Long-Term Release of Iron-Cyanide Complexes from the Soils of a Manufactured Gas Plant Site

Abstract

Iron-cyanide (Fe-CN) complexes have been detected at Manufactured Gas Plant sites (MGP) worldwide. The risk of groundwater contamination depends mainly on the dissolution of ferric ferrocyanide. In order to design effective remediation strategies, it is relevant to understand the contaminant’s fate and transport in soil, and to quantify and mathematically model a release rate. The release of iron-cyanide complexes from four contaminated soils, originating from the former MGP in Cottbus, has been studied by using a column experiment. Results indicated that long-term cyanide (CN) release is governed by two phases: one readily dissolved and one strongly fixed. Different isotherm and kinetic equations were used to investigate the driving mechanisms for the ferric ferrocyanide release. Applying the isotherm equations assumed an approach by which two phases were separate in time, whereas the multiple first order equation considered simultaneous occurrence of both cyanide pools. Results indicated varying CN release rates according to the phase and soil. According to isotherm and kinetic models, the long-term iron cyanide release from the MGP soils is a complex phenomenon driven by various mechanisms parallely involving desorption, diffusion and transport processes. Phase I (rapid release) is presumably mainly constrained by the transport process of readily dissolved iron-cyanide complexes combined with desorption of CN bound to reactive heterogeneous surfaces that are in direct contact with the aqueous phase (outer-sphere complexation). Phase II (limited rate) is presumably driven by the diffusion controlled processes involving dissolution of precipitated ferric ferrocyanide from the mineral or inner-sphere complexation of ferricyanides. CN release rates in phase I and II were mainly influenced by the pH, organic matter (OM) and the total CN content. The cyanide release rates increased with increasing pH, decreased with low initial CN concentration and were retarded by the increase in OM content.

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M. Sut, T. Fischer, F. Repmann and T. Raab, "Long-Term Release of Iron-Cyanide Complexes from the Soils of a Manufactured Gas Plant Site," Journal of Environmental Protection, Vol. 4 No. 11B, 2013, pp. 8-19. doi: 10.4236/jep.2013.411B002.

