填埋场及周边地下水中氯代有机物组成与风险研究

郑敬; 潘琦; 王玉欣; 沙浩群; 王宪革; 刘洪宝; 何小松

doi:10.12153/j.issn.1674-991X.20230351

填埋场及周边地下水中氯代有机物组成与风险研究

doi: 10.12153/j.issn.1674-991X.20230351

郑敬^{1, 2, 3,},
潘琦^{1, 2, 3},
王玉欣^{2, 3},
沙浩群^{2, 3},
王宪革^{2, 3},
刘洪宝^{2, 3},
何小松^{2, 3, ,}

1.
桂林理工大学环境科学与工程学院
2.
环境基准与风险评估国家重点实验室, 中国环境科学研究院
3.
国家环境保护地下水污染模拟与控制重点实验室, 中国环境科学研究院

基金项目: 国家自然科学基金项目(52070174)

详细信息

作者简介:
郑敬(1997—)，男，硕士研究生，主要研究方向为固体废物处理处置及资源化，1304658346@qq.com

通讯作者:
何小松(1982—)，男，研究员，博士，主要从事土壤修复和固体废物处理处置技术研究，hexs82@126.com

中图分类号: X523
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出版历程
- 收稿日期: 2023-05-09
- 录用日期: 2023-08-09
- 修回日期: 2023-08-08
- 网络出版日期: 2023-11-10

Study on the composition and risk of chlorinated organic compounds in landfills and surrounding groundwater

ZHENG Jing^{1, 2, 3
,},
PAN Qi^{1, 2, 3},
WANG Yuxin^{2, 3},
SHA Haoqun^{2, 3},
WANG Xiange^{2, 3},
LIU Hongbao^{2, 3},
HE Xiaosong^{2, 3
, ,}

1.
College of Environmental Science and Engineering, Guilin University of Technology
2.
State Key Laboratory of Environment Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences
3.
State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Sciences

摘要

摘要:
氯代有机物降解难、毒性大，填埋场是氯代有机物的重要汇集地。针对填埋场渗滤液泄漏进入地下水中氯代有机物风险不明现状，采集了一个非正规填埋场的地下水样品，并结合收集的中国、德国、美国、西班牙、波兰、挪威共6个国家13个填埋场附近地下水氯代有机物组成与浓度数据，采用风险评价模型对其健康风险进行评估。结果显示：所研究填埋场地下水总共检出10类41种氯代有机物，这些氯代有机物中，氯代环烷烃类的致癌风险最大，均超过了10⁻⁴，远超人体可接受的水平，具有明确风险；氯代多氟烷基醚磺酸盐的F-53B的致癌风险最低，为10⁻⁶~10⁻⁴，具有可能致癌风险。氯代烷烃类的非致癌风险最大，其中α-六氯环己烷的非致癌风险值均超过1，超过人类可接受水平；而氯代有机农药类如丙环唑和氯菊酯的非致癌风险最低，其非致癌风险值未超过人体可接受的水平。需要加强关注γ-六氯环己烷、氯苯、1,2-二氯苯等氯代有机物风险管控，可采用氧化脱氯、还原脱氯及共代谢脱氯等途径，加速其脱氯和降解，消除其风险。
- 氯代有机物 /
- 地下水 /
- 填埋场 /
- 健康风险评估
Abstract:
Chlorinated organic compounds are difficult to degrade and highly toxic, and landfills are important gathering places for chlorinated organic compounds. To evaluate the uncertain risk of landfill leachate contaminating groundwater with chlorinated organic compounds, a groundwater sample was collected from an informal landfill site. Combined with the collected data on the composition and concentration of chlorinated organic compounds in groundwater near 13 landfills in 6 countries including China, Germany, the United States, Spain, Poland, and Norway, a risk assessment model was used to assess their health risks. A total of 41 different types of chlorinated organic compounds, categorized into 10 classes, were identified in the groundwater near the landfills studied. The chlorinated cycloalkanes pose the highest carcinogenic risk, with all measurements surpassing 10⁻⁴, far exceeding the tolerable limits for human exposure, and presenting significant health hazards. The F-53B of chloropolyfluoroalkyl ether sulfonate has the lowest carcinogenic risk, between 10⁻⁶ and 10⁻⁴, and has a possible carcinogenic risk. The non-carcinogenic risk of chlorinated alkanes is the highest, among which the non-carcinogenic risk value of α-hexachlorocyclohexane (HCH) exceeds 1, more than the acceptable level for human beings. However, chlorinated organic pesticides such as propiconazole and permethrin have the lowest non-carcinogenic risk, and their non-carcinogenic risk value does not exceed the acceptable level for human body. Greater emphasis should be placed on risk management strategies for specific chlorinated organic compounds, namely γ-HCH, chlorobenzene, and 1,2-dichlorobenzene. Various methods, including oxidative dechlorination, reductive dechlorination, and co-metabolism dechlorination, can be employed to expedite the dechlorination and degradation processes, ultimately eliminating associated risks.
- chlorinated organic compounds /
- groundwater /
- landfill /
- health risk assessment

