我国氯化石蜡的环境赋存、人群暴露与管控：现状及展望

宋博宇; 白露; 黎娟; 高鹏; 张彩丽; 高洁玉; 王亚韡

doi:10.13198/j.issn.1001-6929.2022.06.27

我国氯化石蜡的环境赋存、人群暴露与管控：现状及展望

doi: 10.13198/j.issn.1001-6929.2022.06.27

宋博宇^1,,
白露^{2, 3, 4},
黎娟³,
高鹏¹,
张彩丽¹,
高洁玉¹,
王亚韡^{2, 3, 4}

1.
生态环境部对外合作与交流中心，北京　100035
2.
国科大杭州高等研究院，浙江杭州　310000
3.
中国科学院生态环境研究中心，环境化学与生态毒理学国家重点实验室，北京　100085
4.
中国科学院大学，北京　100049

基金项目: 国家自然科学基金项目(No.21625702, 22136006, 22021003)

详细信息

作者简介:
宋博宇（1988-），男，吉林公主岭人，高级工程师，硕士，主要从事POPs控制技术与管理政策研究，song.boyu@fecomee.org.cn

中图分类号: X503
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出版历程
- 收稿日期: 2022-04-14
- 修回日期: 2022-06-20

Occurrence, Population Exposure and Control of Chlorinated Paraffins in China: Current Situation and Prospect

SONG Boyu^1
,,
BAI Lu^{2, 3, 4},
LI Juan³,
GAO Peng¹,
ZHANG Caili¹,
GAO Jieyu¹,
WANG Yawei^{2, 3, 4}

1.
Foreign Economic Cooperation Office, Ministry of Ecology and Environment, Beijing 100035, China
2.
Hangzhou Institute for Advanced Study, UCAS, Hangzhou 310000, China
3.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
4.
University of Chinese Academy of Sciences, Beijing 100049, China

Funds: National Natural Science Foundation of China (No.21625702, 22136006, 22021003)

摘要

摘要: 氯化石蜡(Chlorinated paraffin，CPs)是一类人工合成化学品，被广泛用作阻燃剂和增塑剂，在生产和使用过程中释放到多种环境介质中(如水、沉积物、灰尘、空气和土壤等). 短链氯化石蜡(SCCPs)作为新增持久性有机污染物已于2017年被正式列入《关于持久性有机物的斯德哥尔摩公约》附件A中，中链氯化石蜡(MCCPs)因具有和SCCPs相似的性质和环境效应，已被列入持久性有机污染物候选名单. 我国是CPs的生产和使用大国，但对该类物质的风险评估与管控还存在不足. 本文通过收集并深入讨论已发表的CPs相关文章，在系统梳理不同介质中CPs赋存情况的基础上，利用释放因子解析方法，估算了CPs在生产和使用过程中进入到环境的量，发现土壤介质是环境中CPs的汇. 人类活动、经济活动和经济水平等对CPs在不同区域的赋存具有重要影响. 对人群暴露途径解析表明，职业暴露场景显著高于其他场景；生态风险和人体暴露风险评估表明，目前CPs对我国生态环境与人体健康的危害整体上还处于较低水平. 另外，本文介绍了国内外对于SCCPs和MCCPs的管控措施，并基于化学品管理和风险评估的考虑，提出未来亟需深入开展MCCPs和LCCPs (长链氯化石蜡)的迁移转化和风险研究，特别是评估CPs管控造成的潜在经济、社会和环境影响. 相关数据及分析可更好地为CPs产品的管控和国家开展履约行动提供科学数据和技术支撑，并为将来可能的CPs淘汰政策的制定提供参考.
- 氯化石蜡 (CPs) /
- 排放清单 /
- 健康风险 /
- 化学品管控
Abstract: Chlorinated paraffins (CPs) are synthetic chemicals, widely used as flame retardants and plasticizers. CPs can be released into various environmental media, such as water, sediment, dust, air, and soil. Short-chain CPs (SCCPs). were officially listed in Annex A of the Stockholm Convention as new persistent organic pollutants (POPs) in 2017, and medium-chain CPs (MCCPs) were included POPs candidates by the Convention due to their persistence, bioaccumulations, long range atmospheric transport and adverse effects on ecosystem and organisms. As the major global producer and consumer of CPs, China is facing a huge environmental burden from these compounds. There is a great demand for CPs control and risk assessment, however, there are still many defects in basic research in this field. Based on the in-depth discussion of published related studies, this study estimates the emission of CPs to the environment through production and use, sorts out the occurrence of CPs in different environmental media, and looks forward the possible gap between the research and the chemical managements. The key findings from this review are that: (1) Soil is the sink of CPs in the environment; (2) Human activities, economic activities and economic level have important impacts on the occurrence of CPs in different regions; (3) The risk assessment indicates that ecological risk and human exposure risk of CPs at present levels are relatively low. Furthermore, this study introduces the control measures of SCCPs and MCCPs at home and abroad. In view of the consideration of chemical management and risk assessment, there is urgent need to carry out research on the migration, transformation, and exposure risk of MCCPs and LCCPs, especially to assess the potential economic, social, and environmental impact ascribed to the control management of CPs. This critical review provides important scientific data and technical support for the control of CPs products and national implementation of the Stockholm Convention. Moreover, this study will provide solid support for the risk assessment and possible control management of CPs in China.
- chlorinated paraffin /
- emission inventory /
- health risks /
- chemical control

