不同含磷化合物修复铅污染土壤后的人体健康风险评价
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摘要
磷酸盐钝化铅是铅污染土壤的重要修复技术之一.但磷酸盐修复土壤铅污染后,土壤铅对人体的健康风险仍缺乏系统研究.本研究通过向铅污染土壤添加五种不同的含磷化合物(KH_2PO_4、NH_4H_2PO_4、CaHPO_4,植酸和卵磷脂),分析了其对铅污染土壤的钝化效果,运用in vitro和SHIME模型评估修复后土壤铅对人体的健康风险.结果表明,添加含磷化合物30 d后,五种处理均有效降低了铅的DTPA和CaCl_2可提取态,分别降低了62.5%—66.5%和27.8%—49.5%,其中植酸和CaHPO_4处理效果较好,卵磷脂处理效果较差.5种处理中,铅的生物可给性在胃、小肠和结肠阶段有显著差异,分别为8.67%—9.31%、0.88%—1.55%、2.06%—2.76%,由于受pH的影响,铅在胃阶段生物可给性最高且各处理之间差异不明显,在小肠阶段KH_2PO_4处理土壤铅的生物可给性最低,卵磷脂处理铅的生物可给性最高,结肠阶段NH_4H_2PO_4处理土壤铅的生物可给性最低,卵磷脂处理铅的生物可给性最高.结肠阶段铅的生物可给性均高于小肠阶段的,可见肠道微生物促进了土壤中Pb的溶出,提高了铅的生物可给性,增加了人体的健康风险.在添加同等含量的含磷化合物修复铅污染土壤后,KH_2PO_4处理对人体健康风险最小,卵磷脂最大.
The use of phosphate as a stabilizing agent that is widely accepted and capable of lead-contaminated soil remediation. However, there are few studies on the assessment the risk of human health after remediation. In the study, five different phosphorus materials(KH_2PO_4,NH_4 H_2PO_4,CaHPO_4,Phytic acid and Lecithin) were added to lead-contaminated oil, and theirs inactivation of lead was analyzed. In vitro and SHIME models were adopted to evaluate the risk of human health of soil lead after soil remediation. The results showed that, after adding P material for 30 days, the five materials obviously decreases by 62.5%—66.5% DTPA extractable Pb and by 27.8%—49.5% CaCl_2 extractable Pb. The Pb inactivation of CaHPO_4 and phytic acid was better than the others. Among the five treatments, the Pb bioaccessibility in different phase was quite different, about 8.67%—9.31% in gastric phase, 0.88%—1.55% in small intestinal phase and 2.06%—2.76% in colon phase. The Pb bioaccessibility was highest and no significant difference was observed within the five treatments according to the low pH in gastric phase. In small intestinal, the bioaccessibility of soil lead was lowest after adding KH_2PO_4, highest after adding lecithin. In colon phase, the bioaccessibility of soil lead was lowest after adding NH_4H_2PO_4, highest after adding lecithin. In addition, the bioaccessibility of lead in colon stage was higher than that in small intestine stage, suggested that the human gut microbiota could induced Pb release from soil and increased bioaccessibility, which may resulted in a high risk to human health. After remediation of lead-contaminated soil with the same amount of the five phosphorous materials, the human health risk was the lowest by KH_2PO_4 and the highest by lecithin.
The use of phosphate as a stabilizing agent that is widely accepted and capable of lead-contaminated soil remediation. However, there are few studies on the assessment the risk of human health after remediation. In the study, five different phosphorus materials(KH_2PO_4,NH_4 H_2PO_4,CaHPO_4,Phytic acid and Lecithin) were added to lead-contaminated oil, and theirs inactivation of lead was analyzed. In vitro and SHIME models were adopted to evaluate the risk of human health of soil lead after soil remediation. The results showed that, after adding P material for 30 days, the five materials obviously decreases by 62.5%—66.5% DTPA extractable Pb and by 27.8%—49.5% CaCl_2 extractable Pb. The Pb inactivation of CaHPO_4 and phytic acid was better than the others. Among the five treatments, the Pb bioaccessibility in different phase was quite different, about 8.67%—9.31% in gastric phase, 0.88%—1.55% in small intestinal phase and 2.06%—2.76% in colon phase. The Pb bioaccessibility was highest and no significant difference was observed within the five treatments according to the low pH in gastric phase. In small intestinal, the bioaccessibility of soil lead was lowest after adding KH_2PO_4, highest after adding lecithin. In colon phase, the bioaccessibility of soil lead was lowest after adding NH_4H_2PO_4, highest after adding lecithin. In addition, the bioaccessibility of lead in colon stage was higher than that in small intestine stage, suggested that the human gut microbiota could induced Pb release from soil and increased bioaccessibility, which may resulted in a high risk to human health. After remediation of lead-contaminated soil with the same amount of the five phosphorous materials, the human health risk was the lowest by KH_2PO_4 and the highest by lecithin.
