洪泽湖水体全氟化合物的污染特征、来源及健康风险

黄家浩; 陶艳茹; 黄天寅; 李则婵; 陈书琴; 庞燕

doi:10.13198/j.issn.1001-6929.2022.12.09

洪泽湖水体全氟化合物的污染特征、来源及健康风险

doi: 10.13198/j.issn.1001-6929.2022.12.09

黄家浩^{1, 2,},
陶艳茹¹,
黄天寅²,
李则婵³,
陈书琴³,
庞燕^1, ,

1.
中国环境科学研究院，国家环境保护湖泊污染控制重点实验室，湖泊水污染治理与生态修复技术国家工程实验室，北京　100012
2.
苏州科技大学环境科学与工程学院，江苏苏州　215009
3.
安庆师范大学资源环境学院，安徽安庆　246133

基金项目: 国家重大研发计划项目 (No.2022YFC3204105)

详细信息

作者简介:
黄家浩（1997-），男，江苏苏州人，硕士，主要从事新型持久性有机污染物研究，676856298@qq.com

通讯作者:
庞燕(1970-)，女，山西榆次人，研究员，主要从事湖泊水污染防治研究，pangyan@craes.org.cn

中图分类号: X524
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出版历程
- 收稿日期: 2022-08-12
- 修回日期: 2022-12-05

Occurrence, Sources and Health Risk Assessment of Per- and Polyfluoroalkyl Substances in Surface Water of Hongze Lake

1.
National Engineering Laboratory for Lake Pollution Control and Ecological Restoration, State Environment Protection Key Laboratory for Lake Pollution Control, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
2.
School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China
3.
Resource and Environment College, Anqing Normal University, Anqing 246133, China

Funds: National Key Research and Development Program of China (No.2022YFC3204105)

摘要

摘要: 洪泽湖是南水北调东线工程重要调蓄湖泊，为了解洪泽湖表层水中全氟和多氟烷基化合物(PFASs)的污染状况，通过超高效液相色谱串联四极杆质谱测定了湖区和入湖河流的表层水15种PFASs的含量，分析比较了不同区域水体中PFASs的浓度与组成，运用HCA法解析了不同污染来源，并应用HQ法对不同人群的健康风险进行评价. 结果表明：①洪泽湖表层水中检出15种PFASs，ΣPFASs浓度为63.4～218.0 ng/L(中位值92.9 ng/L)，健康风险较低；②PFASs组分以短链为主，主要污染物为PFPeA，占60.8%；③PFASs在洪泽湖的空间分布呈现由南向北递减的趋势，洪泽湖湖心及过水通道区的PFASs浓度较高；④HCA方法表明，洪泽湖表层水中PFASs主要来自地表径流、橡胶品制造、食品包装和纸类表面处理的工业排放、纺织和金属电镀工业排放和生活污水. 研究显示，洪泽湖表层水中广泛存在多种PFASs，以短链为主，健康风险对居民来说可接受.
- 洪泽湖 /
- 全氟化合物 /
- 污染特征 /
- 来源解析 /
- 健康风险
Abstract: Hongze Lake is an important regulation and storage lake for the eastern route of the South-to-North Water Transfer Project. To understand the pollution status of per- and polyfluoroalkyl substances (PFASs) in the surface water of Hongze Lake, the concentrations of 15 kinds of PFASs in the surface water of the lake area and the rivers entering the lake were determined by ultra-high performance liquid chromatography-tandem quadrupole mass spectrometry. The concentrations and composition of PFASs in different regions were analyzed and compared, and different pollution sources were analyzed by the HCA method. The HQ method was used to evaluate the health risk of different populations. The results showed that: (1) 15 kinds of PFASs were detected in the surface water of Hongze Lake, the concentration of ΣPFASs ranged from 63.4 to 218.0 ng/L (median value was 92.9 ng/L), indicating low health risk. (2) The PFAS components were mainly short chain, and the main pollutant was PFPeA, accounting for 60.8%. (3) The spatial distribution of PFASs in Hongze Lake showed a decreasing trend from south to north, and the concentration of PFASs in the center of Hongze Lake and the water passage area was higher. (4) The HCA method showed that the PFASs in the surface water of Hongze Lake mainly came from surface runoff, industrial discharges from rubber manufacturing, food packaging and paper surface treatment, textile and metal electroplating industrial discharges, and domestic sewage. The research showed that there are many types of PFASs in the surface water of Hongze Lake, mainly in short chain, and the health risk are acceptable to the residents.
- Hongze Lake /
- per- and polyfluoroalkyl substances /
- occurrence characteristics /
- source analysis /
- health risk

