Abstract
The leaching behaviour of Cu and Zn from contaminated soils at a copper mine was investigated using four extractants: citric acid (CA), oxalic acid (OA), ethylenediaminetetraacetic acid (EDTA) and nitrilotriacetic acid (NTA). Six soil samples were characterized for the distribution of four chemical fractions of Cu or Zn (acid-soluble, reducible, oxidizable and residual). For the extraction of Cu, EDTA is more effective than other extractants when the concentration is less than 0.02 mol/L. The leaching efficiency for Cu was at least 15% higher for EDTA than for the other extractants at the same concentrations. Similar leaching behaviour was observed in the extraction of Zn. After extraction by CA, OA, EDTA or NTA, the acid-soluble fractions and the reducible fractions of Cu were the main fractions extracted. The potential environmental risks related to speciation were evaluated, and after extraction these risks were reduced.
摘要
以铜矿受污染土壤为对象,研究柠檬酸(CA)、草酸(OA)、乙二胺四乙酸(EDTA)、氨三乙 酸(NTA)四种提取剂对铜和锌的浸提效果。分析六种土壤样品中酸溶态、还原态、氧化态、残渣态 形式存在铜和锌的占比。研究结果表明:当提取剂的溶度小于 0.02 mol/L 时,相较于其他三种提取剂, EDTA 对于铜的提取效果最好,在相同提取剂浓度下,EDTA 比其他提取剂的提取效率至少高15%。 当提取剂的溶度小于 0.02 mol/L 时,EDTA 对锌的提取效果最好。分别测定四种提取剂提取前、后铜 的化学赋存形态,发现以酸溶态和还原态形式存在的铜被大量提取,含量显著减少。评估环境风险发 现,提取之后环境风险显著下降。
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References
GUO Yao, HUANG Peng, ZHANG Wu, YUAN Xue, FAN Feng, WANG Huan, LIU Jian, WANG Zhao. Leaching of heavy metals from Dexing copper mine tailings pond [J]. Transactions of Nonferrous Metals Society of China, 2013, 23(10): 3068–3075.
HANSEN H K, YIANATOS J B, OTTOSEN L M. Speciation and leachability of copper in mine tailings from porphyry copper mining: Influence of particle size [J]. Chemosphere, 2005, 60(10): 1497–1503.
DERMONT G, BERGERON M, MERCIER G, RICHERLAFLECHE M. Metal-contaminated soils: Remediation practices and treatment technologies [J]. Practice Periodical of Hazardous, Toxic, and Radioactive Waste Management, 2008, 12(3): 188–209.
MULLIGAN C N, YONG R N, GIBBS B F. Remediation technologies for metal-contaminated soils and groundwater: An evaluation [J]. Engineering Geology, 2001, 60(1–4): 193–207.
PETERS R W. Chelate extraction of heavy metals from contaminated soils [J]. Journal of Hazardous Materials, 1999, 66(1, 2): 151–210.
WU L H, LUO Y M, CHRISTIE P, WONG M H. Effects of EDTA and low molecular weight organic acids on soil solution properties of a heavy metal polluted soil [J]. Chemosphere, 2003, 50(6): 819–822.
QIN Fei, SHAN Xiao, WEI Bei. Effects of low-molecular-weight organic acids and residence time on desorption of Cu, Cd, and Pb from soils [J]. Chemosphere, 2004, 57(4): 253–263.
YUAN Song, XI Zhi, JIANG Yi, WAN Jin, WU Chan, ZHENG Zhong, LU Xiao. Desorption of copper and cadmium from soils enhanced by organic acids [J]. Chemosphere, 2007, 68(7): 1–9.
LI Li, HOLM P E, MARCUSSEN H, BRUUN H C. Release of cadmium, copper and lead from urban soils of Copenhagen [J]. Environmental Pollution, 2014, 187: 90–97.
GAO Yan, HE Ji, LING Wan, HU Hong, LIU Fan. Effects of organic acids on copper and cadmium desorption from contaminated soils [J]. Environment International, 2003, 29(5): 613–618.
JIANG Hong, LI Ting, HAN Xuan, YANG Xiao, HE Zhen. Effects of pH and low molecular weight organic acids on competitive adsorption and desorption of cadmium and lead in paddy soils [J]. Environmental Monitoring and Assessment, 2012, 184(10): 6325–6335.
MADRID F, REINOSO R, FLORIDO M C, DIAZBARRIENTOS E, AJMONE-MARSEN F, DAVIDSON C M, MADRID L. Estimating the extractability of potentially toxic metals in urban soils: A comparison of several extracting solutions [J]. Environmental Pollution, 2007, 147(3): 713–722.
CHEN Su, HU Guan. A preliminary discussion on the analysis methods for inorganic elements used in the national investigation program of soil pollution [J]. Environ Monit China, 2007, 23(5): 6–10. (in Chinese)
LU R K. Analytical methods for soils and agricultural chemistry [M]. Beijing: China Agricultural Science and Technology Press, 1999. (in Chinese)
TANDY S, BOSSART K, MUELLER R, RITSCHEL J, HAUSER L, SCHULIN R, NOWACK B. Extraction of heavy metals from soils using biodegradable chelating agents [J]. Environmental Science & Technology, 2004, 38(3): 937–944.
ZHAI Yu, THOMASSON J A, BOGGESS III J E, SUI Rui. Soil texture classification with artificial neural networks operating on remote sensing data [J]. Computers and Electronics in Agriculture, 2006, 54(2): 53–68.
