications, 2 ( 4) 212, [7] S. Mumtazuddin, AK. Azad, International Journal of Advances in Pharmacy, Biology And Chemistry Vol. 1(3), Jul- Sep, 212 ISSN: [8] A. V. Jamode,V. S. Sapkal, V. S. Jamode, Defluoridation of water using inexpensive adsorbents, J. Indian Inst. Sci., Sept. Oct. 24, 84, [9] Dipak Mangrulkar, R.M. Dhoble, Ranjeet Kirkate, Defluoridation from Groundwater by Seed Coat of Tur (SCOT): A Low Cost Adsorbent, International Journal of Environmental Research and Development. Volume 1, Number 1 (211), pp [1] Sharmila. D, P. Muthusamy, Removal of heavy metal from industrial effluent using bio adsorbents(camellia sinensis) Journal of Chemical and Pharmaceutical Research, 213, 5(2):1-13 [11] Rasha Salah Mahdi, Removal of The Blue Methylene Dye from an Aqueous Solution By Using Powdered Corn Cob,International journal of Civil Engineering and technology, Volume 5, Issue 1, January (214), pp [12] Afrah A. Hassan, Removal of Reactive Red 3b From Aqueous Solution By Using Treated Orange Peel, International journal of Civil Engineering and technology, Volume 5, Issue 3, March (214), pp [13] Suleyman Baslar, Yunus Dogan, Nazmi Durkan,Huseyin Bag, Biomonitoring of zinc and manganese in bark of Turkish red pine of western Anatolia, Journal of Environmental Biology, 3(5) (29) [14] J. Aravind; G. Sudha; P. Kanmani; A.J. Devisri; S. Dhivyalakshmi; M. Raghavprasad, Equilibrium and kinetic study on chromium (VI) removal from simulated waste water using gooseberry seeds as a novel biosorbent, Global J. Environ. Sci. Manage., 1(3): , Summer 215 ISSN [15] Deepa Panhekar, Activated Tree Bark as an Adsorbent for Heavy Metal Removal:Study Through Isotherm Analysis, International Journal of Chemical and Physical Sciences, ISSN: IJCPS Vol. 4 Special Issue NCSC Jan editor@iaeme.com

10 Removal of Fluoride from Ground Water by Using Treated Bark of Phyllanthus Emblica (Amla) Tree [16] Casmir E. Gimba1, Odike Ocholi, Peter A. Egwaikhide, Turoti Muyiwa, Emmanuel E. Akporhonor, New raw material for activated carbon. I. Methylene blue adsorption on activated carbon prepared from Khaya senegalensis fruits, Cien. Inv. Agr. 36(1): [17] Ranjit N. Patil, Dr. P. B. Nagarnaik, Dr. D. K. Agrawal, An Experimental Analysis of Adsorption Behavior of HTB for the Removal of Fluoride, International Journal of Engineering Research & Technology, 4 (216) [18] Sanghranta S. Waghmare,Tanvir Arfin, Nilesh Manwar, Dilip H. Lataye, Nitin Labhsetwar & Sadhana Rayalu, Preparation and Characterization of Polyalthia longifolia Based Aluminaas a Novel Adsorbent for Removing Fluoride from Drinking Water, Asian J. Adv. Basic Sci.: 215, 4(1), [19] Manisha Poudyal 1, Sandhya Babel, Removal of Fluoride using Granular Activated Carbon and Domestic Sewage Sludge, 4th International Conference on Informatics, Environment, Energy and Applications Volume 82 of IPCBEE (215) [2] Dilip Thakre, Priyadarshini Dixit, Sanghratna Waghmare, Nilesh Manwar, Nitin Labhsetwar and Sadhana S. Rayalu, Synthesis Optimization and Fluoride Uptake Properties of High Capacity Composite Adsorbent for Defluoridation of Drinking Water, Environmental Progress & Sustainable Energy, AIChE (Vol., No.) March 215 [21] Sanghratna Waghmare1, Dilip Lataye2, Tanvir Arfin3, Nilesh Manwar4, Sadhana Rayalu5, Nitin Labhsetwar, Adsorption Behavior of Eggshell Modified Polyalthia Longifolia Leaf based Alumina as a Novel adsorbents for Fluoride Removal from Drinking water, International Journal of ARIIE-ISSN(O) pp [22] Angelie I. Jover, Jonathan W. L. Salvacion, Adsorption Capability of Gmelina arborea Bark using Crystal Violet 2nd International Conference on Environment and Industrial Innovation IPCBEE vol.35 (212),87-92 [23] Shihabudheen M. Maliyekkal, Sanjay Shukla, Ligy Philip, Indumathi M. Nambi, Enhanced fluoride removal from drinking water bymagnesia-amended activated alumina granules, Chemical Engineering Journal 14 (28) [24] M.Mamatha, H.B.Aravinda, S.Manjappa, E.T.Puttaiah, Kinetics and Mechanism for Adsorption of Lead in Aqueous and Industrial Effluent from Pongamia pinnata Tree Bark, Journal Of Environmental Science, Toxicology And Food Technology, Volume 2, Issue 3 (Nov. - Dec. 212), PP 1-9 [25] Sanghratna Waghmare, Tanvir Arfin, Sadhana Rayalu, Dilip Lataye, Samujjwala Dubey, Sangeeta Tiwari, Adsorption Behaviour of Modified Zeolite as Novel Adsorbents for Fluoride Removal from Drinking Water: Surface Phenomena, Kinetics and Thermodynamics Studies International Journal of Science, Engineering and Technology Research (IJSETR), Volume 4, Issue 12, December [26] K. Kamal Das, D. Vijay Kumar, G. Udayalaxmi and M. Muralidhar, Fluoride Contamination in the Groundwater in Mathadi Vague Basin in Adilabad District, Telangana State, India. International Journal of Civil Engineering and Technology (IJCIET), 5(7), 214, pp [27] C. P. Pise, Dr. S. A. Halkude, Blend of Natural and Chemical Coagulant for Removal of Turbidity in Water. International Journal of Civil Engineering and Technology (IJCIET), 3(2), 212, pp editor@iaeme.com