Study of Remediation of Soil Contamined with Heavy Metals by Coal Fly Ash

Elżbieta Sitarz-Palczak, Jan Kalembkiewicz

Department of Inorganic and Analytical Chemistry, Faculty of Chemistry, Rzeszów University of Technology, Rzeszów, Po- land.

DOI: 10.4236/jep.2012.310156                

Abstract

The labile fraction of heavy metals in soils is the most important for toxicity for plants. Thus it is crucial to reduce this fraction in contamined soils to decrease the negative effect of heavy metals. In an experiment, the effects of two additives on the labile fractions of Cu, Mn and Zn were investigated in a soil contamined during long-term application. The additive used was the coal fly ash. The treated soil was further enriched with heavy metals and allowed to age at room temperature for 30 days. After this period, they were extracted plant-available (EDTA; HNO₃; CH₃COOH) metal species. The addition of fly ash strongly reduced the plant-available of Mn for plants but to a lesser extent this applies to the plant-available of Cu and Zn for plants. By addition of 1% of fly ash as well as 2% of fly ash, the labile fraction of Cu, Mn and Zn were lowered by 6.3, 145.0 and 29.7 mg?kg^-1, respectively. Moreover essential correlation between total Cu and Zn contents was stated in the soil with plant-available content of metals, with reference to both metals. Value of coefficients of correlation is attesting to it between the total and plant-available Cu and Zn contents which are respectively equal: R(Cu) = 0.845, R(Mn) = 0.864 and R(Zn) = 0.872 for p = 99.5%. The results suggested that leading into the soil of the additional amount of fly ash can be an effective way of chemical remediation with reference to soils contaminated by Cu or Mn or Zn. Because he causes immobilization of examined heavy metals in the soil and in the process in the arrangement a—soil is limiting the availability of these metals plant and more distant bonds of the food chain.