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1] P. Kjeldsen, “Behavior of Cyanides in Soil and Groundwater: A Review,” Water, Air & Soil Pollution, Vol. 115, No. 1-4, 1998, pp. 279-307.
http://dx.doi.org/10.1023/A:1005145324157
[2] C. M. Saffron, J. H. Park, B. E. Dale and T. C. Voice, “Kinetics of Contaminant Desorption Form Soil: Comparison of Model Formulations Using the Akaika Information Criterion,” Environmental Science Technology, Vol. 40, 2006, pp. 7662-7667.
http://dx.doi.org/10.1021/es0603610
[3] T. Rennert and T. Mansfeldt, “Sorption of Iron-Cyanide Complexes in Soil,” Soils Science Society of American Journal, Vol. 66, No. 2, 2002, pp. 437-444.
http://dx.doi.org/10.2136/sssaj2002.0437
[4] T. Mansfeldt, “Mobilitat und Mobilisierbarkeit von Eisenkomplexierten Cyaniden. Materialien zur Altlastensanierung und zum Bodenschutz (MALBO),” Landesumweltamt Nordrhein-Westfalen (LUA NRW), Vol. 16, 2003, pp. 17-44.
[5] W. H. Fuller, “Cyanides in the Environment with Particular Attention to the Soil,” In: D. Van Zyl, Ed., Cyanide and the Environment, Colorado State University, Fort Collins, 1985, pp. 19-44.
[6] T. Ohno, “Levels of Total Cyanide and NaCl in Surface Waters Adjacent to Road Salt Storage Facilities,” Environmental Pollution, Vol. 67, No. 2, 1990, pp. 123-132.
http://dx.doi.org/10.1016/0269-7491(90)90077-P
[7] T. Rennert and T. Mansfeldt, “Sorption of Iron-Cyanide Complexes on Goethite,” European Journal of Soil Science, Vol. 52, No. 1, 2001, pp. 121-128.
http://dx.doi.org/10.1046/j.1365-2389.2001.t01-1-00368.x
[8] W. P. Cheng and C. Huang, “Adsorption Characteristics of Iron-Cyanide Complex on γ-Al2O3,” Journal of Colloid Interface Science, Vol. 181, No. 2, 1996, pp. 627-637.
http://dx.doi.org/10.1006/jcis.1996.0420
[9] R. S. Ghosh, D. A. Dzombak, R. G. Luthy and D. V. Nakles, “Subsurface Fate and Transport of Cyanide Species at a Manufactured Gas Plant Site,” Water Environment Research, Vol. 71, No. 6, 1999, pp. 1205-1216.
http://dx.doi.org/10.2175/106143096X122474
[10] M. Linder, H. Bugmann, P. Lasch, M. Fleschig and W. Cramer, “Regional Impacts of Climatic Change on Forests in the State of Brandenburg, Germany,” Agricultural and Forest Meteorology, Vol. 84, No. 1-2, 1997, pp. 123-135.
http://dx.doi.org/10.1016/S0168-1923(96)02381-7
[11] M. C. Peel, B. L. Finlayson and T. A. McMahon, “Updated World Map of the Koppen Geiger Climate Classification,” Hydrology and Earth System Sciences, Vol. 11, 2007, pp. 1633-1644.
http://dx.doi.org/10.5194/hess-11-1633-2007
[12] M. Sut, T. Fischer, F. Repmann, T. Raab and T. Dimitrova, “Feasibility of Field Portable Near Infrared (NIR) Spectroscopy to Determine Cyanide Concentrations in Soil,” Water, Air & Soil Pollution, Vol. 223, No. 8, 2012, pp. 5495-5504.
http://dx.doi.org/10.1007/s11270-012-1298-y
[13] H. W. Müller, R. Dohrmann, D. Klosa, S. Rehder and W. Eckelmann, “Comparison of Two Procedures for Particle-Size Analysis: Kohn Pipette and X-Ray Granulometry,” Journal of Plant Nutrition and Soil science, Vol. 172, No. 2, 2009, pp. 172-179.
http://dx.doi.org/10.1002/jpln.200800065
[14] M. Sut, T. Fischer, F. Repmann and T. Raab, “Stability of Prussian Blue in Soils of a Former Manufactured Gas Plant Site,” Soil and Sediments Contamination an International Journal.
http://dx.doi.org/10.1080/15320383.2014.839626
[15] USEPA, “Method 10-204-00-1-X, Lachat US EPA Approved and Equivalent Method,” Revision 3, 2008.
[16] DIN EN ISO 14 403, “Bestimmung von Gesamt Cyanid und Freiem Cyanid mit Derkontinuerlichen Fließanalytik-Teil D,” 2002.
[17] S. H. Chien, W. R. Clayton and G. H. McClellan, “Kinetics of Dissolution of Phosphate Rocks in Soil,” Soils Science Society of American Journal, Vol. 44, No. 2, 1980, pp. 260-264.
http://dx.doi.org/10.2136/sssaj1980.03615995004400020012x
[18] R. J. Atkinson, F. J. Hingston, A. M. Posner and J. P. Quirk, “Elovich Equation for the Kinetics of Isotope Exchange Reaction at Soild-Liquid Interfaces,” Nature, Vol. 226, 1970, pp. 148-149.
http://dx.doi.org/10.1038/226148a0
[19] S. H. Chien and W. R. Clayton, “Application of Elovich Equation to the Kinetics of Phosphate Release and Sorption in Soils,” Soils Science Society of American Journal, Vol. 44, No. 2, 1980, pp. 265-268.
http://dx.doi.org/10.2136/sssaj1980.03615995004400020013x
[20] J. Torrent, “Rapid and Slow Phosphate Sorption by Mediterranean Soils. Effect of Iron Oxides,” Soils Science Society of American Journal, Vol. 51, 1987, pp. 78-82.
[21] K. J. Laidler, “Chemical Kinetics,” McGraw-Hill, New York, 1965.