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图 1 地下水采样点布设示意

Figure 1. Layout of groundwater sampling points

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图 2 垃圾填埋场地下水氯代有机物致癌风险

注：F-53B为氯代多氟烷基醚磺酸盐的一种。

Figure 2. Carcinogenic risk of chlorinated organic compounds in groundwater of landfill sites

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图 3 垃圾填埋场地下水氯代有机物非致癌风险

Figure 3. Non carcinogenic risk of chlorinated organic compounds in groundwater of landfill sites

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表 1 填埋场场地信息

Table 1. Landfill Site Information

时间(年-月)	场地类型	地下水类型	地点	特征污染物
2014-06	医疗及建筑垃圾堆场	孔隙水	中国河南省开封市	1,2,4-三氯苯
2021-06	非正规填埋场	裂隙水	中国四川省资阳市	重金属、氯苯、氯仿等
2021-03	非正规填埋场	孔隙水	中国江苏省徐州市	三氯甲烷、四氯化碳、甲苯
2021-01	非正规填埋场	孔隙水	中国浙江省杭州市	全氟烷基物
2020-10	非正规填埋场		中国福建省某县	重金属
2015-04	正规垃圾填埋场		美国佛罗里达州	铁、氨、氯苯
2016-05	小型垃圾堆场	孔隙水	美国内布拉斯加州	三氯乙烯
2009-03	非正规填埋场		美国印第安纳州	PPCP
2018-12	农药类垃圾堆场	孔隙水	西班牙萨比尼亚尼戈	六氯环己烷、氯苯类化合物
2017-07	农药类垃圾堆场	孔隙水	德国萨克森州	六氯环己烷
2018-04	非正规填埋场	孔隙水	德国杜塞尔多夫	1,4-二噁烷
2021-01	危险废物填埋场		波兰华沙	多氯联苯
2008-12	农药类垃圾堆场	孔隙水	挪威奥斯陆	DDT

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表 2 风险计算过程中污染物相关参数

Table 2. Pollutant related parameters in the risk calculation process

污染物	q/ 〔mg/(kg·d)〕⁻¹	RfD/ 〔mg/(kg·d)〕	PC/(cm/h)
α-六氯环己烷	6.30
β-六氯环己烷	1.80
γ-六氯环己烷	1.10	3.00×10⁻⁴
氯苯		2.00×10⁻²	2.66×10⁻²
1,4-二氯苯	5.40×10⁻³		5.57×10⁻²
1,2-二氯苯		9.00×10⁻²	5.25×10⁻²
1,2,4-三氯苯		1.00×10⁻²	6.87×10⁻²
1,2,4,5-四氯苯		3.00×10⁻⁴	0.21
五氯苯		8.00×10⁻⁴	0.36
2和4-一氯酚			3.02×10⁻⁴
2,4-二氯酚		3.00×10⁻³	2.40×10⁻²
四氯酚		3.00×10⁻²	5.41×10⁻⁵
一氯乙烯	0.72		5.77×10⁻³
1,1-二氯乙烯		5.00×10⁻²	3.38×10⁻³
反式1,2-二氯乙烯		2.00×10⁻²	9.49×10⁻³
顺式1,2-二氯乙烯		2.00×10⁻³	9.49×10⁻³
三氯乙烯	4.60×10⁻²	5.00×10⁻⁴	1.12×10⁻²
二氯甲烷	2.00×10⁻³	6.00×10⁻³	3.54×10⁻³
三氯甲烷	3.10×10⁻²	1.00×10⁻²	6.79×10⁻³
四氯化碳	7.00×10⁻²	4.00×10⁻³	1.21×10⁻²
二氯乙烷	5.70×10⁻³		4.19×10⁻³
1，2-二氯丙烷	9.10×10⁻²		7.95×10⁻³
1,1-二氯乙醚	3.70×10⁻²		1.78×10⁻³
丙环唑		1.30×10⁻³	1.92×10⁻⁵
氯菊酯		5.00×10⁻²	1.02×10⁻⁵
滴滴涕	0.34	5.00×10⁻⁴	1.64×10⁻⁵
氯代多氟烷基醚磺酸盐F-53B	5.00×10⁻⁴		1.01×10⁻⁶
二氯二氟甲烷		0.20	8.88×10⁻³