Keywords

Soil Remediation; Heavy Metals; Coal Fly Ash; FAAS

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1]	B. J. Alloway, “Heavy Metals in Soils,” John Wiley & Sons, New York, 1990.
[2]	B. J. Alloway and D. C. Ayres, “Chemical Principles of Environmental Pollution,” 2nd Edition, Blackie Academic & Professional (Chapman & Hall), London, 1997, pp. 205- 211.
[3]	A. Bradshaw, “The Use of Natural Processes in Reclamation—Advantages and Difficulties,” Landscape and Urban Planning, Vol. 51, No. 2-4, 2000, pp. 89-100.doi:10.1016/S0169-2046(00)00099-2
[4]	“The Regulation on Minister of Environment of 9 September 2002 r. on the Quality Standards for Soil and Land—Dz. U. Nr 165, poz. 1359,” Polish Ministry of Environment, Varsov, 2002.
[5]	S. Tandy, K. Bossart, R. Mueller, J. Ritschel, L. Hauser, R. Schulin and B. Nowack, “Extraction of Heavy Metals from Soils Using Biodegradable Chelating Agents,” Environmental Science & Technology, Vol. 38, No. 3, 2004, pp. 937-944. doi:10.1021/es0348750
[6]	G. M. Hettiarachchi, G. M. Pierzynski and M. D. Ransom, “In Situ Stabilization of Soil Lead Using Phosphorus and Manganese Oxide,” Environmental Science & Technology, Vol. 34, No. 21, 2000, pp. 4614-4619.doi:10.1021/es001228p
[7]	E. Lombi, R. E. Hamon, S. P. McGrath and M. J. Mc- Laughlin, “Lability of Cd, Cu and Zn in Polluted Soils Treated with Lime, Beringite, and Red Mud and Identi- fication of a Non-Labile Colloidal Fraction of Metals Using Isotopic Techniques,” Environmental Science & Technology, Vol. 37, No. 5, 2003, pp. 979-984. doi:10.1021/es026083w
[8]	G. Heron, M. Van Zutphen, T. H. Christensen and C. G. Enfield, “Soil Heating for Enhanced Remediation of Chlorinated Solvents: A Laboratory Study on Resistive Heating and Vapor Extraction in a Silty, Low-Permeable Soil Contaminated with Trichloroethylene,” Environmental Science & Technology, Vol. 32, No. 10, 1998, pp. 1474- 1481. doi:10.1021/es970563j
[9]	S. I. Wada and Y. Umegaki, “Major Ion and Electrical Potential Distribution in Soil under Electrokinetic Re- mediation,” Environmental Science & Technology, Vol. 35, No. 11, 2001, pp. 2151-2155. doi:10.1021/es001335j
[10]	J. Singh, S. D. Comfort and P. J. Shea, “Iron-Mediated Remediation of RDx-Contaminated Water and Soil under Controlled Eh/Ph,” Environmental Science & Technology, Vol. 33, No. 9, 1999, pp. 1488-1494. doi:10.1021/es9806175
[11]	M. O. Oyanader, P. E. Arce and A. Dzurik, “Design Criteria for Soil Cleaning Operations in Electrokinetic Re- mediation: Hydrodynamic Aspects in an Annular Ge- ometry,” Industrial & Engineering Chemistry Research, Vol. 44, No. 16, 2005, pp. 6200-6211.doi:10.1021/ie049045p
[12]	L. Zhongming, Y. Ji-Wei and N. Ivars, “Electroreme- diation: Removal of Heavy Metals from Soils by Using Cation Selective Membrane,” Environmental Science & Technology, Vol. 32, No. 3, 1998, pp. 394-397.doi:10.1021/es9703584
[13]	Y. L. Wei, Y. W. Yang and N. Cheng, “Study of Ther- mally Immobilized Cu in Analogue Minerals of Contami- nated Soils,” Environmental Science & Technology, Vol. 35, No. 2, 2001, pp. 416-421. doi:10.1021/es0008721
[14]	W. Y. Shi, H. Shao, H. Li, M. Shao and S. Du, “Progress in the Remediation of Hazardous Heavy Metal—Polluted Soils by Natural Zeolite,” Journal of Hazardous Mater- ials, Vol. 170, No. 1, 2009, pp. 1-6. doi:10.1016/j.jhazmat.2009.04.097
[15]	B. Lothenbach, G. Furrer, H. Scharli and R. Schulin, “Immobilization of Zinc and Cadmium by Montmoril- lonite Compounds: Effects of Aging and Subsequent Aci- dification,” Environmental Science & Technology, Vol. 33, No. 17, 1999, pp. 2945-2952. doi:10.1021/es981317q
