杭州市环境介质中有机氯化物的污染特征研究
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摘要
农药,长久以来为解决人类的温饱问题和促进社会发展做出了杰出贡献,但其带来的环境污染问题也不容忽视。滴滴涕(dichlorodiphenyltrichloroethanes, DDTs)、六六六(hexachlorocyclohexanes, HCHs)、多效唑(paclobutrazol, PBZ)、烯效唑(uniconazole, UCZ)分子中都含有氯原子,可归为有机氯化物(organochlirine compounds, OCs),在环境中不易降解、能够持久存在。在中国,前两类化合物在农业上的使用已被全面禁止,后两类化合物作为植物生长调节剂仍在使用。杭州市作为农业曾经非常发达的区域,曾使用了大量DDTs和HCHs,但其污染特征至今不明。随着城市化进程的发展,虽然杭州市区已经基本不存在农业,但为了保障杭州市生态功能的完整和粮食供应,郊区仍保留有农田,并为了提高农作物经济效益,部分农田采用了大棚栽培。为评估杭州市环境中禁用有机氯化物污染特征和大棚栽培对现用有机氯化物污染的影响,进一步研判杭州市环境中有机氯化物的污染趋势,本论文研究了DDTs和HCHs在杭州市区的大气、水体和沉积物等环境介质中的污染特征和分布规律,以及PBZ和UCZ在杭州市郊农田中露地和大棚两种栽培环境下的消散特征,并分析了其中手性化合物的对映体选择性。
杭州市水体环境中ΣOCs (DDTs和HCHs的质量和)在沉积物、溶解相和颗粒相中的高值点均出现在钱塘江-西湖换水口,说明钱塘江水体中的DDTs和HCHs是杭州水体环境介质中的一个重要来源。在相间分配中,气相-水相间DDTs和HCHs趋向存在于气相；沉积物-水相间DDTs和HCHs趋向存在于沉积物；颗粒相-溶解相间,DDTs趋向存在于颗粒相,而HCHs趋向存在于溶解相。绝大部分沉积物样品中的(-)-α-HCH和(-)-o,p-DDT对映体被优先降解。
Ingersoll风险评估结果表明,杭州市内河河道沉积物中DDTs类污染物(主要是p,p'-DDE)和γ-HCH存在一定的潜在生态风险,有可能对沉积物层生物产生潜在危害,并通过生物富集作用对人类的健康造成潜在的负面影响。水体中有部分p,p'-DDT超过了美国EPA(2009)规定的持续浓度标准(CCC)参考值(该参考值旨在保护水生生物不受低浓度污染物长期作用所造成的慢性毒性效应影响),这表明p,p'-DDT有可能使水生生物受到慢性毒性效应,应当引起注意。
大棚环境中PBZ和UCZ的消散特征与露地环境不同。相比露地土壤,PBZ和UCZ在大棚土壤中更能持久存在,露地和大棚接受的降雨量不同是造成这两种农药在杭州露地和大棚土壤中差异的主要原因。PBZ和UCZ有渗透到深层土壤中的可能性,而且UCZ的渗透性比PBZ的强。PBZ和UCZ在土壤中的降解都存在对映体选择性,PBZ和UCZ的(+)-对映体优先在露地土壤、大棚土壤和实验室培育土壤中降解。
大棚中PBZ和UCZ更容易持久存在,增加了下一期作物受药害的可能性,因此大棚中使用PBZ和UCZ需要减少剂量。受降雨的影响,PBZ和UCZ在露地土壤中的淋溶有污染地下水环境风险。此外,PBZ和UCZ的对映体选择性降解表明对其的环境风险和监管应从对映体水平考虑。
Pesticides give a contribution to social development for a long time. However, it can not be ignored that the environmental pollution produced by them. Dichlorodiphenyltrichloroethanes (DDTs), hexachlorocyclohexanes (HCHs), paclobutrazol (PBZ) and uniconazole (UCZ), which can be classified as organochlirine compounds (OCs), were persistent and not easily degraded in environment. In China, DDTs and HCHs have been banned, while PBZ and UCZ were still use now. Hangzhou, which was developed agriculture area, had used a large amount of organochlorine compounds. Pollution by these compounds is still unknown in this area. With the development of urbanization, agriculture has been basically disappeared in Hangzhou. However, the suburb still retains farmland for ecological functions and purveyance,. Some greenhouses used in farmland to increase economic benefit of crops. The pollution characteristic of DDTs and HCHs which have been banned and dissipation differences by greenhouse and open field cultivation of PBZ and UCZ which are currently used were still unclear. This work investigate the pollution characteristic of the above compounds in Hangzhou including residues and distribution characteristics of DDTs and HCHs in air, water and sediment, dissipation characteristics of PBZ and UCZ in open field and greenhouse, and enantioselective degradation of organochlirine compounds in environment.