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表 3 国内外填埋场地下水中氯代有机物组成与浓度分布

Table 3. Composition and concentration of chlorinated organic compounds in groundwater of landfill sites at home and abroad μg/L

类别	污染物	样本数	浓度范围	均值	地点	数据来源
氯代环烷烃类化合物	α-六氯环己烷	26	ND~1 740.1	237.85	德国萨克森州、西班牙萨比尼亚尼戈	文献[16-17]
	β-六氯环己烷	26	ND~735.6	129.27
	δ-六氯环己烷	26	ND~17 886.4	3 116.93
	γ-六氯环己烷	39	ND~7 051.5	533.06	德国萨克森州、西班牙萨比尼亚尼戈、挪威奥斯陆	文献[11，16-17]
	ε-六氯环己烷	8	7.3~1 030.7	565.83	西班牙萨比尼亚尼戈	文献[17]
氯苯类化合物	氯苯	43	ND~32 730	5 384.09	美国佛罗里达州、西班牙萨比尼亚尼戈、中国四川、中国江苏（实测）	文献[8，17，26]、实测数据
	1,3-二氯苯	8	0.1~188	101.36	西班牙萨比尼亚尼戈	文献[17]
	1,4-二氯苯	15	ND~3 895	822.02	美国佛罗里达州、西班牙萨比尼亚尼戈	文献[8，17]
	1,2-二氯苯	35	0.1~2 068.1	317.97	西班牙萨比尼亚尼戈、中国河南	文献[17-18]
	1,3,5-三氯苯	8	0.1~13.9	5.59	西班牙萨比尼亚尼戈	文献[17]
	1,2,4-三氯苯	35	0.76~1 316	161.52	西班牙萨比尼亚尼戈、中国河南	文献[17-18]
	1,2,3-三氯苯	35	0.2~101	18.58	西班牙萨比尼亚尼戈、中国河南	文献[17-18]
	1,2,3,5-四氯苯	8	0.8~39.8	21.4	西班牙萨比尼亚尼戈	文献[17]
	1,2,4,5-四氯苯	8	0.3~58.3	28.34
	五氯苯	8	0.2~7.8	2.85
氯酚类化合物	2-氯酚和4-氯酚	8	0.1~271	160.23	西班牙萨比尼亚尼戈	文献[17]
	3-氯酚	8	0.1~4 704.2	2263.06
	2,6-二氯酚	8	0.1~65.2	33.34
	2,4-二氯酚	8	0.1~327	163.84
	四氯酚	8	0.2~778.4	227.13
联苯^1）	多氯联苯	49	0.2~3.1	0.00058	波兰华沙	文献[10]
氯代烯烃类化合物	一氯乙烯	7	ND~2	0.39	美国佛罗里达州	文献[8]
	1,1-二氯乙烯	13	2~488	232.08	美国内布拉斯加州	文献[13]
	反式1,2-二氯乙烯	13	ND~4	0.62	美国内布拉斯加州	文献[13]
	顺式1,2-二氯乙烯	26	ND~280	62.95	美国内布拉斯加州、中国江苏（实测）	文献[13]、实测数据
	三氯乙烯	31	0.1~150	21.51	德国杜塞尔多夫	文献[9]
氯代烷烃类化合物	一氯甲烷	8	0.1~2.5	1.975	西班牙萨比尼亚尼戈	文献[17]
	二氯甲烷	7	ND~0.89	0.25	美国佛罗里达州	文献[8]
	三氯甲烷	40	ND~19900	498.34	中国江苏、中国江苏（实测）	文献[27]、实测数据
	四氯化碳	12	0.1~4.2	1.16	中国江苏	文献[27]
	二氯乙烷	27	ND~912	39.07	西班牙萨比尼亚尼戈、中国四川、中国福建	文献[17，26，28]
	1,2-二氯丙烷	17	ND~33.5	3.37	美国印第安纳州、中国江苏（实测）	文献[12]、实测数据
氯醚	1,1-二氯乙醚	13	10~69	38.69	挪威奥斯陆	文献[11]
	1,2-二氯乙醚	13	ND~280	0.15	美国内布拉斯加州	文献[13]
	1,1,1-三氯乙醚	13	15~378	169.77	美国内布拉斯加州	文献[13]
有机氯农药	丙环唑	13	ND~0.25	0.04	挪威奥斯陆	文献[11]
	氯菊酯	13	ND~0.61	0.05
	异丙二酮	13	ND~0.13	0.01
	滴滴涕	13	ND~0.1	0.01
氯有机盐^1）	氯代多氟烷基醚磺酸盐F-53B	15	0.2~5.01	1.56	中国浙江	文献[14]
氟氯烃	二氯二氟甲烷	4	ND~7	2.75	美国印第安纳州	文献[12]
注：ND表示未检出。1）单位为ng/L。