[16]	B. Kos and D. Lestan, “Induced Phytoextraction/Soil Washing of Lead Using Biodegradable Chelate and Per- meable Barriers,” Environmental Science & Technology, Vol. 37, No. 3, 2003, pp. 624-629. doi:10.1021/es0200793
[17]	A. Kabata-Pendias, M. Piotrowska and T. Witek, “Evalua- tion of the Quality and Capabilities of Agricultural Use of Soils Contamined with Heavy Metals,” Soil Science and Plant Institute, Pu?awy, 1993.
[18]	A. Kabata-Pendias and H. Pendias, “Biogeochemistry of Trace Elements,” Polish Scientific Publishing Company, Varsov, 1999.
[19]	A. Badora, G. Furrer, A. Grünwald and R. Schulin, “Immo- bilization of Zinc and Cadmium in Polluted Soils by Polynuclear Al13 and and Al-Montmorillonite,” Journal of Soil Contamination, Vol. 7, No. 5, 1998, pp. 573-588.
[20]	M. Mench, J. Vangronsveld, N. Lepp and R. Edwards, “Physicochemical Aspects and Efficiency of Trace Ele- ment Immobilization by Soil Amendments,” In: J. Van- gronsveld and S. Cunningham, Eds., Metal-Contaminated Soils: In-Situ Inactivation and Phytorestoration, Springer Verlag and Landes Bioscience, New York, 1998, pp. 151- 182.
[21]	L. A. Oste, T. M. Lexmond and W. H. Van Riemsdijk, “Metal Immobilization in Soils Using Synthetic Zeolites,” Journal of Environmental Quality, Vol. 31, No. 3, 2002, pp. 813-821. doi:10.2134/jeq2002.0813
[22]	B. Gworek, “Inactivation of Cadmium in Contaminated Soil Using Synthetic Zeolites,” Environmental Pollution, Vol. 75, No. 3, 1992, pp. 269-271.doi:10.1016/0269-7491(92)90126-U
[23]	I. Corrales, P. Barcelo and J. Barcelo, “Influence of Silicon Pretreament on Aluminum Toxicity in Maize Roots,” Plants and Soil, Vol. 190, No. 2, 1997, pp. 203-209.doi:10.1023/A:1004209828791
[24]	A. Badora, “Aluminium Solubility in the Presence of Citric Acid,” Advances of Agricultural Sciences Problem Issues, Polish Academy of Sciences, Varsov, 1998, pp. 197-201.
[25]	A. Karczewska, T. Chodak and J. Kaszubkiewicz, “The Suitability of Brown Coal as a Sorbent for Heavy Metals in Polluted Soils,” Applied Geochemistry, Vol. 11, No. 1-2, 1996, pp. 343-346. doi:10.1016/0883-2927(95)00043-7
[26]	A. Maciejewska, “An Organic-Mineral Fertilizer from Brown Coal Applied to Soil Decreases Cadmium, Lead and Zinc Concentrations in Plants. Understanding and Managing Organic Matter in Soils,” Sediments and Waters, Vol. 44, No. 3, 2001, pp. 517-523.
[27]	A. Maciejewska, “Study of the Properties and Fertility of Sandy Soil after the Use of Unconventional Fertilizer Obtained from Lignite,” Acta Academic Agricultural Technical Academy Olsztyn, Agricultural Academy Olsztyn, 1994, pp. 1-67.
[28]	V. Laperche, S. J. Traina, P. G. Gaddam and T. J. Logan, “Chemical and Mineralogical Characterization of Pb in Contamined Soil. Reactions with Apatite,” Environmental Science & Technology, Vol. 30, No. 11, 1996, pp. 3321- 3326. doi:10.1021/es960141u
[29]	J. Boisson, A. Ruttens, M. Mench and J. Vangronsveld, “Evaluation of Hydroxyapatite as a Metal Immobilizing Soil Additive for the Remediation of Polluted Soils. Part 1. Influence of Hydroxyapatite on Metal Exchangeability in Soil, Plant, Growth and Plant Metal Accumulation,” Environmental Pollution, Vol. 104, No. 2, 2005, pp. 225- 233doi:10.1016/S0269-7491(98)00184-5.
[30]	M. Mench, J. Vangronsveld, V. Didier and H. Clijsters, “Evaluation of Metal Mobility, Plant Availability and Immobilization by Chemical Agents in a Limed-Silty Soil,” Environmental Pollution, Vol. 86, No. 3, 1994, pp. 279-286. doi:10.1016/0269-7491(94)90168-6