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图 1 2019年中国SCCPs和MCCPs从生产、使用到排放的质量平衡分析

Figure 1. Mass balance of SCCPs and MCCPs in China from production, use to emission in 2019

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图 2 CPs的生命周期

Figure 2. The CPs life cycle

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图 3 国际CPs管控进程时间轴

Figure 3. Timeline of international control process of CPs

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表 1 不同环境介质中CPs的含量

Table 1. CPs concentration in different environmental media

地区	时间	样品类别	单位	SCCPs含量		MCCPs含量		数据来源
地区	时间	样品类别	单位	中间值	范围	中间值	范围	数据来源
中国18个城市	2008年	气相	ng/m³	116	13.5~517	—	—	文献[12]
中国山东省	2016年	气相	ng/m³	—	98~988	—	—	文献[11]
印度	2006年	气相	ng/m³	10.2	<2.65~47.4	3.62	<1.8~38.2	文献[13]
日本	2008年	气相	ng/m³	1.19	0.28~14.2	—	—	文献[12]
韩国	2008年	气相	ng/m³	1.12	0.60~8.96	—	—	文献[12]
瑞士	2011年	气相	ng/m³	4.3	1.8~17	—	—	文献[14]
巴基斯坦	2011年	气相	ng/m³	5.13	<2.65~14.2	4.21	<1.8~9.45	文献[13]
瑞士	2013年	气相	ng/m³	2.7	1.1~42	—	—	文献[14]
挪威	2013—2014年	气相	ng/m³	9.6	1.7~54	1.2	<0.35~13	文献[15]
中国10个城市	2013—2014年	颗粒相	ng/m³	19.9	1.98~274	15.6	1.27~312	文献[16]
中国山东省	2016年	颗粒相	ng/m³	—	32~454	—	—	文献[11]
中国北京市	2016年	颗粒相	ng/m³	14.9	9.2~19.6	1.7	0.6~2.7	文献[17]
中国北京市	2016年	河流	ng/L	456	77~652	—	—	文献[18]
中国北京市	2016年	湖泊	ng/L	124	<18~377	—	—	文献[18]
中国上海市	2016年	河流	ng/L	278	15.0~1 640	939	40.3~3 870	文献[19]
美国	2000—2004年	河流	ng/L	1.194	0.606~1.935	0.0074	<0.000 5~0.047	文献[20]
法国	2015年	河流	ng/L	—	<50~200	—	—	文献[21]
中国31个省份	2016年	土壤	ng/g¹⁾	374	39~1 609	860	127~1 969	文献[22]
中国台州市	2017年	土壤	ng/g¹⁾	—	68.5~2.20×10⁵	—	507~4.40×10⁶	文献[23]
中国江苏省	2018年	土壤	ng/g¹⁾	154	37.5～995.7	121	15.1~739.6	文献[24]
挪威	2008年	土壤	ng/g¹⁾	22	<0.6~490	—	—	文献[25]
英国	2008年	土壤	ng/g¹⁾	50	<0.8~570	—	—	文献[25]
瑞士	1989—2014年	土壤	ng/g¹⁾	—	3.0~35	—	5.1~160	文献[26]
中国山东省	2009年	河流沉积物	ng/g¹⁾	160	8.4~2 000	360	1.8~3 200	文献[27]
中国山东省	2009年	海洋沉积物	ng/g¹⁾	11.0	5~22	9.0	6~63	文献[27]
中国珠三角地区	2013年	海洋沉积物	ng/g¹⁾	173	46.3~1 540	868	102~6 650	文献[28]
中国深圳市	2013年	海洋沉积物	ng/g¹⁾	401	14.7~574	541	10.9~2 500	文献[28]
中国香港	2013年	海洋沉积物	ng/g¹⁾	12.2	<0.6~75.9	12.5	<1.0~286	文献[28]
中国上海市	2016年	河流沉积物	ng/g¹⁾	89.3	<1.70~2 020	947	10.1~10 800	文献[19]
西班牙	2003年	海洋沉积物	ng/g¹⁾	0.46	0.21~2.09	—	—	文献[29]
日本	2013年	海洋沉积物	ng/g¹⁾	8.0	1.3~27.4	16.6	3.2~56.8	文献[28]
注：1)表示以干质量计.

