淋洗对农田土壤镉铅锌的去除、移动性和有效性的影响
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摘要
以福建省Cd-Pb-Zn矿区周边的农田污染土壤为材料,通过室内连续振荡淋洗和ICP-MS测定,研究了4种常用的淋洗剂(柠檬酸、EDTA、FeCl_3和HCl)一次和连续5次淋洗对土壤Cd、Pb和Zn的去除效果,及对其形态、移动性和有效性的影响。结果表明,与一次淋洗相比,连续5次淋洗能够增加这4种淋洗剂对Cd、Pb和Zn的去除效果,FeCl_3、EDTA和柠檬酸分别对Cd、Pb和Zn的去除效果最好,5次淋洗后分别达到89. 29%、24. 95%和36. 72%。BCR形态分析结果表明,4种淋洗剂对土壤Cd和Zn的淋洗主要是通过对弱酸提取和可还原态的Cd和Zn去除而实现的;对于土壤Pb的淋洗主要是对可还原态Pb的去除;对可氧化态和残余态重金属影响不大。其次,淋洗可导致土壤Cd、Pb和Zn移动性和有效性的增加,从而会增加其生态环境风险而导致淋洗效果的丧失,在评价淋洗效果时应予以关注。最后,从淋洗前后土壤重金属有效态变化角度考虑,对Cd-Pb-Zn复合污染土壤,EDTA是较好的淋洗剂选择。
The paper is inclined to make an investigation and examination of the effets of the soil washing on the heavy metals( Cd,Pb and Zn) removal from the Cd-Pb-Zn contaminated farmlands nearby a Pb-Zn mining area in Fujian Province. For the research purpose,we have chosen 4 commonly used reagents as washing extractants,that is,the citric acid( CA),the ethylenediaminetetraacetic acid( EDTA), the hydrochloride acid( HCl) and the ferric chloride( FeCl_3). To make our study more purposeful and effective,we have managed to conduct 5 successive rounds of laboratory washing of Cd,Pb and Zn contaminants by oscillating washing for the effectiveness of single round,and managed to account and measure the contents of Cd,Pb and Zn in the leacheate by the inductively coupled plasma mass spectrometry( ICP-MS). The European Community Bureau of Reference( BCR) sequential extraction was used to assess the redistribution of Cd,Pb and Zn between the fractions before and after washing. Additionally,changes of soil Cd,Pb and Zn mobility and availability( DTPA-extracted) were also assessed. The results of our experimental study proved that the 5 successive washing rounds has successfully removed more metal contaminants than those of the single round washing. The best removal efficiency with FeCl_3,EDTA and citric acid from the contaminatedsoil could reach 89. 29% of Cd,24. 95% of Pb and 36. 27% of Zn through a series of 5 successive washing rounds,respectively.The results of BCR sequential extraction demonstrated that the Cd and Zn removal with the 4 commonly used washing extractants tend to remove mainly from exchangeable/acid extractable( F1)and easily reducible fraction( F2), respectively. However,Lead( Pb) has been mainly removed form the easily reducible fractions,though no significant impact has been detected on the oxidizable( F3) and residual fraction( F4) of Cd,Pb and Zn as a result of the soil washing. Moreover,the results also verified that the soil washing could lead to the increase of Cd,Pb and Zn mobility and availability in the soil so as to aggrevate their ecoenvironmental risk and the loss of washing effects. Therefore,greater attention has to be paid to the evaluation of the washing effects. And,finally,from the point of view of availability,it is recommanded to take EDTA as the alternative of the washing extractant for the Cd-Pb-Zn contaminated farm land soil.