引文
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[15] 崔岩山,陈晓晨.土壤中镉的生物可给性及其对人体的健康风险评估[J].环境科学,2010,31(2):403-408.CUI Y S,CHEN X C.Bioaccessibility of soil cadmium and its health risk assessment [J].Environmental Science,2010,31(2):403-408(in Chinese).
[16] CAO X D,MA L,GAO B,et al.Dairy-manure derived biochar effectively sorbs lead and atrazine [J].Environmental Science & Technology,2009,43(9):3285-3291.
[17] KHAN M J,JONES D L.Effect of composts,lime and diammonium phosphate on the phytoavailability of heavy metals in a copper mine tailing soil [J].Pedosphere,2009,19(5):631-641.
[18] XENIDIS A,STOURAITI C,PAPASSIOPI N.Stabilization of Pb and As in soils by applying combined treatment with phosphates and ferrous iron [J].Journal of Hazardous Materials,2010,177(1):929-937.
[19] LIN C W,LIAN J,FANG H H.Soil lead immobilization using phosphate rock [J].Water Air & Soil Pollution,2005,161(1-4):113-123.
[20] 周吉峙,徐霞,张怡,等.铅羟基磷灰石的形成与稳定性[J].无机材料学报,2009,24(2):259-263.ZHOU J Z,XU X,ZHANG Y,et al.Synthesis and stability of lead-hydroxyapatite [J].Journal of Inorganic Materials,2009,24(2):259-263(in Chinese).
[21] HE M,SHI H,ZHAO X,et al.Immobilization of Pb and Cd in contaminated soil using nano-crystallite hydroxyapatite [J].Procedia Environmental Sciences,2013,18(18):657-665.
[22] 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.
[23] ZHANG J G,PROVIS J L,FENG D W,et al.Geopolymers for immobilization of Cr6+,Cd2+,and Pb2+[J].Journal of Hazardous Materials,2008,157(2):587-598.
[24] AND S S,MCBRIDE M,HENDERSHOT W.Lead phosphate solubility in water and soil suspensions [J].Environmental Science & Technology,1998,32(3):388-393.
[25] ZHANG P,RYAN J A,YANG J.In vitro soil Pb solubility in the presence of hydroxyapatite [J].Environmental Science & Technology,1998,32(32):2763-2768.
[26] RUBY M V,SCHOOF R,BRATTIN W,et al.Advances in evaluating the oral bioavailability of inorganics in soil for use in human health risk assessment [J].Environmental Science & Technology,1999,33(21):3697-3705.
[27] SCHRODER L,BASTA N T,CASTEEL S W,et al.Validation of the in vitro gastrointestinal (IVG) method to estimate relative bioavailable lead in contaminated soils [J].Journal of Environmental Quality,2004,33(2):513-521.
[28] 崔岩山,陈晓晨,朱永官.利用3种in vitro方法比较研究污染土壤中铅、砷生物可给性[J].农业环境科学学报,2008,1(2):414-419.CUI Y S,CHEN X C,ZHU Y G.Comparison of three in vitro methods to study the bioaccessibility of soil lead and arsenic [J].Journal of Agro-Environment Science,2008,1(2):414-419(in Chinese).
[29] 付瑾,崔岩山.In vitro系统评价胃肠液pH及土液比对铅、镉、砷生物可给性的影响[J].农业环境科学学报,2012,31(2):245-251.FU J,CUI Y S.In vitro model system to evaluate the influence of pH and soil-gastric/intestinal juices ratio on bioaccessibility of Pb,Cd and As in two typical contaminated soils [J].Journal of Agro-Environment Science,2012,31(2):245-251(in Chinese).
[30] WRAGG J,CAVE M,BASTA N,et al.An inter-laboratory trial of the unified BARGE bioaccessibility method for arsenic,cadmium and lead in soil [J].Science of the Total Environment,2011,409(19):4016-4030.