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表 2 CPs在母乳及血液中的暴露浓度

Table 2. Exposure concentration of CPs in breast milk and blood

地区	时间	样品类别	单位	SCCPs含量		MCCPs含量		LCCPs含量		数据来源
地区	时间	样品类别	单位	中间值	范围	中间值	范围	中间值	范围	数据来源
中国11个省份	2017年	城市母乳	ng/g¹⁾	393	131~808	494.5	94~1 714	—	—	文献[58]
中国11个省份	2017年	农村母乳	ng/g¹⁾	478.5	139~1 543	572	211~1 089	—	—	文献[58]
中国12个省份	2007年	城市母乳	ng/g¹⁾	681	170~6 150	60.4	18.7~350	—	—	文献[59]
中国8个省份	2007年	农村母乳	ng/g¹⁾	303	68~1 580	35.7	9.05~139	—	—	文献[60]
中国16个省份	2011年	城市母乳	ng/g¹⁾	733	131~16100	137	22.3~1 501	—	—	文献[59]
中国16个省份	2011年	农村母乳	ng/g¹⁾	360	65.6~2 310	45.4	9.51~146	—	—	文献[60]
中国北京市	2007—2009年	城市母乳	ng/g¹⁾	28	<20~54	—	—	—	—	文献[61]
中国绍兴市	2010年	城市母乳	ng/g¹⁾	37.9	<12~124	121	38~187	14.6	4.90~184	文献[62]
中国上海市	2015—2016年	城市母乳	ng/g¹⁾	35.0	<12~676	70.1	38~1 260	10.5	<1.1~56.9	文献[62]
中国嘉兴市	2015—2016年	城市母乳	ng/g¹⁾	28.6	<12~642	63.0	<16~547	5.23	<1.1~18.4	文献[62]
中国绵阳市	2018年	城市母乳	ng/mL	82.6	29.2~271	26.1	11.0~164	—	—	文献[63]
英国	2001—2002年	母乳	ng/g¹⁾	180	<80~820	21.0	6.2~320	—	—	文献[64]
日本	2007—2010年	母乳	ng/g¹⁾	<20	<20	—	—	—	—	文献[61]
韩国	2007—2010年	母乳	ng/g¹⁾	<20	<20	—	—	—	—	文献[61]
瑞典	2011年	母乳	ng/g¹⁾	15.6	<12~24.1	37.3	<16~77.7	4.28	<1.1~21.4	文献[62]
挪威	2014年	母乳	ng/g¹⁾	10.2	<12~120	43.1	<16~311	4.26	<1.1~29.0	文献[62]
瑞典	2016年	母乳	ng/g¹⁾	<12	<12~27.8	21.0	<16~60.0	2.80	<1.1~9.34	文献[62]
中国深圳市	2012年	全血	ng/g²⁾	98	14~3500	21	6.3~320	4.5	1.0~21	文献[65]
中国北京市	2013年	母体血清	ng/g²⁾	113	21.7~373	11	3.76~31.8	—	—	文献[66]
中国北京市	2013年	脐带血清	ng/g²⁾	24	8.51~107	3.89	1.33~12.9	—	—	文献[66]
中国大连市	2015年	血浆	ng/g²⁾	26	<12.6~203	—	—	—	—	文献[67]
中国武汉市	2015—2016年	母体血清	ng/mL	66	15.9~584	126	29.3~1 006	—	—	文献[26]
中国武汉市	2015—2016年	脐带血清	ng/mL	37	8.46~223	34.2	13.6~90.1	—	—	文献[26]
中国广州市	2016—2017年	母体血浆	ng/mL	5.93	3.28~10.4	2.88	1.30~5.50	—	—	文献[68]
中国广州市	2016—2017年	脐带血浆	ng/mL	2.65	0.89~4.13	1.18	0.89~1.69	—	—	文献[68]
中国广州市	2018年	血清	ng/mL	1.7	1.0~5.5	1.6	<1.0~2.7	—	—	文献[69]
中国绵阳市	2018年	母体血清	ng/mL	202	51.0~620	57.8	17.4~225	—	—	文献[63]
中国绵阳市	2018年	脐带血清	ng/mL	88.0	13.3~242	26.6	11.9~67.8	—	—	文献[63]
中国济南市	2018—2019年	血清	ng/g²⁾	107	24.2~384	134	23.8~371	—	—	文献[70]
澳大利亚	2002—2015年	血清	ng/g²⁾	0.56	<0.13~0.68	1.0	<0.12~3.1	—	—	文献[71]
注：1)表示以脂质量计；2)表示以湿质量计.

