短链氯化石蜡分析方法、环境行为与健康效应的研究进展

吴静; 于海斌; 张静星; 郑晓燕; 袁懋

doi:10.13198/j.issn.1001-6929.2021.12.06

短链氯化石蜡分析方法、环境行为与健康效应的研究进展

doi: 10.13198/j.issn.1001-6929.2021.12.06

中国环境监测总站, 北京　100012

基金项目: 国家自然科学基金项目(No.41101476)

详细信息

作者简介:
吴静(1989-)，女，山东日照人，工程师，博士，主要从事新污染物的环境行为研究，wujing@cnemc.cn

通讯作者:
袁懋(1974-)，男，吉林公主岭人，正高级工程师，博士，主要从事环境监测分析技术研究，yuanmao@cnemc.cn

中图分类号: X132
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出版历程
- 收稿日期: 2021-08-19
- 修回日期: 2021-11-25
- 网络出版日期: 2022-03-07

Research Process on Analytical Methods, Environmental Behavior and Health of Short-Chain Chlorinated Paraffins

China National Environmental Monitoring Centre, Beijing 100012, China

Funds: National Natural Science Foundation of China (No.41101476)

摘要

摘要: 氯化石蜡(chlorinated paraffins, CPs)是我国目前广泛应用在工业生产中的阻燃剂和增塑剂，其中短链氯化石蜡(short chain chlorinated paraffins, SCCPs)作为新污染物，因具有持久性、高毒性、长距离迁移特性和生物蓄积性等持久性有机污染物(persistent organic pollutants, POPs)特性引起了国内外的关注，尤其是SCCPs的环境赋存对环境健康的危害亟需进一步研究. 国内对SCCPs的研究集中在分析方法与环境行为等方面，对SCCPs的环境健康效应研究较少. 本文总结了近年来SCCPs分析方法的研究进展，并对其环境健康效应进行了梳理. 结果表明，SCCPs已被证实具有潜在的毒性效应，并且随着时间的推移，SCCPs在环境介质中的暴露浓度越来越高，因此SCCPs的环境外暴露对人体健康的潜在威胁越来越大. 研究显示，我国尚未停止SCCPs的生产与使用，因此在我国“十四五”规划之际，应加快SCCPs分析方法的研究进程，利用高分辨质谱将SCCPs的分析方法规范与标准化，并且在研究SCCPs的环境行为、迁移转化机制与毒性效应的基础上，深入开展SCCPs人体暴露风险与健康效应评估的研究，建立有效的环境健康风险评价模型与机制.
- 短链氯化石蜡 /
- 新污染物 /
- 分析方法 /
- 环境健康
Abstract: Chlorinated paraffins (CPs) are widely used as flame retardant and plasticizer. As new organic pollutants, short chain chlorinated paraffins (SCCPs) have attracted tremendous attention due to their persistence, chronic toxicity, long-range transport potential and bioaccumulation potential. In particular, their potential impact on environmental health requires further study. However, so far, the research on SCCPs has mostly focused on their analytical methods and environmental behavior, while research on their environmental health effects is scarce. This paper reviews the development of analytical methods of SCCPs and thoroughly analyzes the environmental health effects of SCCPs. SCCPs have posed increasingly potential threats to human health with their rising environmental concentrations. However, China has no control policies on the production and usage of SCCPs. Therefore, by the time of the ‘14th Five-Year Plan’, it is vital for us to accelerate the research process of SCCP analytical methods and to further investigate the environmental behavior, migration and transformation, and toxicity effects of SCCPs, so that we will be able to provide related reference and build a solid foundation for health risk assessment model and mechanism of SCCPs．
- short chain chlorinated paraffins (CPs) /
- new organic pollutants /
- analytical method /
- environmental health

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表 1 SCCPs的常见分析方法特征

Table 1. Common analytical methods of SCCPs

分析方法	检出限	适用范围	优点	缺点	数据来源
气相色谱-电子捕获检测器(GC-ECD)法	4~15 ng/mL	氯代化合物	对卤代化合物有较高的特异灵敏响应	缺乏选择性，易受到其他电负性强的共存污染物干扰	文献[12]
全二维气相色谱-微电子捕获器(GC×GC-μECD)法	1~5 ng/mL	卤代化合物等	灵敏度高，操作便捷	无法完全去除MCCPs的干扰，并且无法对MCCPs进行准确定量	文献[12]
气相色谱仪-火焰离子化检测器(GC-FID)法	10 mg/kg	非极性化合物	操作便捷	无法去除萃取液中直链烷烃的干扰	文献[18]
碳骨架色谱-火焰离子化检测器(carbon skeleton chromatography-FID)法	0.6 mg/kg	非极性化合物	操作便捷，可获得CPs碳链长度组成的信息	无法分析CPs单体的氯化信息	文献[19]
液相色谱-大气压化学电离源质谱(LC-MS/APCI)法	1~2 ng/μL	非极性与半极性化合物	响应良好	无法去除基质干扰效应	文献[19]
气相色谱-电子捕获负离子源-质谱(GC-ECNI-MS)法	0~60 pg/μL	卤代化合物等	操作便捷，普适性强	无法完全去除MCCPs的干扰	文献[8]
气相色谱-串联高分辨四级杆飞行时间质谱(GC-QTOF-HRMS)法	24~81 ng/mL	卤代化合物等	较高的质量分辨率与质量精度，可降低基质干扰效应，数据处理便捷	价格高，普及性低	文献[16]
全二维气相色谱-串联高分辨四级杆飞行时间质谱(GC×GC-QTOF-HRMS)法	20 pg/μL	卤代化合物等	较高的质量分辨率与质量精度，可降低基质干扰效应，数据处理便捷	价格高，普及性低	文献[17]