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图 1 洪泽湖采样点示意

Figure 1. Location of sampling sites in Hongze Lake

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图 2 洪泽湖表层水中PFASs的组成占比

Figure 2. Composition proportion of PFASs in surface water

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图 3 洪泽湖表层水中PFASs的聚类分析热图

Figure 3. Heat map of PFASs in surface water around Hongze Lake

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图 4 洪泽湖周围表层水中主要PFASs浓度的空间分布

Figure 4. Spatial distribution of concentrations of main PFASs (PFBA, PFPeA, PFOA) in surface waters around Hongze Lake

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图 5 洪泽湖表层水中PFASs在高暴露情景时的健康风险评估结果

Figure 5. Health risk assessment of PFASs in the high exposure scenario

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表 1 表层水中15种目标PFASs的方法检出限和回收率

Table 1. Method detection limits and recoveries of PFASs in the surface water samples

分析物	检出限/(ng/L)	回收率/%
全氟丁酸 (PFBA，C₄)	0.987	87.7
全氟戊酸(PFPeA，C₅)	0.062	74.5
全氟己酸(PFHxA，C₆)	0.007	92.8
全氟庚酸(PFHpA，C₇)	0.020	83.5
全氟辛酸(PFOA，C₈)	0.008	104.0
全氟壬酸(PFNA，C₉)	0.005	94.3
全氟癸酸(PFDA，C₁₀)	0.041	92.6
全氟十一酸(PFUnA，C₁₁)	0.025	75.8
全氟十二酸(PFDoDA，C₁₂)	0.012	90.5
全氟十三酸(PFTrA，C₁₃)	0.082	72.7
全氟十四酸(PFTeA，C₁₄)	0.081	66.2
全氟丁基磺酸(PFBS，C₄)	0.211	74.6
全氟己基磺酸 (PFHxS，C₆)	0.100	95.3
全氟辛基磺酸(PFOS，C₈)	0.015	90.2
全氟癸烷磺酸(PFDS，C₁₀)	0.044	64.8

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表 2 我国不同年龄/性别组的平均体重(BW)、饮用水摄入量(DWI)和PFASs每日可接受摄入量(ADI)^[25]

Table 2. Mean body weight (BW), the quantity of drinking water intake (DWI), and the acceptable daily intake of PFASs values (ADI) for different age/gender groups in China

年龄	性别	BW/kg	DWI/(L/d)
3～6岁	男性	19.63	1.08
3～6岁	女性	18.65	1.08
7～11岁	男性	33.84	1.24
7～11岁	女性	31.94	1.24
12～16岁	男性	55.16	1.73
12～16岁	女性	49.44	1.73
17～19岁	男性	63.43	2.26
17～19岁	女性	52.67	2.26
20～24岁	男性	67.20	2.81
20～24岁	女性	53.80	2.81
25～59岁	男性	70.77	2.81
25～59岁	女性	58.37	2.81
>60岁	男性	67.10	2.81
>60岁	女性	59.45	2.81

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表 3 洪泽湖表层水中PFASs的浓度

Table 3. PFASs concentration in the surface water of Hongze Lake ng/L

采样点编号	PFBA	PFPeA	PFHxA	PFHpA	PFOA	PFNA	PFDA	PFUnDA
1	18.2	47.6	4.43	4.54	14.2	1.88	0.241	0.133
2	37.5	45.5	4.64	4.28	18.4	1.70	0.220	0.036
3	18.5	89.7	7.12	3.12	8.98	1.15	0.136	nd
4	12.3	58.9	4.70	3.30	9.30	1.17	0.125	nd
5	17.8	102.5	8.06	3.45	15.5	1.08	0.116	nd
6	16.4	38.7	4.34	3.41	8.90	1.07	0.121	nd
7	23.1	100.9	9.28	3.29	9.14	1.31	0.159	0.029
8	24.3	167.4	11.4	3.13	8.74	1.30	0.175	nd
9	32.5	96.3	11.1	3.16	8.20	1.17	0.125	0.048
10	16.0	57.2	6.25	2.94	8.36	1.11	0.095	nd
11	18.0	66.2	7.54	3.61	15.8	1.12	0.128	0.041
HH	14.4	161.3	11.4	3.11	16.1	1.29	0.262	nd
HHXH	7.99	32.0	3.23	3.49	15.1	1.29	0.434	0.052
LSH	13.5	33.4	4.38	4.84	12.3	1.23	0.184	nd
SH	13.9	29.0	3.51	4.31	16.8	1.58	0.183	0.076
XBH	7.84	26.9	2.68	3.09	17.0	0.89	0.157	0.243
XHH	21.1	30.7	3.59	3.75	9.61	1.25	0.199	0.039

