Abstract
The present study aimed to minimize the environmental impact from the disposal of electrocoagulated metal hydroxide sludge (EMHS) generated during an electrocoagulation process using aluminum electrode by reusing it as an effective adsorbent for simultaneous removal of fluoride ion (F−) and arsenic (As) from aqueous solutions. The adsorbent was characterized by using coupled plasma optical emission spectroscopy (ICP-OES), surface areas and porosity properties, point of zero charge, and X-Ray diffractometry techniques. The surface morphology of adsorbent was studied by scanning electron microscopy (SEM). The dissolution of the adsorbent in function of pH was analyzed in batch experiments. Batch adsorption tests were employed to evaluate the removal and adsorption capacity of adsorbent, under conditions of contact time and adsorbate concentration. In order to determine maximum adsorption capacity of adsorbent and to understand the nature of reaction on their surface, the Langmuir and Freundlich isotherm were calculated. Preferable fitting of the Langmuir isotherm over Freundlich isotherm suggests monolayer coverage of adsorbate at the surface of the adsorbent. Data obtained were also applied to pseudo-first-order and pseudo-second-order equations. The rates of adsorption were found to conform to pseudo-second-order kinetics. The findings of this study revealed that the reuse of EMHS is a promising and efficient adsorbent in order to diminish the fluoride and arsenic pollution from drinking water.
Similar content being viewed by others
Abbreviations
- WHO:
-
World Health Organization
- EMHS:
-
Electrocoagulated metal hydroxide sludge
- EC:
-
Electrocoagulation
- ICP-OES:
-
Inductively coupled plasma optical emission spectroscopy
- XRD:
-
X-ray diffraction
- pHpzc :
-
Point of zero charge
- SEM:
-
Scanning electron microscopy
- BSE:
-
Signal backscattered electrons
- EDS:
-
Energy dispersive spectroscopy
- RL :
-
Separation factor or equilibrium parameter
- SSE:
-
Sum of error squares
- PSO:
-
Particle Swarm Optimization
References
Abernathy, C., Thomasy, D., & Calderon, R. (2003). Toxicity and risk assessment of trace elements. Health effects and risk assessment of arsenic. Am SocNutrSci, 133, 1536–1538.
Afkhami, A., Tehrani, M. S., & Bagheri, H. (2010). Modified maghemite nanoparticles as an efficient adsorbent for removing some cationic dyes from aqueous solution. Desalination, 263, 240–248.
Ayoob, S., & Gupta, A. (2006). Fluoride in drinking water a review on the status and stress effects. Crit Rev Environ SciTechnol, 36, 433–487.
Badruzzaman, M., Westerhoff, P., & Knappe, D. R. U. (2004). Intraparticle diffusion and adsorption of arsenate onto granular ferric hydroxide (GFH). Water Research, 38(18), 4002–4012.
Baig, J., Kazi, T., Arain, M., Afridi, H., Kandhro, G., Sarfraz, R., Jamali, M., & Shah, A. (2009). Evaluation of arsenic and other physico-chemical parameters of surface and ground water of Jamshoro, Pakistan. Journal of Hazardous Materials, 166, 662–669.
Ballinas, M., Rodríguez, E., Rodríguez, D., Silva, O., Munoz, M., & Gyves, J. (2003). Arsenic(V) removal with polymer inclusion membranes from sulfuric acid media using DBBP as carrier. Environ SciTechnol, 38, 886–891.
Berg, M., Caroline, S., Pham, T., Mickey, H., Sampson, L., Leng, M., Samreth, S., & Fredericks, D. (2007). Magnitude of arsenic pollution in the Mekong and Red River Deltas—Cambodia and Vietnam. Science of the Total Environment, 372, 413–425.
Bhatnagar, A., Minocha, A., & Sillanpaa, M. (2010). Adsorptive removal of cobalt from aqueous solution by utilizing lemon peel as biosorbent. BiochemEng J, 48, 181–186.
Bishop, P., & Sansoucy, G. (1978). Fluoride removal from drinking-water by fluidized acticated alumina adsorption. Journal of the American Water Works Association, 70, 554–559.
Brunson, L., & Sabatini, D. (2009). An evaluation of fish bone char as an appropriate arsenic and fluoride removal technology for emerging regions. EnvironEngSci, 26, 1777–1784.
Camacho, L., Torres, A., Saha, D., & Deng, S. (2010). Adsorption equilibrium and kinetics of fluoride on sol gel derived activated alumina adsorbents. Journal of Colloid and Interface Science, 349, 307–313.
Castel, C., Schweizer, M., Simonnot, M., & Sardin, M. (2000). Selective removal of fluoride ions by a two way ion exchange cyclic process. ChemEngSci, 55, 3341–3352.