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表 4 经口摄入和皮肤接触途径日暴露量

Table 4. Daily exposure levels through oral intake and skin contact pathways mg/(kg·d)　

类别	污染物	经口摄入			皮肤接触
类别	污染物	平均值	最小值	最大值	平均值	最小值	最大值
氯代环烷烃	α-六氯环己烷	7.93	3.33×10⁻⁴	58.00	2.45×10⁻³	1.03×10⁻⁷	1.79×10⁻²
	β-六氯环己烷	4.31	3.33×10⁻⁴	24.50	1.33×10⁻³	1.03×10⁻⁷	7.58×10⁻³
	δ-六氯环己烷	1.04×10²	3.33×10⁻⁴	5.96×10²	3.21×10⁻²	1.03×10⁻⁷	0.18
	γ-六氯环己烷	17.80	3.33×10⁻⁴	2.35×10²	5.50×10⁻³	1.03×10⁻⁷	7.27×10⁻²
	ε-六氯环己烷	18.90	0.24	34.40	5.83×10⁻³	7.53×10⁻⁵	1.06×10⁻²
氯苯类化合物	氯苯	1.79×10²	3.33×10⁻⁴	1.09×10³	39.57	7.35×10⁻⁵	2.41×10²
	1,3-二氯苯	3.38	3.33×10⁻³	6.27	1.14	1.12×10⁻³	2.11
	1,4-二氯苯	27.40	3.33×10⁻⁴	1.30×10²	12.70	1.54×10⁻⁴	60.10
	1,2-二氯苯	10.60	3.33×10⁻³	68.90	4.61	1.45×10⁻³	30.00
	1,3,5-三氯苯	0.19	3.33×10⁻³	0.46	0.16	2.78×10⁻³	0.39
	1,2,4-三氯苯	5.38	2.53×10⁻²	43.90	3.07	1.44×10⁻²	25.00
	1,2,3-三氯苯	0.62	6.67×10⁻³	3.37	0.52	5.56×10⁻³	2.81
	1,2,3,5-四氯苯	0.71	2.67×10⁻²	1.33	1.25	4.67×10⁻²	2.32
	1,2,4,5-四氯苯	0.95	1.00×10⁻²	1.94	1.65	1.75×10⁻²	3.40
	五氯苯	9.50×10⁻²	6.67×10⁻³	0.26	0.28	1.98×10⁻²	0.77
氯酚类化合物	2-氯酚和4-氯酚	5.34	3.33×10⁻³	9.03	1.34×10⁻²	8.36×10⁻⁶	2.26×10⁻²
	3-氯酚	75.40	3.33×10⁻³	1.57×10²	0.19	8.36×10⁻⁶	0.39
	2,6-二氯酚	1.11	3.33×10⁻³	2.17	0.21	6.33×10⁻⁴	0.41
	2,4-二氯酚	5.46	3.33×10⁻³	10.9	1.09	6.63×10⁻⁴	2.17
	四氯酚	7.57	6.67×10⁻³	25.90	3.40×10⁻³	2.99×10⁻⁶	1.17×10⁻²