The paper is inclined to make an investigation and examination of the effets of the soil washing on the heavy metals( Cd,Pb and Zn) removal from the Cd-Pb-Zn contaminated farmlands nearby a Pb-Zn mining area in Fujian Province. For the research purpose,we have chosen 4 commonly used reagents as washing extractants,that is,the citric acid( CA),the ethylenediaminetetraacetic acid( EDTA), the hydrochloride acid( HCl) and the ferric chloride( FeCl_3). To make our study more purposeful and effective,we have managed to conduct 5 successive rounds of laboratory washing of Cd,Pb and Zn contaminants by oscillating washing for the effectiveness of single round,and managed to account and measure the contents of Cd,Pb and Zn in the leacheate by the inductively coupled plasma mass spectrometry( ICP-MS). The European Community Bureau of Reference( BCR) sequential extraction was used to assess the redistribution of Cd,Pb and Zn between the fractions before and after washing. Additionally,changes of soil Cd,Pb and Zn mobility and availability( DTPA-extracted) were also assessed. The results of our experimental study proved that the 5 successive washing rounds has successfully removed more metal contaminants than those of the single round washing. The best removal efficiency with FeCl_3,EDTA and citric acid from the contaminatedsoil could reach 89. 29% of Cd,24. 95% of Pb and 36. 27% of Zn through a series of 5 successive washing rounds,respectively.The results of BCR sequential extraction demonstrated that the Cd and Zn removal with the 4 commonly used washing extractants tend to remove mainly from exchangeable/acid extractable( F1)and easily reducible fraction( F2), respectively. However,Lead( Pb) has been mainly removed form the easily reducible fractions,though no significant impact has been detected on the oxidizable( F3) and residual fraction( F4) of Cd,Pb and Zn as a result of the soil washing. Moreover,the results also verified that the soil washing could lead to the increase of Cd,Pb and Zn mobility and availability in the soil so as to aggrevate their ecoenvironmental risk and the loss of washing effects. Therefore,greater attention has to be paid to the evaluation of the washing effects. And,finally,from the point of view of availability,it is recommanded to take EDTA as the alternative of the washing extractant for the Cd-Pb-Zn contaminated farm land soil.
引文
[1] BOLAN N,KUNHIKRISHNAN A,THANGARAJAN R,et al. Remediation of heavy metal(loid)s contaminated soils-to mobilize or to immobilize?[J]. Journal of Hazardous Materials,2014,266:141-166.
[2] GUMTZ G D. Restoration of beaches contaminated by oil,EPA-R2-72-045[R]. U. S. Environmental Protection Agency,1972.
[3] LI Y J,HU P J,ZHAO J,et al. Remediation of cadmium-and lead-contaminated agriculture soil by composite washing with chloride and citric acid[J]. Environmental Science and Pollution Research, 2015, 22(7):5563-5571.
[4] VOGLAR D,LESTAN D. Chelant soil-washing technology for metal contaminated soil[J]. Environmental Technology,2014,35(11):1389-1400.
[5] TAO Huchun(陶虎春),DING Wenyi(丁文毅),LI Jinbo(李金波). Ways for remediation to Pb and Zn contaminated soil via washing-out effluent combined oxalic acid with Fe Cl3[J]. Journal of Safety and Environment(安全与环境学报),2017,17(5):1937-1942.
[6] ZHAI X,LI Z,HUANG B,et al. Remediation of multiple heavy metal-contaminated soil through the combination of soil washing and in situ immobilization[J]. Science of the Total Environment,2018,635:92-99.
[7] UDOVIC M,LESTAN D. Pb,Zn and Cd mobility,availability and fractionation in aged soil remediated by EDTA leaching[J]. Chemosphere,2009,74(10):1367-1373.
[8] ZENG Min(曾敏),LIAO Bohan(廖柏寒),ZENG Qingru(曾清如),et al. Effects of three extractants on removal and availabilities of heavy metals in the contaminated soil[J]. Journal of Agro-Environment Science(农业环境科学学报),2006,25(4):979-982.
[9] GUO X,WEI Z,PENN C J,et al. Effect of soil washing and liming on bioavailability of heavy metals in acid contaminated soil[J]. Soil Science Society of America Journal,2011,77(2):432-441.
[10] OH S,BADE R,LEE H,et al. Risk assessment of metal(loid)-contaminated soils before and after soil washing[J]. Environmental Earth Science,2015,74(1):703-713.
[11] LEE S,KIM J,LEE J,et al. Removal of arsenic in tailings by soil flushing and the remediation process monitoring[J]. Environmental Geochemistry and Health,2004,26(3/4):403-409.