Chassapis, K., Roulia, M., Vrettou, E., Fili, D., & Zervaki, M. (2010). Biofunctional characteristics of lignite fly ash modified by humates: a new soil conditioner. Bioinorganic ChemAppl, 10, 1–8.
Chen, Y., Lin, M., Xia, Y., Gan, W., Min, D., & Chen, C. (1997). Nutritional survey in dental fluorosis-afflicted area. Fluoride, 30, 77–80.
Choi, W., & Chen, K. (1979). The removal of fluoride from waters by adsorption. Journal of the American Water Works Association, 71, 562–570.
Crittenden, J.C., Berrigan, J.K., Hand, D.W. (1986). Design of rapid small-scale adsorption test for a constant diffusivity. Journal - Water Pollution Control Federation, 58(4), 312–319.
Dang, Q., Olga, N., & Richard, C. (2004). Analytical methods for inorganic arsenic in water: a review. Talanta, 64, 269–277.
Deniz, F., & Karaman, S. (2011). Removal of Basic Red 46 dye from aqueous solution by pine tree leaves. ChemEng J, 170, 67–74.
Dey, R., Swain, S., Mishra, S., Sharma, P., & Patnaik, T. (2011). Hydrogeochemical processes controlling the high fluoride concentration in groundwater: a case study at the Boden block area, Orissa, India. Environmental Monitoring and Assessment, 184, 3279–3291.
Engelolu, Y., KIr, E., & Ers, M. (2002). Removal of fluoride from aqueous solution by using red mud. Sep PurifTechnol, 28, 81–86.
Farooqi, A., Masuda, H., & Firdous, N. (2007). Toxic fluoride and arsenic contaminated groundwater in the Lahore and Kasur districts, Punjab, Pakistan and possible contaminant sources. Environmental Pollution, 145, 839–849.
Gao, S., Sun, R., Wei, Z., Zhao, H., Li, H., & Hu, F. (2009). Size-dependent defluoridation properties of synthetic hydroxyapatite. Journal of Fluorine Chemistry, 130, 550–556.
Goh, K., Lim, T., & Dong, Z. (2009). Enhanced arsenic removal by hydrothermally treated nanocrystalline Mg/Al layered double hydroxide with nitrate intercalation. Environ SciTechnol, 43, 2537–2543.
Gomez, M., Blarasin, M., & Martínez, D. (2009). Arsenic and fluoride in a loess aquifer in the central area of Argentina. Environmental Geology, 57(1), 143–155.
Hameed, B., Ahmad, A., & Latiff, K. (2007). Adsorption of basic dye (methylene blue) onto activated carbon prepared from rattan sawdust. Dyes and Pigments, 75, 143–149.
Hlavay, J., & Polyak, K. (2005). Determination of surface properties of iron hydroxide-coated alumina adsorbent prepared for removal of arsenic from drinking water. J. Colloid InterfSci, 284(1), 71–77.
Ho, Y., & Mckay, G. (1999). Pseudo-second order model for sorption processes. Process Biochemistry, 34, 451–465.
Ho, Y., Ng, J., & McKay, G. (2000). Kinetics of pollutant sorption by biosorbents: review. Separation and Purification Methods, 29, 189–232.
Hu, K., & Dickson, J. (2006). Nanofiltration membrane performance on fluoride removal from water. J MembrSci, 279, 529–538.
Hurtado-Jiménez, R., & Gardea-Torresdey, J. (2006). Arsenic in drinking water in the Los Altos de Jalisco region of Mexico. Pan American Journal of Public Health, 20(4), 236–247.
Islam, M., & Patel, R. (2007). Evaluation of removal efficiency of fluoride from aqueous solution using quick lime. Journal of Hazardous Materials, 143, 303–310.
Jang, M., Chen, W., & Cannon, F. (2008). Preloading hydrous ferric oxide into granular activated carbon for arsenic removal. Environ SciTechnol, 42, 3369–3375.
Joshi, S., Mehta, S., Rao, A., & Rao, A. (1992). Estimation of sodium fluoride using HPLC in reverse osmosis experiments. Water Treat, 7, 207–210.
Kamala, C., Chu, K., Chary, N., Pandey, P., Ramesh, S., Sastry, A., & Sekhar, K. (2005). Removal of arsenic (III) from aqueous solutions using fresh and immobilized plant biomass. Water Research, 39, 2815–2826.
Ku, Y., & Chiou, H. (2002). The adsorption of fluoride ion from aqueous solution by activated alumina. Water, Air, and Soil Pollution, 133, 349–361.
Kuriakose, S., Singh, T. S., & Pant, K. K. (2004). Adsorption of As(III) from aqueous solution onto iron oxide impregnated activated alumina. Water Quality Research Journal of Canada, 39(3), 258–266.
Lakshmipathiraj, P., Narasimhan, B. R. V., Prabhakar, S., & Raju, G. B. (2006). Adsorption of arsenate on synthetic goethite from aqueous solutions. Journal of Hazardous Materials, 136(2), 281–287.