[31] 尹乃毅,都慧丽,张震南,等.应用SHIME模型研究肠道微生物对土壤中镉、铬、镍生物可给性的影响[J].环境科学,2016,37(6):2353-2358.YIN N Y,DU H L,ZHANG Z N,et al.Effects of human gut microbiota on bioaccessibility of soil Cd,Cr and Ni using SHIME model [J].Environmental Science,2016,37(6):2353-2358(in Chinese).
[32] VAND W T,GALLAWA C M,KUBACHKA K M,et al.Arsenic metabolism by human gut microbiota upon in vitro digestion of contaminated soils [J].Environmental Health Perspectives,2010,118(7):1004-1009.
[2] YAN L,KONG L,QU Z,et al.Magnetic biochar decorated with ZnS nanocrytals for Pb (II) removal [J].Acs Sustainable Chemistry & Engineering,2015,3(1):125-132.
[3] 郑袁明,陈同斌,陈煌,等.北京市不同土地利用方式下土壤铅的积累[J].地理学报,2005,60(5):791-797.ZHENG Y M,CHEN T B,CHEN H,et al.Lead accumulation in soils under different land use types in Beijing City [J].Acta Geographica Sinica,2005,60(5):791-797(in Chinese).
[4] 白雁斌,赵晓玉,王天娇.土壤铅污染修复技术研究进展及展望 [J].新疆环境保护,2012,34(4):16-19.BAI Y B,ZHAO X Y,WANG T J.Progress and prospective in lead contaminated soil remediation technology[J].Environmental Protection of Xinjiang,2012,34(4):16-19(in Chinese).
[5] 佟亚欧,金兰淑.土壤铅污染现状及钝化修复技术探讨[J].农业科技与装备,2010(6):31-32.TONG Y O,JIN L S.Discussion on the current soil lead pollution and inactivation restoring Technology [J].Agricultural Science & Technology & Equipment,2010(6):31-32(in Chinese).
[6] 宋波,曾炜铨,陆素芬,等.含磷材料在铅污染土壤修复中的应用[J].环境工程学报,2015,9(12):5649-5658.SONG B,ZENG W Q,LU S F,et al.Application of phosphorus materials in remediation of lead-contaminated soil [J].Chinese Journal of Environmental Engineering,2015(in Chinese).
[7] MIRETZKY P,FERNANDEZ-CIRELLI A.Phosphates for Pb immobilization in soils:A review [J].Environmental Chemistry Letters,2008,6(3):121-133.
[8] 龙梅,胡锋,李辉信,等.低成本含磷材料修复环境重金属污染的研究进展[J].环境污染治理技术与设备,2006,7(7):1-10.LONG M,HU F,LI X H,et al.Recent trends in the remediation of heavy metal-contaminated environments with low-cost phosphorus-containing materials [J].Techniques & Equipment for Environmental Pollution Control,2006,7(7):1-10(in Chinese).
[9] TANG X Y,ZHU Y G,CHEN S B,et al.Assessment of the effectiveness of different phosphorus fertilizers to remediate Pb-contaminated soil using in vitro test [J].Environment International,2004,30(4):531-537.
[10] CAO X,MA L Q,CHEN M,et al.Impacts of phosphate amendments on lead biogeochemistry at a contaminated site [J].Environmental Science & Technology,2002,36(24):5296-5304.
[11] 鲁如坤.土壤农业化学分析方法[M].北京:中国农业科技出版社,2000.LU R K.Methods of soil agricultural chemistry analysis [M].Beijing:Chinese Agricultural Science and Technology Press,2000(in Chinese).
[12] 唐翔宇,朱永官.土壤中重金属对人体生物有效性的体外试验评估[J].环境与健康杂志,2004,21(3):183-185.TANG X Y,ZHU Y G.Advances in in vitro tests in evaluating bioavailability of heavy metals in contaminated soil via oral intake [J].Journal of Environment & Health,2004,21(3):183-185(in Chinese).
[13] YIN N Y,ZHANG Z N,CAI X L,et al.In vitro method to assess soil arsenic metabolism by human gut microbiota:Arsenic speciation and distribution [J].Environmental Science & Technology,2015,49(17):10675-10681.
[14] 都慧丽,尹乃毅,张震南,等.肠道微生物对土壤中铜、锌、锰生物可给性的影响[J].生态毒理学报,2017,12(3):301-308.DU H L,YIN N Y,ZHANG Z N,et al.Effect of human gut microbiota on bioaccessibility of soil Cu,Zn and Mn [J].Asian Journal of Ecotoxicology,2017,12(3):301-308.(in Chinese).