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表 2 SCCPs暴露的毒性效应汇总

Table 2. Summary of the exposed toxic effects of SCCPs

暴露对象	无可见效应浓度 (NOEC)	最低观察效应水平 (LOEC)	暴露时间	暴露剂量	病理现象	数据来源
虹鳟鱼幼鱼	—	0.79~5.5 μg/g	85 d	920 ng/g C₁₀H_{15. 3}Cl_{6. 7}或5500 ng/g C₁₁H_{18. 4}Cl_{5. 6}	出现严重的肝脏组织病理学反应，包括大范围的纤维损害和肝脏细胞坏死，未观察到对甲状腺的损害	文献[29]
非洲爪蟾胚胎	0~0.5 mg/L	0.5 mg/L(生物化学反应)；50 mg/L(畸形发育)	96 h	5~50 mg/L	观察到发育畸形现象	文献[30]
非洲爪蟾胚胎	0~0.5 mg/L	0.5 mg/L(生物化学反应)；50 mg/L(畸形发育)	96 h	500 mg/L	胚胎出现了11%的死亡，存活胚胎中出现50%的畸形现象	文献[30]
日本青鳉晶胚	9.6 μg/L	55~460 μg/L	40 d	1.5×10⁻³、15×10⁻³ μg/g	促使青鳉鱼卵黄囊增大，使其昏睡或无运动特征	文献[31]
斑马鱼胚胎	—	—	48 h	1 000、10 000 μg/L	可显著抑制胚胎48 h (受精后的时间)的孵化过程	文献[32-35]
斑马鱼胚胎	—	—	96 h	10 000 μg/L	导致斑马鱼胚胎死亡率升高	文献[32-33]
仓鼠卵巢细胞	—	39.7×10⁹~397×10⁹(雌激素与抗雌激素效应)；2.69×10⁻⁹ (雌激素受体α)；269×10⁻⁹ (糖皮质激素受体介导)	24、48 h	40.40%氯含量的C₁₀-CPs； 66.10%氯含量的C₁₀-CPs； 43.20%氯含量的C₁₁-CPs ；	均具有雌激素效应. 这3种SCCPs均没有表现出甲状腺受体β的拮抗作用，此外，C₁₀-CPs (氯含量为66.10%)和C₁₁-CPs (氯含量为43.20%)两种SCCPs的暴露会导致H295R癌细胞株中的皮质醇增加	文献[34]
人体肝癌细胞HepG2	—	—	24、48 h	0、1、10、100 μg/L	细胞在糖代谢、氨基酸代谢和脂肪酸代谢方面发生不同程度的紊乱；同时，SCCPs的暴露使饱和脂肪酸代谢紊乱，使不饱和脂肪酸水平上调	文献[35]

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表 3 我国环境介质中CPs在人体内的暴露浓度

Table 3. Summary of CP concentrations in different matrices which posed exposure risks for human in China

研究区域	时间	样品类型(单位)	化合物	平均值	中间值	最小值	最大值	数据来源
18个省份	2011年	食物 (ng/g，以湿质量计)	SCCPs	1 472		215	4 200	文献[48]
18个省份	2011年	食物 (ng/g，以湿质量计)	MCCPs	80.5		9.0	586	文献[48]
20个省份	2011年	肉类食物 (ng/g，以湿质量计)	SCCPs	129		15.7	469	文献[49]
20个省份	2011年	肉类食物 (ng/g，以湿质量计)	MCCPs	5.7		0.3	23.8	文献[49]
北京市	2016年	饮用水/(ng/L)	SCCPs	23.0	23.0	20.0	26.0	文献[37]
	2016年	双份饭 (ng/g，以湿质量计)	SCCPs	113	79.3	24.4	546	文献[37]
	2016年	双份饭 (ng/g，以湿质量计)	MCCPs	82.2	40.5	17.3	384	文献[37]
	2014—2015年	牛奶 (ng/g，以湿质量计)	SCCPs	18.3	18.1	16.2	20.5	文献[37]
		牛奶 (ng/g，以湿质量计)	MCCPs	14.2	17.6	1.70	23.3	文献[37]
		室内空气(ng/m³)	SCCPs	181	71.9	9.77	966	文献[37]
		室内空气(ng/m³)	MCCPs	41.9	3.47	<LOD (检出限)	613	文献[37]
		室内灰尘(ng/g)	SCCPs	148	98.7	5.35	1 022	文献[37]
		室内灰尘(ng/g)	MCCPs	139	89.8	2.10	725	文献[37]
北京市	2013—2014年	室内空气(μg/m³)	SCCPs			0.06	1.35	文献[39]
12个省份	2007年	城市母乳 (ng/g，以脂质量计)	SCCPs	1 300	681	170	6 150	文献[43]
12个省份	2007年	城市母乳 (ng/g，以脂质量计)	MCCPs	99.6	60.4	18.7	350	文献[43]
16个省份	2011年	城市母乳 (ng/g，以脂质量计)	SCCPs	2 280	733	131	16 100	文献[44]
16个省份	2011年	城市母乳 (ng/g，以脂质量计)	MCCPs	233	137	22.3	1 501	文献[44]
8个省份	2007年	农村母乳 (ng/g，以脂质量计)	SCCPs	571.75	303	68	1 580	文献[44]
8个省份	2007年	农村母乳 (ng/g，以脂质量计)	MCCPs	50.73	35.7	9.05	139	文献[44]
16个省份	2011年	农村母乳 (ng/g，以脂质量计)	SCCPs	606.59	360	65.6	2 310	文献[44]
16个省份	2011年	农村母乳 (ng/g，以脂质量计)	MCCPs	52.65	45.4	9.51	146	文献[44]

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