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表 3 CPs的国内外管控措施

Table 3. Management and control of CPs at home and abroad

资料来源	限制条件
欧盟《持久性有机污染物法规》(EU)2019/1021	继续允许生产、投放市场和使用含有SCCPs质量分数低于1%(质量)的物质或混合物或含有浓度低于0.15%(质量)的SCCPs的消费产品；允许使用采矿业中的传送带和2015年12月4日或之前已使用的SCCPs大坝密封剂，以及2012年7月10日或之前已使用的除上述以外含SCCPs的物品
欧盟REACH法规SVHC清单	物品中含有的SCCPs、MCCPs浓度超过0.1%，欧盟生产商或进口商应履行法规规定的告知或通报等义务
欧盟2022年第10次联合执法行动	重点检查REACH法规和POPs法规相关有害物质限制的合规性
挪威《消费性产品中禁用特定有害物质》PoHS	考虑到SCCPs已经被限制，PoHS增加了消费品MCCPs不超过0.1%的限制
加拿大环境保护法(CEPA)	将SCCP列入首要的控制物质清单
美国环境保护局(US EPA)	将SCCP列入TRI (Toxic Release Inventory)有毒物质排放清单
OEKO-TEX STANDARD 100^®及LEATHER STANDARD by OEKO-TEXR^®	SCCPs或MCCPs含量小于10 mg/kg，CPs总量小于50 mg/kg
欧盟RoHS指令	均质材料中，MCCPs浓度不得超过0.1%(质量)
中国重点管控新污染物清单(2021版)	自2024年1月1日起，SCCPs禁止生产、使用和进出口，以下用途除外：在天然及合成橡胶工业中生产传送带时使用的添加剂；采矿业和林业使用的橡胶输送带的备件；皮革业，尤其是皮革加脂；润滑油添加剂，尤其用于汽车、发电机和风能设施的发动机以及油气勘探钻井和生产柴油的炼油厂；户外装饰灯管；防水和阻燃油漆；黏合剂；金属加工；柔性聚氯乙烯的第二增塑剂(但玩具及儿童产品中的使用除外). 废弃的SCCPs应当按照危险废物实施环境管理

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