[31]	R. Mohapatra and J. R. Rao, “Some Aspects of Characterisation, Utilisation and Environmental Effects of Fly Ash (a Review),” Journal of Chemical Technology & Biotechnology, Vol. 76, No. 1, 2001, pp. 9-26. doi:10.1002/1097-4660(200101)76:1<9::AID-JCTB335>3.0.CO;2-5
[32]	C. Fernández-Pereira, Y. L. Galiano, M. A. Rodriguez- Piňero, J. Vale and X. Querol, “Utilisation of Zeolitised Coal Fly Ash as Immobilizing Agent of a Metallurgical Waste,” Journal of Chemical Technology & Biotechnology, Vol. 77, No. 16, 2002, pp. 305-310.doi:10.1002/jctb.584
[33]	M. Polat, E. Lederman, J. Pelly and H. Cohen, “Chemical Neutralization of Acidic Wastes Using Fly Ash in Israel,” Journal of Chemical Technology & Biotechnology, Vol. 77, No. 3, 2002, pp. 377-381. doi:10.1002/jctb.567
[34]	T. Matsi and V. Z. Keramidas, “Fly Ash Application on Two Acid Soils and Its Effect on Soil Salinity, pH, B, P and Ryegrass Growth and Composition,” Environmental Pollution, Vol. 104, No. 1, 1999, pp. 107-112. doi:10.1016/S0269-7491(98)00145-6
[35]	R. Ciccu, M. Ghiani, A, Serci, S. Fadda, R. Peretti and A. Zucca, “Heavy Metal Immobilization in the Mining- Contaminated Soils Using Various Industrial Wastes,” Minerals Engineering, Vol. 16, No. 3, 2003, pp. 187-192.doi:10.1016/S0892-6875(03)00003-7
[36]	X. Querol, A. Alastuey, N. Moreno, E. Alvarez-Ayuso, A. García-Sánchez, J. Cama, C. Ayora and M. Simón, “Immobilization of Heavy Metals in Polluted Soils by the Addition of Zeolitic Material Synthesized from Coal Fly Ash,” Chemosphere, Vol. 62, No. 2, 2006, pp. 171-180. doi:10.1016/j.chemosphere.2005.05.029
[37]	The Perkin-Elmer Corporation, “Analytical Methods for Atomic Absorption Spectrophotometry,” Norwalk Connec- ticut, USA, 1982. doi:10.1016/0010-4485(82)90253-6
[38]	Polish Branch Standard BN-81/0623-01, “Fly Ashes and Slags from Kettles Heated with Hard and Brown Coal,” Polish Committee for Standardization, Varsov, 1982.
[39]	Polish Standard PN-77/G-04528/00, “Solid Fuels. Determi- nation of Chemical Composition of Ash,” Preparation of Ash Sample and Solution for Testing.
[40]	Polish Standard PN-R-04031, “Agrochemical Soil analyses,” Sampling.
[41]	J. Namie?nik, Z. Jamrógiewicz, M. Pilarczyk and L. Torres, “The Preparation of Environmental Samples for Analysis,” Publishing Company of Science and Technology, Varsov, 2000.
[42]	J. Kalembkiewicz and E. Sitarz-Palczak, “Optimization of Mineralization Procedures for the Determination of Mn in Soil Samples,” Atomic Spectroscopy, Vol. 22, No. 6, 2001, pp. 433-437.
[43]	M. J. ??czny, “Non-conventional Method of Utilization of Fly Ash,” Central Mining Institute, Katowice, 2002, pp. 7-19.
[44]	J. Kalembkiewicz, E. Sitarz-Palczak and L. Zapa?a, “A Study of the Chemical Forms or Species of Manganese Found in Coal Fly Ash and Soil,” Microchemical Journal, Vol. 90, No. 1, 2008, pp. 37-43. doi:10.1016/j.microc.2008.03.003
[45]	J. B. Diatta, “Comparison if NH4OAc and NH4-EDTA Differing in Concentration and pH for Cu and Zn Extraction in Soils Contamined by a Cooper Smelter,” Polish Journal of Soil Science, Vol. 31, No. 1, 1998, pp. 25-32.
[46]	Y. B. Ma and N. C. Uren, “Transformations of Heavy Metals Added to Soil—Application of a New Sequential Extraction Procedure,” Geoderma, Vol. 84, No. 1-3, 1998, pp. 157-168. doi:10.1016/S0016-7061(97)00126-2
[47]	M. J. Sánchez-Martin, M. Garcia-Delgado, L. F. Lorenzo, M. S. Rodriguez-Cruz and M. Arienzo, “Heavy Metals in Sewage Sludge Amended Soils Determined by Sequential Extractions as a Function of Incubation Time of Soils,” Geoderma, Vol. 142, No. 3-4, 2007, pp. 262-273. doi:10.1016/j.geoderma.2007.08.012