[12] GB/T 1739—1997 Soil quality—determination of lead,cadmium—graphite furnace atomic absorption spectrophotometry(土壤质量—铅镉的测定—石墨炉原子吸收分光光度法)[S].
[13] LU Rukun(鲁如坤). Analysis method of soil agricultural chemistry(土壤农化分析)[M]. Beijing:Chinese Agricultural Science and Technology Press,2000.
[14] GB 15618—2018 Soil environmental quality—risk control standard for soil contamination of agricultural land(土壤环境质量农用地土壤污染风险管控标准)[S].
[15] RAURET G,LPEZ-SANCHEZ J F,SAHUQUILLO A,et al. Application of a modified BCR sequential extraction(three-step)procedure for the determination of extractable trace metal contents in a sewage sludge amended soil reference material(CRM 483),complemented by a three-year stability study of acetic acid and EDTA extractable metal content[J]. Journal of Environmental Monitoring,2000,2(3):228-233.
[16] NY/T 890—2004 Determination of available zinc,manganese,iron and copper in soil—extraction with buffered DTPA solution(土壤有效态锌、锰、铁、铜含量的测定—二乙三胺五乙酸(DTPA)浸提法)[S].
[17] GUSIATIN Z M,KLIMIUK E. Metal(Cu,Cd and Zn)removal and stabilization during multiple soil washing by saponin[J]. Chemosphere,2012,86(4):383-391.
[18] YE Tao(叶涛),HUANG Li(黄丽),ZHANG Keqiang(张克强),et al. Evaluation of the combined removal of heavy metals by saponin and citric acid from municipal sewage sludges and metal stability features[J]. Environmental Science(环境科学), 2017, 38(11):4850-4859.
[19] SUN B,ZHAO F J,LOMBI E,et al. Leaching of heavy metals from contaminated soils using EDTA[J]. Environmental Pollution,2001,113(2):111-120.
[20] POLETTINI A,POMI R,ROLLE E. The effect of operating variables on chelant-assisted remediation of contaminated dredged sediment[J]. Chemosphere,2007,66(5):866-877.
[21] PETERS R W. Chelant extraction of heavy metals from contaminated soils[J]. Journal of Hazardous Materials,1999,66(1/2):151-210.
[22] DERMONT G,BERGERON M,MERCIER G,et al.Soil washing for metal removal:a review of physic/chemical technologies and field applications[J]. Journal of Hazardous Materials,2008,152(1):1-31.
[23] NOWACK B,SIGG L. Adsorption of EDTA and metalEDTA complexes onto goethite[J]. Journal of Colloid&Interface Science,1996,177(1):106-121.
[24] TSANG D C W,ZHANG W,LO I M C. Copper extraction effectiveness and soil dissolution issue of EDTAflushing of artificially contaminated soils[J]. Chemosphere,2007,68(2):234-243.
[25] TSANG D C W,HARTLEY N R. Metal distribution and spectroscopic analysis after soil washing with chelating agents and humic substances[J]. Environmental Science and Pollution Research,2014,21(5):3987-3995.
[26] LELEYTER L,ROUSSEAU C,BIREE L,et al. Comparison of EDTA,HCl and sequential extraction procedures,for selected metals(Cu,Mn,Pb,Zn),in soils,riverine and marine sediments[J]. Journal of Geochemical Exploration,2012,116/117:51-59.
[27] JEAN-SORO L,BORDAS F,BOLLINGER J C. Column leaching of chromium and nickel from a contaminated soil using EDTA and citric acid[J]. Environmental Pollution,2012,164:175-181.
[28] UDOVIC M,LESTAN D. EDTA and HCl leaching of calcareous and acidic soils polluted with potentially toxic metals:remediation efficiency and soil impact[J].Chemosphere,2012,88(6):718-724.
[29] MAKINO T,TAKANO H,KAMIYA T,et al. Restoration of cadmium-contaminated paddy soils by washing with ferric chloride:Cd extraction mechanism and bench-scale verification[J]. Chemosphere,2008,70(6):1035-1043.
[30] CHEN C,CHEN Y,XIE T,et al. Removal,redistribution,and potential risks of soil Cd,Pb,and Zn after washing with various extractants[J]. Environmental Science and Pollution Research, 2015, 22(21):16881-16888.