Langmuir, I. (1908). The adsorption of gases on plane surfaces of glass, mica and platinum. J Am ChemSoc, 40(9), 1361–1403.
Li, X., Zhi, J., & Gao, R. (1995). Effect of fluoride exposure on intelligence in children. Fluoride, 28, 189–192.
Lin, T., & Wu, J. (2001). Adsorption of arsenite and arsenate within activated alumina grains: equilibrium and kinetics. Water Research, 35, 2049–2057.
Manju, G. N., Raji, C., & Anirudhan, T. S. (1998). Evaluation of coconut husk carbon for the removal of arsenic from water. Water Research, 32(10), 3062–3070.
Marshall, G., Ferreccio, C., Yuan, Y., Bates, M., Steinmaus, C., Selvin, S., Liaw, J., & Smith, A. (2007). Fifty-year study of lung and bladder cancer mortality in Chile related to arsenic in drinking water. Journal of the National Cancer Institute, 99, 920–928.
Massumi, A., Najafi, N.M., Barzegari, H. (2002). Specification of Cr(VI)/Cr(III) in environmental waters by fluorimetric method using central composite, full and factorial design. Microchemical Journal, 72(1), 93–101.
Myers, R.H., Montgomery, D.C. (1995). Response surface methodology: process and product optimisation using designed experiments. Wiley Series in Probability and Statistics. Wiley, New York.
Mollah, M., Morkovsky, P., Gomes, J., Kesmez, M., Parga, J., & Cocke, D. (2004). Fundamentals, present and future perspectives of electrocoagulation. Journal of Hazardous Materials, 114, 199–210.
Mollah, M., Schennach, R., Parga, J., & Cocke, D. (2001). Electrocoagulation (EC): science and applications. Journal of Hazardous Materials, 84, 29–41.
Nguyen, T., Vigneswaran, S., Ngo, H., & Kandasamy, J. (2010). Arsenic removal by Iron oxide coated sponge: experimental performance and mathematical models. Journal of Hazardous Materials, 182, 723–729.
Nickson, R., McArthur, J., Shrestha, B., Kyaw-Myint, T., & Lowry, D. (2005). Arsenic and other drinking water quality issues, Muzaffargarh District, Pakistan. Applied Geochemistry, 2, 55–68.
Nowak, M., Seubert, A. (1999). Application of experimental design for the characterisation of a novel evolution system for high-capacity anion chromatography with suppressed conductivity detection. Journal of Chromatography. A, 855(1), 91–109.
Ofomaja, A., Naidoo, E., & Modise, S. (2009). Removal of copper(II) from aqueous solution by pine and base modified pine cone powder as biosorbent. Journal of Hazardous Materials, 168, 909–917.
Onyango, M., Kojima, Y., Aoyi, O., Bernardo, E., & Matsuda, H. (2004). Adsorption equilibrium modeling and solution chemistry dependence of fluoride removal from water by trivalent cation exchanged zeolite F-9. Journal of Colloid and Interface Science, 279, 341–350.
Pauwels, H., & Ahmed, S. (2007). Fluoride in groundwater: origin and health impacts. Geosciences, 5, 68–73.
Pommerenk, P., & Schafran, G. (2002). Effects of prefluoridation on removal of particles and organic matter. Journal of the American Water Works Association, 94, 99–108.
Rafique, T., Naseem, S., Usmani, T., Bashir, E., Khan, F., & Bhanger, M. (2009). Geochemical factors controlling the occurrence of high fluoride groundwater in the Nagar Parkar area, Sindh, Pakistan. Journal of Hazardous Materials, 171, 424–430.
Raichur, A., & Jyoti, M. (2001). Adsorption of fluoride onto mixed rare earth oxides. Sep PurifTechnol, 24, 121–127.
Raven, K., Jain, A., & Loeppert, R. (1998). Arsenite and arsenate adsorption on ferrihydrite: kinetics, equilibrium, and adsorption envelopes. Environ SciTechnol, 32, 344–349.
Reardon, E., & Wang, Y. (2000). A limestone reactor for fluoride removal from wastewaters. Environmental Science and Technology, 34, 3247–3253.
Saha, S. (1993). Treatment of aqueous effluent for fluoride removal. Water Research, 27, 1347–1350.
Saifuddin, M., & Kumaran, P. (2005). Removal of heavy metal from industrial wastewater using chitosan coated oil palm shell charcoal. Electronic Journal of Biotechnology, 8, 43–53.
Say, R., Yilmaz, N., & Denizli, A. (2003). Biosorption of cadmium, lead, mercury, and arsenic ions by the fungus Penicillium purpurogenum. Sep SciTechnol, 38, 2039–2053.