The highest concentration of DDTs and HCHs were found in water exchange outlet of Qiantang River to West Lake in dissolved, particle phase and surface sediment, which indicate Qiantang River might be source of DDTs and HCHs in Hangzhou.DDTs and HCHs tend to exist in the air and sediment according to the distribution coefficient Ki.j. DDTs tend to exist in the particle phase, while HCHs are prone to present in the dissolved phase in water.
The (+)-enantiomers of a-HCH and o,p-DDT were more prevalent than (-)-enantiomer in most sediment column samples.
The concentrations of DDTs and HCHs in water and sediment do not exceed the national environmental quality standard. Risk assessment for surface sediment indicates that DDTs (especially p, p'-DDE) and y-HCH are the main species of ectoxicological concern. p,p'-DDT in some samples exceeded the Criterion Continuous Concentration (CCC,USEPA2009) value in water. It should be paid more attention that aquatic life suffered chronic toxicity by p,p'-DDT.
The dissipation of paclobutrazol(PBZ) and uniconazole(UCZ) in greenhouse were different from those in open field.They were more persistent in greenhouse than in open field soil. The penetration produced by rainfall gave a greater contribution to the dissipation of PBZ and UCZ in open field surface soil than that in greenhouse surface soil. PBZ and UCZ had potentials to penetrate into deep soil layers. UCZ was more potent than paclobutrazol in penetration and leaching. Enantioselective degradation of PBZ and UCZ were observed in both soils.
The persistence of PBZ and UCZ in greenhouse soil increased the possibility of phytotoxicity to the next crops, whereas the leaching in open field surface soil would produce environmental risk to groundwater and also contaminate surface water by ground-water input. It should be paid attention to the use amount of PBZ and UCZ in greenhouses and application time in open field. Additionally, environment risk and management of PBZ and UCZ should be considered at enantiomers level.
杭州市水体环境中ΣOCs (DDTs和HCHs的质量和)在沉积物、溶解相和颗粒相中的高值点均出现在钱塘江-西湖换水口,说明钱塘江水体中的DDTs和HCHs是杭州水体环境介质中的一个重要来源。在相间分配中,气相-水相间DDTs和HCHs趋向存在于气相；沉积物-水相间DDTs和HCHs趋向存在于沉积物；颗粒相-溶解相间,DDTs趋向存在于颗粒相,而HCHs趋向存在于溶解相。绝大部分沉积物样品中的(-)-α-HCH和(-)-o,p-DDT对映体被优先降解。
Ingersoll风险评估结果表明,杭州市内河河道沉积物中DDTs类污染物(主要是p,p'-DDE)和γ-HCH存在一定的潜在生态风险,有可能对沉积物层生物产生潜在危害,并通过生物富集作用对人类的健康造成潜在的负面影响。水体中有部分p,p'-DDT超过了美国EPA(2009)规定的持续浓度标准(CCC)参考值(该参考值旨在保护水生生物不受低浓度污染物长期作用所造成的慢性毒性效应影响),这表明p,p'-DDT有可能使水生生物受到慢性毒性效应,应当引起注意。
大棚环境中PBZ和UCZ的消散特征与露地环境不同。相比露地土壤,PBZ和UCZ在大棚土壤中更能持久存在,露地和大棚接受的降雨量不同是造成这两种农药在杭州露地和大棚土壤中差异的主要原因。PBZ和UCZ有渗透到深层土壤中的可能性,而且UCZ的渗透性比PBZ的强。PBZ和UCZ在土壤中的降解都存在对映体选择性,PBZ和UCZ的(+)-对映体优先在露地土壤、大棚土壤和实验室培育土壤中降解。
大棚中PBZ和UCZ更容易持久存在,增加了下一期作物受药害的可能性,因此大棚中使用PBZ和UCZ需要减少剂量。受降雨的影响,PBZ和UCZ在露地土壤中的淋溶有污染地下水环境风险。此外,PBZ和UCZ的对映体选择性降解表明对其的环境风险和监管应从对映体水平考虑。