[15] 崔岩山,陈晓晨.土壤中镉的生物可给性及其对人体的健康风险评估[J].环境科学,2010,31(2):403-408.CUI Y S,CHEN X C.Bioaccessibility of soil cadmium and its health risk assessment [J].Environmental Science,2010,31(2):403-408(in Chinese).
[16] CAO X D,MA L,GAO B,et al.Dairy-manure derived biochar effectively sorbs lead and atrazine [J].Environmental Science & Technology,2009,43(9):3285-3291.
[17] KHAN M J,JONES D L.Effect of composts,lime and diammonium phosphate on the phytoavailability of heavy metals in a copper mine tailing soil [J].Pedosphere,2009,19(5):631-641.
[18] XENIDIS A,STOURAITI C,PAPASSIOPI N.Stabilization of Pb and As in soils by applying combined treatment with phosphates and ferrous iron [J].Journal of Hazardous Materials,2010,177(1):929-937.
[19] LIN C W,LIAN J,FANG H H.Soil lead immobilization using phosphate rock [J].Water Air & Soil Pollution,2005,161(1-4):113-123.
[20] 周吉峙,徐霞,张怡,等.铅羟基磷灰石的形成与稳定性[J].无机材料学报,2009,24(2):259-263.ZHOU J Z,XU X,ZHANG Y,et al.Synthesis and stability of lead-hydroxyapatite [J].Journal of Inorganic Materials,2009,24(2):259-263(in Chinese).
[21] HE M,SHI H,ZHAO X,et al.Immobilization of Pb and Cd in contaminated soil using nano-crystallite hydroxyapatite [J].Procedia Environmental Sciences,2013,18(18):657-665.
[22] 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.
[23] ZHANG J G,PROVIS J L,FENG D W,et al.Geopolymers for immobilization of Cr6+,Cd2+,and Pb2+[J].Journal of Hazardous Materials,2008,157(2):587-598.
[24] AND S S,MCBRIDE M,HENDERSHOT W.Lead phosphate solubility in water and soil suspensions [J].Environmental Science & Technology,1998,32(3):388-393.
[25] ZHANG P,RYAN J A,YANG J.In vitro soil Pb solubility in the presence of hydroxyapatite [J].Environmental Science & Technology,1998,32(32):2763-2768.
[26] RUBY M V,SCHOOF R,BRATTIN W,et al.Advances in evaluating the oral bioavailability of inorganics in soil for use in human health risk assessment [J].Environmental Science & Technology,1999,33(21):3697-3705.
[27] SCHRODER L,BASTA N T,CASTEEL S W,et al.Validation of the in vitro gastrointestinal (IVG) method to estimate relative bioavailable lead in contaminated soils [J].Journal of Environmental Quality,2004,33(2):513-521.
[28] 崔岩山,陈晓晨,朱永官.利用3种in vitro方法比较研究污染土壤中铅、砷生物可给性[J].农业环境科学学报,2008,1(2):414-419.CUI Y S,CHEN X C,ZHU Y G.Comparison of three in vitro methods to study the bioaccessibility of soil lead and arsenic [J].Journal of Agro-Environment Science,2008,1(2):414-419(in Chinese).
[29] 付瑾,崔岩山.In vitro系统评价胃肠液pH及土液比对铅、镉、砷生物可给性的影响[J].农业环境科学学报,2012,31(2):245-251.FU J,CUI Y S.In vitro model system to evaluate the influence of pH and soil-gastric/intestinal juices ratio on bioaccessibility of Pb,Cd and As in two typical contaminated soils [J].Journal of Agro-Environment Science,2012,31(2):245-251(in Chinese).
[30] WRAGG J,CAVE M,BASTA N,et al.An inter-laboratory trial of the unified BARGE bioaccessibility method for arsenic,cadmium and lead in soil [J].Science of the Total Environment,2011,409(19):4016-4030.
[31] 尹乃毅,都慧丽,张震南,等.应用SHIME模型研究肠道微生物对土壤中镉、铬、镍生物可给性的影响[J].环境科学,2016,37(6):2353-2358.YIN N Y,DU H L,ZHANG Z N,et al.Effects of human gut microbiota on bioaccessibility of soil Cd,Cr and Ni using SHIME model [J].Environmental Science,2016,37(6):2353-2358(in Chinese).
[32] VAND W T,GALLAWA C M,KUBACHKA K M,et al.Arsenic metabolism by human gut microbiota upon in vitro digestion of contaminated soils [J].Environmental Health Perspectives,2010,118(7):1004-1009.