Sinha, S., Pandey, K., Mohan, D., & Singh, K. P. (2003). Removal of fluoride from aqueous solutions by Eichhornia crassipes biomass and its carbonized form. IndEngChem Res., 42(26), 6911–6918.
Smith, A., Goycolea, M., Haque, R., & Biggs, M. (1998). Marked increase in bladder and lung cancer mortality in a region of northern Chile due to arsenic in drinking water. American Journal of Epidemiology, 147, 660–669.
Sundaram, C., Viswanathan, N., & Meenakshi, S. (2008). Defluoridation chemistry of synthetic hydroxyapatite at nano scale: equilibrium and kinetic studies. Journal of Hazardous Materials, 155, 206–215.
Vaaramaa, K., & Lehto, J. (2003). Removal of metals and anions from drinking water by ion exchange. Desalination, 155, 157–170.
Vega, L., Styblo, M., Patterson, R., Cullen, W., Wang, C., & Germolec, D. (2001). Differential effects of trivalent and pentavalent arsenicals on cell proliferation and cytokine secretion in normal human epidermal keratinocytes. ToxicolApplPharmacol, 172, 225–232.
Violante, A., Gaudio, S., Pigna, M., Ricciardella, M., & Banerjee, D. (2007). Coprecipitation of arsenate with metal oxides: 2. Nature, mineralogy, and reactivity of iron(III) precipitates. EnvironSciTechnol, 41, 8275–8280.
Violante, A., Pigna, M., Del Gaudio, S., Cozzolino, V., & Banerjee, D. (2009). Coprecipitation of arsenate with metal oxides: 3. Nature, mineralogy, and reactivity of iron(III)–aluminum precipitates. Environ SciTechnol, 43, 1515–1521.
Waldbott, G. (1998). The pre-skeletal phase of chronic fluoride intoxication. Fluoride, 31, 13–20.
Warren, C., Burgess, W., & Garcia, M. (2005). Hydrochemical associations and depth profiles of arsenic and fluoride in quaternary loess aquifers of northern Argentina. Mineralogical Magazine, 69, 877–886.
Weng, Y., Chaung-Hsieh, L., Lee, H., Li, K., & Huang, C. (2005). Removal of arsenic and humic substances (HSs) by electro-ultrafiltration (EUF). Journal of Hazardous Materials, 122, 171–176.
WHO—Word Health Organization (2011) Guidelines for Drinking-Water Quality, Fourth ed.
Wood, J. (1974). Biological cycle for toxic elements in the environment. Science, 183, 1049–1052.
Xu, Y., Dai, Y., Zhou, J., Xu, Z., Qian, G., & Lu, G. (2010). Removal efficiency of arsenate and phosphate from aqueous solution using layered double hydroxide materials: intercalation vs. precipitation. Journal of Materials Chemistry, 20, 4684–4691.
Yuan, Y., Marshall, G., Ferreccio, C., Steinmaus, C., Selvin, S., Liaw, J., Bates, M., & Smith, A. (2007). Acute myocardial infarction mortality in comparison with lung and bladder cancer mortality in arsenic-exposed Region II of Chile from 1950 to 2000. American Journal of Epidemiology, 166, 1381–1391.
Zohouri, F., & Rugg-Gunn, A. (2000). Sources of dietary fluoride intake in 4-year-old children residing in low, medium and high fluoride areas in Iran. Int J Food SciNutr, 51, 317–326.
Acknowledgments
The authors acknowledge the financial support provided by National Council of Science and Technology of Mexico (CONACYT) for their financial support to this study.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no competing interests.
Electronic supplementary material
Below is the link to the electronic supplementary material.
Supplementary Fig. S1
SEM micrographs and EDS spectrum showing the main elemental chemical composition from EMHS: (a) 100 μm reference scale, and (b) 30 μm reference scale (JPEG 313 kb)
Supplementary Fig. S2
SEM micrographs and EDS spectrum showing the presence of Au from EMHS: a) 300 μm reference scale, b) 100 μm reference scale, c) 30 μm reference scale, and d) EDS spectrum (JPEG 376 kb)
Supplementary Fig. S3
SEM micrographs and EDS spectrum showing the presence of Fe from EMHS: (a) 20 μm reference scale, and (b) 40 μm reference scale (JPEG 284 kb)
Supplementary Fig. S4
SEM micrographs and EDS spectrum showing the presence of Pb from EMHS (JPEG 156 kb)
Rights and permissions
About this article
Cite this article
García-Gómez, C., Rivera-Huerta, M.L., Almazán-García, F. et al. Electrocoagulated Metal Hydroxide Sludge for Fluoride and Arsenic Removal in Aqueous Solution: Characterization, Kinetic, and Equilibrium Studies. Water Air Soil Pollut 227, 96 (2016). https://doi.org/10.1007/s11270-016-2783-5
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-016-2783-5