联苯	多氯联苯	1.93×10⁻⁵	6.67×10⁻⁶	1.03×10⁻⁴	2.54×10⁻⁷	8.77×10⁻⁸	1.36×10⁻⁶
氯代烯烃	一氯乙烯	1.30×10⁻²	3.33×10⁻⁴	6.67×10⁻²	6.22×10⁻⁴	1.60×10⁻⁵	3.19×10⁻³
	1,1-二氯乙烯	7.74	6.67×10⁻²	16.30	0.22	1.87×10⁻⁴	0.46
	反式1,2-二氯乙烯	2.07×10⁻²	3.33×10⁻⁴	0.13	1.63×10⁻³	2.62×10⁻⁵	1.05×10⁻²
	顺式1,2-二氯乙烯	2.10	3.33×10⁻⁴	9.33	0.17	2.62×10⁻⁵	0.74
	三氯乙烯	0.72	3.33×10⁻³	5.00	6.65×10⁻²	3.09×10⁻⁴	0.46
氯代烷烃	一氯甲烷	6.58×10⁻²	3.33×10⁻³	8.33×10⁻²	1.80×10⁻³	9.12×10⁻⁵	2.28×10⁻³
	二氯甲烷	8.33×10⁻³	3.33×10⁻⁴	2.97×10⁻²	2.45×10⁻⁴	9.80×10⁻⁶	8.72×10⁻⁴
	三氯甲烷	16.61	3.33×10⁻⁴	6.63×10⁻²	0.94	1.88×10⁻⁵	37.37
	四氯化碳	3.87×10⁻²	3.33×10⁻³	0.14	3.87×10⁻³	3.33×10⁻⁴	1.40×10⁻²
	二氯乙烷	1.30	3.33×10⁻⁴	30.40	4.53×10⁻²	1.16×10⁻⁵	1.06
	1，2-二氯丙烷	0.11	3.33×10⁻²	1.12	7.40×10⁻³	2.20×10⁻³	7.37×10⁻²
氯醚	1,1-二氯乙醚	1.29	0.33	2.30	1.91×10⁻²	4.93×10⁻³	3.40×10⁻²
	1,2-二氯乙醚	5.00×10⁻³	3.33×10⁻⁴	9.33	1.04×10⁻⁵	6.94×10⁻⁷	1.94×10⁻²
	1,1,1-三氯乙醚	5.66	0.50	12.60	7.45×10⁻³	6.59×10⁻⁴	1.66×10⁻²
有机氯农药	丙环唑	1.33×10⁻³	3.33×10⁻⁴	8.33×10⁻³	2.13×10⁻⁷	5.32×10⁻⁸	1.33×10⁻⁶
	氯菊酯	1.67×10⁻³	3.33×10⁻⁴	2.03×10⁻²	1.41×10⁻⁷	2.82×10⁻⁸	1.72×10⁻⁶
	异丙二酮	3.33×10⁻⁴	3.33×10⁻⁴	4.33×10⁻³	6.21×10⁻⁸	6.21×10⁻⁸	8.07×10⁻⁷
	滴滴涕	3.33×10⁻⁴	3.33×10⁻⁴	3.33×10⁻³	4.54×10⁻⁸	4.54×10⁻⁸	4.54×10⁻⁷
氯有机盐	氯多氟烷基醚磺酸盐F-53B	5.20×10⁻²	6.67×10⁻³	0.17	4.36×10⁻⁷	5.59×10⁻⁸	1.40×10⁻⁶
氟氯烃	二氯二氟甲烷	9.17×10⁻²	3.33×10⁻⁴	0.23	6.76×10⁻³	2.46×10⁻⁵	1.72×10⁻²

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