[22] P. M. Jardine and D. L. Sparks, “Potassium-Calcium Exchange in Multireactive Soil System. I. Kinetics,” Soils Science Society of American Journal, Vol. 48, No. 1, 1984, pp. 39-45.
http://dx.doi.org/10.2136/sssaj1984.03615995004800010007x
[23] C. Aharoni, D. L. Sparks, S. Levinson and I. Ravina, “Kinetics of Soil Chemical Reactions: Relationships between Empirical Equations and Diffusion Models,” Soils Science Society of American Journal, Vol. 55, 1991, pp. 1307-1312.
http://dx.doi.org/10.2136/sssaj1991.03615995005500050019x
[24] E. A. Elkhatib, G. M. ElShebiny and A. M. Balba, “Comparison of Four Equations to Describe the Kinetics of Lead Desorption from Soils,” Zeitschrift für Pflanzenernahrung und Bodenkunde, Vol. 155, 1992, pp. 285-291.
http://dx.doi.org/10.1002/jpln.19921550408
[25] E. A. Elkhatib, A. M. Mahdy, M. E. Saleh and N. H. Barakat, “Kinetics of Copper Desorption from Soils as Affected by Different Organic Ligands,” International Journal of Envirnomental Science Technology, Vol. 4, No. 3, 2007, pp. 331-338.
[26] M. M. Nederlof, W. H. Van Riemsdijk and L. K. Koopal, “Analysis of the Rate of Dissociation of Ligand Complexes,” Environmental Science and Technology, Vol. 28, 1994, pp. 1048-1053.
http://dx.doi.org/10.1021/es00055a013
[27] S. E. A. T. M. Van der Zee and W. H. Van Riemsdijk, “Model for Long-Term Phosphate Reaction Kinetics in Soil,” Journal of Environmental Quality, Vol. 17, No. 1, 1998, pp. 35-41.
http://dx.doi.org/10.2134/jeq1988.00472425001700010005x
[28] Bodenkundliche Kartieranleitung, AG Boden, 5. Aufl., 438 S., 41 Abb., 103 Tab., 31 Listen, Hannover, 2005.
[29] F. J. Hingston, A. M. Posner and J. P. Quirk, “Anion Adsorption by Goethite and Gibbsite. II. Desorption of Anions from Hydrous Oxide Surfaces,” Journal of Soil Sciences, Vol. 25, No. 1, 1974, pp. 16-26.
http://dx.doi.org/10.1111/j.1365-2389.1974.tb01098.x
[30] M. J. D. Low, “Kinetics of Chemisorption of Gases on Solids,” Chemical Reviews, Vol. 60, No. 3, 1960, pp. 267-312. http://dx.doi.org/10.1021/cr60205a003
[31] R. J. Umpleby II, S. C. Baxter, M. Bode, J. K. Berch Jr., R. N. Shah and K. D. Shimizu, “Application of the Freundlich Adsorption Isotherm in the Characterization of Molecularly Imprinted Polymers,” Analitica Chimica Acta, Vol. 435, No. 1, 2001, pp. 35-42.
http://dx.doi.org/10.1016/S0003-2670(00)01211-3
[32] J. L. Meeussen, M. G. Keizer, W. H. Van Riemsdijk and F. A. M. de Haan, “Dissolution Behavior of Iron Cyanide (Prussian Blue) in Contaminated Soils,” Environmental Science & Technology, Vol. 26, No. 9, 1992, pp. 1832-1838. http://dx.doi.org/10.1021/es00033a019
[33] T. L. Theis and M. L. West, “Effects of Cyanide Complexation on the Adsorption of Trace Metals at the Surface of Goethite,” Environmental Technology Letters, Vol. 7, No. 1-12, 1986, pp. 309-318.
http://dx.doi.org/10.1080/09593338609384417
[34] T. Mansfeldt and R. Dohrmann, “Identification of a Crystalline Cyanide-Containing Compound in Blast Furnace Sludge Deposits,” Journal of Environmental Quality, Vol. 30, No. 6, 2001, pp. 1927-1932.
http://dx.doi.org/10.2134/jeq2001.1927
[35] T. Rennert and T. Mansfeldt, “Sorption of Iron-Cyanide Complexes on Goethite in the Presence of Sulfate and Desorption with Phosphate and Chloride,” Journal of Environmental Quality, Vol. 31, No. 3, 2002, pp. 745-751.
http://dx.doi.org/10.2134/jeq2002.0745
[36] F. C. Wu, R. L. Tseng and R. S. Juang, “Characteristics of Elovich Equation Used for the Analysis of Adsorption Kinetics in Dye-Chitosan Systems,” Chemical Engineering Journal, Vol. 150, 2009, pp. 366-373.
http://dx.doi.org/10.1016/j.cej.2009.01.014
[37] B. Schenk and B. M. Wilke, “Cyanidadsorption an Sesquioxiden, Tonmineralen und Huminstoffen,” Zeitschrift für Pflanzenernahrung und Bodenkunde, Vol. 147, No. 6, 1984, pp. 669-679.
http://dx.doi.org/10.1002/jpln.19841470604
[38] R. L. Evans and J. J. Jurinak, “Kinetics of Phosphate Release from a Desert Soil,” Soil Science, Vol. 121, No. 4, 1976, pp. 205-211.
http://dx.doi.org/10.1097/00010694-197604000-00003
[39] D. Freese, “Criteria and Methods for the Assessment of Long-Term Phosphate Sorption and Desorption in Soils,” Habilitationsschrift, Landwirtschaftlich-Gartnerischen Fakultat, Humboldt-Universitat zu Berlin, 1994.
[40] J. C. Meeussen, G. Meindert, W. H. Van Riemsdijk and F. A. M. de Haan, “Solubility of Cyanide in Contaminated Soils,” Journal of Environmental Quality, Vol. 23, No. 4, 1994, pp. 785-787.
http://dx.doi.org/10.2134/jeq1994.00472425002300040024x

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