DERMONT G, BERGERON M, MERCIER G, RICHERLAFLECHE M. Soil washing for metal removal: A review of physical/chemical technologies and field applications [J]. Journal of Hazardous Materials, 2008, 152(1): 1–31.
CUONG D T, OBBARD J P. Metal speciation in coastal marine sediments from Singapore using a modified BCRsequential extraction procedure [J]. Applied Geochemistry, 2006, 21(8): 1335–1346.
ARENAS-LAGO D, ANDRADE M L, LAGO-VILO M, RODRIGUEZ-SEIJO A, VEGA F A. Sequential extraction of heavy metals in soils from a copper mine: Distribution in geochemical fractions [J]. Geoderma, 2014, 230–231: 108–118.
YANG J S, LEE J Y, BAEK K, KWON T S, CHOI J. Extraction behavior of As, Pb, and Zn from mine tailings with acid and base solutions [J]. Journal of Hazardous Materials, 2009, 171(1–3): 443–451.
REMIREZ M, MASSOLO S, FRACHE R, CORREA J A. Metal speciation and environmental impact on sandy beaches due to El Salvador copper mine, Chile [J]. Marine Pollution Bulletin, 2005, 50(1): 62–72.
RODRIGUEZ L, RUIZ E, ALONSO-AZCARATE J, RINCON J. Heavy metal distribution and chemical speciation in tailings and soils around a Pb–Zn mine in Spain [J]. J Environ Manage, 2009, 90(2): 1106–1116.
ZALECKAS E, PAULAUSKAS V, SENDZIKIENE E. Fractionation of heavy metals in sewage sludge and their removal using low-molecular-weight organic acids [J]. Journal of Environmental Management, 2013, 21(3): 189–198.
BURT R, WILON M A, KECK T J, DOUGHERTY B D, STROM D E, LINDAHL J A. Trace element speciation in selected smelter-contaminated soils in Anaconda and Deer Lodge Valley Montana, USA [J]. Advances in Environmental Research, 2003, 8(1): 51–67.
GIANNIS A, NIKOLAOU A, PENTARI D, GIDARAKOS E. Chelating agent-assisted electrokinetic removal of cadmium, lead and copper from contaminated soils [J]. Environmental Pollution, 2009, 157(12): 3379–3386.
KRISHNAMURTI G S R, CIESLINSKI G, HUANG P M, VAN-REES K C J. Kinetics of cadmium release from soils as influenced by organic acids: Implication in cadmium availability [J]. Journal of Environmental Quality, 1997, 26(1): 271–277.
CHAIRIDCHAI P, RITCHIE G S P. Zinc adsorption by a lateritic soil in the presence of organic ligands [J]. Soil Science Society of America Journal, 1990, 54(5): 1242–1248.
XIA Wen, LI Xin, GAO Hui, HUANG Bao, ZHANG Hui, LIU Yun, ZENG Guang, FAN Ting. Influence factors analysis of removing heavy metals from multiple metal-contaminated soils with different extractants [J]. Journal of Central South University of Technology, 2009, 16(1): 108–111.
PETERS R W. Feasibility treatability studies for removal of heavy metals from training range soils at the Grafenwoehr training area, Germany [M]. Argonne, IL: ANL/ESD/TM-81, Argonne National Laboratory, 1995
VEGA F A, COVELO E F, ANDRADE M L. Competitive sorption and desorption of heavy metals in mine soils: Influence of mine soil characteristics [J]. Journal of Colloid and Interface Science, 2006, 298(2): 582–592.
CHENG Zhong, LEE L, DAYAN S, GRINSHTEIN M, SHAW R. Speciation of heavy metals in garden soils: evidences from selective and sequential chemical leaching [J]. Journal of Soils and Sediments, 2011, 11(4): 628–638.
PEREZ-ESTEBAN J, ESCOLASTICO C, MOLINER A, MASAGUER A. Chemical speciation and mobilization of copper and zinc in naturally contaminated mine soils with citric and tartaric acids [J]. Chemosphere, 2013, 90(2): 276–283.
SHAN Xiao, LIAN Jun, WEN Bei. Effect of organic acids on adsorption and desorption of rare earth elements [J]. Chemosphere, 2002, 47(7): 701–710.
BACON J R, DAVIDSON C M. Is there a future for sequential chemical extraction? [J]. Analyst, 2008, 133(1): 25–46.
SINGH K P, MOHAN D, SINGH V K, MALIK A. Studies on distribution and fractionation of heavy metals in Gomti river sediments-a tributary of the Ganges, India [J]. Journal of Hydrology, 2005, 312(1): 14–27.
YOO J C, LEE C D, YANG J S, BAEK K. Extraction characteristics of heavy metals from marine sediments [J]. Chemical Engineering Journal, 2013, 228(28): 688–699.
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The authors would like to thank Dr. Nicholas Ward and Dr. Nadia Toppler of Southern Cross University for their editing assistance.
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Foundation item: Project(2232013A3-08) supported by the Fundamental Research Funds for the Central Universities, China; Project supported by Shanghai Pujiang Program and DHU Distinguished Young Professor Program, China
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Xiao, Jh., Zhou, J., Wang, Zh. et al. Extraction of copper and zinc from naturally contaminated copper mine soils: Chemical fractionation analysis and risk assessment. J. Cent. South Univ. 25, 1274–1284 (2018). https://doi.org/10.1007/s11771-018-3824-6
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DOI: https://doi.org/10.1007/s11771-018-3824-6