[31] SEO B H,KIM H S,KWON S I,et al. Heavy metal accumulation and mobility in a soil profile depend on the organic waste type applied[J]. Journal of Soils and Sediments,2019,19(2):822-829.
[32] YU M,ZHANG J,TIAN Y. Change of heavy metal speciation, mobility, bioavailability, and ecological risk during potassium ferrate treatment of waste-activated sludge[J]. Environmental Science and Pollution Research,2018,25(14):1-10.
[33] HONG K J,TOKUNAGA S,KAJIUCHI T. Evaluation of remediation process with plant-derived biosurfactant for recovery of heavy metals from contaminated soils[J].Chemosphere,2002,49(4):379-387.
[34] KUMPIENE J,LAGERKVIST A,MAURICE C. Stabilization of As,Cr,Cu,Pb and Zn in soil using amendments-a review[J]. Waste Management,2008,28(1):215-225.
[2] GUMTZ G D. Restoration of beaches contaminated by oil,EPA-R2-72-045[R]. U. S. Environmental Protection Agency,1972.
[3] LI Y J,HU P J,ZHAO J,et al. Remediation of cadmium-and lead-contaminated agriculture soil by composite washing with chloride and citric acid[J]. Environmental Science and Pollution Research, 2015, 22(7):5563-5571.
[4] VOGLAR D,LESTAN D. Chelant soil-washing technology for metal contaminated soil[J]. Environmental Technology,2014,35(11):1389-1400.
[5] TAO Huchun(陶虎春),DING Wenyi(丁文毅),LI Jinbo(李金波). Ways for remediation to Pb and Zn contaminated soil via washing-out effluent combined oxalic acid with Fe Cl3[J]. Journal of Safety and Environment(安全与环境学报),2017,17(5):1937-1942.
[6] ZHAI X,LI Z,HUANG B,et al. Remediation of multiple heavy metal-contaminated soil through the combination of soil washing and in situ immobilization[J]. Science of the Total Environment,2018,635:92-99.
[7] UDOVIC M,LESTAN D. Pb,Zn and Cd mobility,availability and fractionation in aged soil remediated by EDTA leaching[J]. Chemosphere,2009,74(10):1367-1373.
[8] ZENG Min(曾敏),LIAO Bohan(廖柏寒),ZENG Qingru(曾清如),et al. Effects of three extractants on removal and availabilities of heavy metals in the contaminated soil[J]. Journal of Agro-Environment Science(农业环境科学学报),2006,25(4):979-982.
[9] GUO X,WEI Z,PENN C J,et al. Effect of soil washing and liming on bioavailability of heavy metals in acid contaminated soil[J]. Soil Science Society of America Journal,2011,77(2):432-441.
[10] OH S,BADE R,LEE H,et al. Risk assessment of metal(loid)-contaminated soils before and after soil washing[J]. Environmental Earth Science,2015,74(1):703-713.
[11] LEE S,KIM J,LEE J,et al. Removal of arsenic in tailings by soil flushing and the remediation process monitoring[J]. Environmental Geochemistry and Health,2004,26(3/4):403-409.
[12] GB/T 1739—1997 Soil quality—determination of lead,cadmium—graphite furnace atomic absorption spectrophotometry(土壤质量—铅镉的测定—石墨炉原子吸收分光光度法)[S].
[13] LU Rukun(鲁如坤). Analysis method of soil agricultural chemistry(土壤农化分析)[M]. Beijing:Chinese Agricultural Science and Technology Press,2000.
[14] GB 15618—2018 Soil environmental quality—risk control standard for soil contamination of agricultural land(土壤环境质量农用地土壤污染风险管控标准)[S].
[15] RAURET G,LPEZ-SANCHEZ J F,SAHUQUILLO A,et al. Application of a modified BCR sequential extraction(three-step)procedure for the determination of extractable trace metal contents in a sewage sludge amended soil reference material(CRM 483),complemented by a three-year stability study of acetic acid and EDTA extractable metal content[J]. Journal of Environmental Monitoring,2000,2(3):228-233.