采样点编号	PFDoDA	PFTrDA	PFTeDA	PFBS	PFHxS	PFOS	PFDS
1	nd	nd	nd	2.320	0.743	1.130	nd
2	nd	<0.0005	nd	2.640	0.902	1.610	nd
3	0.025	nd	<0.000 5	0.598	0.281	0.593	<0.000 5
4	0.015	<0.0005	nd	0.555	0.315	0.661	<0.000 5
5	nd	<0.0005	0.006	0.643	0.299	0.474	nd
6	nd	<0.000 5	0.001	0.726	0.314	0.592	<0.000 5
7	0.020	<0.000 5	0.007	0.606	0.181	0.557	<0.000 5
8	nd	<0.000 5	0.001	0.709	0.171	0.687	<0.000 5
9	0.020	<0.000 5	<0.000 5	0.594	nd	0.557	nd
10	0.181	<0.000 5	0.014	nd	0.138	0.648	0.002
11	nd	<0.000 5	0.001	0.782	0.246	0.578	<0.000 5
HH	nd	nd	nd	0.554	0.107	0.953	0.003
HHXH	0.066	nd	nd	0.660	0.442	0.971	nd
LSH	nd	<0.000 5	<0.000 5	5.230	0.889	0.702	0.002
SH	nd	<0.000 5	nd	0.793	0.280	0.770	nd
XBH	0.430	0.281	0.122	1.780	0.381	1.450	0.186
XHH	0.016	<0.000 5	nd	2.610	0.625	2.200	0.002
注：nd表示低于检出限.

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表 4 不同研究区表层水中主要PFASs比较

Table 4. Comparison of PFASs in surface water of different regions

研究区	采样日期	污染物	范围/(ng/L)	平均值/(ng/L)	数据来源
洪泽湖	2020年11月	PFPeA(C₅)	26.9~167.4	69.7	本研究
		PFBA(C₄)	7.84~37.5	18.4
		∑PFASs	63.4~217.9	114.6
骆马湖	2020年10月	PFPeA(C₅)	14.5~44	28.64	文献[33]
		PFOA(C₈)	7.6~81.34	24.69
		∑PFASs	46.09~120.33	76.35
太湖	2009年11月	PFOS(C₈)	3.6~394	26.5	文献[9]
		PFOA(C₈)	10.6~36.7	21.7
		∑PFASs	1.4~131	43.6
淮河流域	2011年3月	PFOA(C₈)	6.2~47	18	文献[15]
		PFOS(C₈)	1.4~25	4.7
		∑PFASs	11~79	28
南四湖	2013年4月	PFOA(C₈)	34.9~84.6	61.38	文献[34]
		PFHpA(C₇)	1.34~3.42	2.38
		∑PFASs	38.4~91.4	67.05
小清河	2013年6月	PFOA(C₈)	15.3~967611	101.22	文献[35]
		PFBA(C₄)	1.77~34306	89.33
		∑PFASs	32.2~1060295	165.4
白洋淀	2016年3月	PFHxS(C₆)	2.07~1688	684	文献[36]
		PFOA(C₈)	13.6~441	147
		∑PFASs	140.5~1828.5	—
长江和秦淮河南京段	2017—2018年	PFOA(C₈)	12.5~66	25.8	文献[10]
		PFHpA(C₇)	nd~237.8	—
		∑PFASs	13.8~274.6	—
韩国六大河流	2010—2012年	PFOS(C₈)	nd~15.07	3.89	文献[37]
		PFOA(C₈)	nd~8.34	2.49
		∑PFASs	1.17~40.63	10.44
南非瓦尔河	2014年9月	PFPeA(C₄)	5.7~45	25.8	文献[38]
		PFOS(C₈)	0.4~35.7	5.6
		∑PFASs	—	73.43
美国拉斯维加斯过水区	2019年1月、7月	PFHxA(C₆)	1.5~187	80.7	文献[39]
		PFPeA(C₄)	2.3~170	52.3
		∑PFASs	3.8~591	223.44
注：nd表示低于检出限，“—”表示文献中没有相关数据.

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