Pesticides give a contribution to social development for a long time. However, it can not be ignored that the environmental pollution produced by them. Dichlorodiphenyltrichloroethanes (DDTs), hexachlorocyclohexanes (HCHs), paclobutrazol (PBZ) and uniconazole (UCZ), which can be classified as organochlirine compounds (OCs), were persistent and not easily degraded in environment. In China, DDTs and HCHs have been banned, while PBZ and UCZ were still use now. Hangzhou, which was developed agriculture area, had used a large amount of organochlorine compounds. Pollution by these compounds is still unknown in this area. With the development of urbanization, agriculture has been basically disappeared in Hangzhou. However, the suburb still retains farmland for ecological functions and purveyance,. Some greenhouses used in farmland to increase economic benefit of crops. The pollution characteristic of DDTs and HCHs which have been banned and dissipation differences by greenhouse and open field cultivation of PBZ and UCZ which are currently used were still unclear. This work investigate the pollution characteristic of the above compounds in Hangzhou including residues and distribution characteristics of DDTs and HCHs in air, water and sediment, dissipation characteristics of PBZ and UCZ in open field and greenhouse, and enantioselective degradation of organochlirine compounds in environment.
The highest concentration of DDTs and HCHs were found in water exchange outlet of Qiantang River to West Lake in dissolved, particle phase and surface sediment, which indicate Qiantang River might be source of DDTs and HCHs in Hangzhou.DDTs and HCHs tend to exist in the air and sediment according to the distribution coefficient Ki.j. DDTs tend to exist in the particle phase, while HCHs are prone to present in the dissolved phase in water.
The (+)-enantiomers of a-HCH and o,p-DDT were more prevalent than (-)-enantiomer in most sediment column samples.
The concentrations of DDTs and HCHs in water and sediment do not exceed the national environmental quality standard. Risk assessment for surface sediment indicates that DDTs (especially p, p'-DDE) and y-HCH are the main species of ectoxicological concern. p,p'-DDT in some samples exceeded the Criterion Continuous Concentration (CCC,USEPA2009) value in water. It should be paid more attention that aquatic life suffered chronic toxicity by p,p'-DDT.
The dissipation of paclobutrazol(PBZ) and uniconazole(UCZ) in greenhouse were different from those in open field.They were more persistent in greenhouse than in open field soil. The penetration produced by rainfall gave a greater contribution to the dissipation of PBZ and UCZ in open field surface soil than that in greenhouse surface soil. PBZ and UCZ had potentials to penetrate into deep soil layers. UCZ was more potent than paclobutrazol in penetration and leaching. Enantioselective degradation of PBZ and UCZ were observed in both soils.
The persistence of PBZ and UCZ in greenhouse soil increased the possibility of phytotoxicity to the next crops, whereas the leaching in open field surface soil would produce environmental risk to groundwater and also contaminate surface water by ground-water input. It should be paid attention to the use amount of PBZ and UCZ in greenhouses and application time in open field. Additionally, environment risk and management of PBZ and UCZ should be considered at enantiomers level.
引文
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