[16] NY/T 890—2004 Determination of available zinc,manganese,iron and copper in soil—extraction with buffered DTPA solution(土壤有效态锌、锰、铁、铜含量的测定—二乙三胺五乙酸(DTPA)浸提法)[S].
[17] GUSIATIN Z M,KLIMIUK E. Metal(Cu,Cd and Zn)removal and stabilization during multiple soil washing by saponin[J]. Chemosphere,2012,86(4):383-391.
[18] YE Tao(叶涛),HUANG Li(黄丽),ZHANG Keqiang(张克强),et al. Evaluation of the combined removal of heavy metals by saponin and citric acid from municipal sewage sludges and metal stability features[J]. Environmental Science(环境科学), 2017, 38(11):4850-4859.
[19] SUN B,ZHAO F J,LOMBI E,et al. Leaching of heavy metals from contaminated soils using EDTA[J]. Environmental Pollution,2001,113(2):111-120.
[20] POLETTINI A,POMI R,ROLLE E. The effect of operating variables on chelant-assisted remediation of contaminated dredged sediment[J]. Chemosphere,2007,66(5):866-877.
[21] PETERS R W. Chelant extraction of heavy metals from contaminated soils[J]. Journal of Hazardous Materials,1999,66(1/2):151-210.
[22] DERMONT G,BERGERON M,MERCIER G,et al.Soil washing for metal removal:a review of physic/chemical technologies and field applications[J]. Journal of Hazardous Materials,2008,152(1):1-31.
[23] NOWACK B,SIGG L. Adsorption of EDTA and metalEDTA complexes onto goethite[J]. Journal of Colloid&Interface Science,1996,177(1):106-121.
[24] TSANG D C W,ZHANG W,LO I M C. Copper extraction effectiveness and soil dissolution issue of EDTAflushing of artificially contaminated soils[J]. Chemosphere,2007,68(2):234-243.
[25] TSANG D C W,HARTLEY N R. Metal distribution and spectroscopic analysis after soil washing with chelating agents and humic substances[J]. Environmental Science and Pollution Research,2014,21(5):3987-3995.
[26] LELEYTER L,ROUSSEAU C,BIREE L,et al. Comparison of EDTA,HCl and sequential extraction procedures,for selected metals(Cu,Mn,Pb,Zn),in soils,riverine and marine sediments[J]. Journal of Geochemical Exploration,2012,116/117:51-59.
[27] JEAN-SORO L,BORDAS F,BOLLINGER J C. Column leaching of chromium and nickel from a contaminated soil using EDTA and citric acid[J]. Environmental Pollution,2012,164:175-181.
[28] UDOVIC M,LESTAN D. EDTA and HCl leaching of calcareous and acidic soils polluted with potentially toxic metals:remediation efficiency and soil impact[J].Chemosphere,2012,88(6):718-724.
[29] MAKINO T,TAKANO H,KAMIYA T,et al. Restoration of cadmium-contaminated paddy soils by washing with ferric chloride:Cd extraction mechanism and bench-scale verification[J]. Chemosphere,2008,70(6):1035-1043.
[30] CHEN C,CHEN Y,XIE T,et al. Removal,redistribution,and potential risks of soil Cd,Pb,and Zn after washing with various extractants[J]. Environmental Science and Pollution Research, 2015, 22(21):16881-16888.
[31] SEO B H,KIM H S,KWON S I,et al. Heavy metal accumulation and mobility in a soil profile depend on the organic waste type applied[J]. Journal of Soils and Sediments,2019,19(2):822-829.
[32] YU M,ZHANG J,TIAN Y. Change of heavy metal speciation, mobility, bioavailability, and ecological risk during potassium ferrate treatment of waste-activated sludge[J]. Environmental Science and Pollution Research,2018,25(14):1-10.
[33] HONG K J,TOKUNAGA S,KAJIUCHI T. Evaluation of remediation process with plant-derived biosurfactant for recovery of heavy metals from contaminated soils[J].Chemosphere,2002,49(4):379-387.
[34] KUMPIENE J,LAGERKVIST A,MAURICE C. Stabilization of As,Cr,Cu,Pb and Zn in soil using amendments-a review[J]. Waste Management,2008,28(1):215-225.
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