上海农田土壤中六溴环十二烷的赋存特征及健康风险评估

doi:10.3969/j.issn.1000-5641.2024.06.015

华东师范大学学报（自然科学版） ›› 2024, Vol. 2024 ›› Issue (6): 178-187.doi: 10.3969/j.issn.1000-5641.2024.06.015

上海农田土壤中六溴环十二烷的赋存特征及健康风险评估

杨静¹(), 邬言¹, 李月², 刘霞¹, 杨丁业¹, 陈圆圆¹, 金芮合¹, 李晔¹, 刘敏¹^,*()

1. 华东师范大学地理科学学院地理信息科学教育部重点实验室, 上海　200241
2. 华东师范大学河口海岸学国家重点实验室, 上海　200241

收稿日期:2024-07-30 接受日期:2024-09-05 出版日期:2024-11-25 发布日期:2024-11-29
通讯作者: 刘敏 E-mail:jyang@geo.ecnu.edu.cn;mliu@geo.ecnu.edu.cn
作者简介:杨　静, 女, 工程师, 研究方向为新污染物环境行为及风险评估. E-mail: jyang@geo.ecnu.edu.cn
基金资助:
国家自然科学基金 (42230505, 41730646)

Occurrence characteristics and healthy risk assessment of hexabromocyclododecane in agricultural soils in Shanghai

Jing YANG¹(), Yan WU¹, Yue LI², Xia LIU¹, Dingye YANG¹, Yuanyuan CHEN¹, Ruihe JIN¹, Ye LI¹, Min LIU¹^,*()

1. Key Laboratory of Geographic Information Science (Ministry of Education), School of Geographic Sciences, East China Normal University, Shanghai　200241, China
2. State Key Laboratory for Estuarine and Coastal Research, East China Normal University, Shanghai　200241, China

Received:2024-07-30 Accepted:2024-09-05 Online:2024-11-25 Published:2024-11-29
Contact: Min LIU E-mail:jyang@geo.ecnu.edu.cn;mliu@geo.ecnu.edu.cn

摘要/Abstract

摘要：

通过方差分析和风险商值(hazard quotient, HQ)法探究了上海34份农田土壤中六溴环十二烷(hexabromocyclododecane, HBCD)的空间分布特征和潜在健康风险. 结果表明, 所有样品中均检出了3种同系物(α-、β-和γ-HBCD), 总HBCD浓度(∑HBCDs)范围为0.30 ~ 25.41 ng/g, 算术均值为1.78 ng/g. 各采样区∑HBCDs呈现明显的空间分异特征, 其中, 宝山区和嘉定区∑HBCDs的平均浓度显著高于其他行政区(p < 0.05), 推断HBCDs主要受工业源和道路源排放的共同影响. 上海农田土壤中3种非对映异构体α-、β-和γ-HBCD占∑HBCDs的比例范围分别为2.90% ~ 73.36%、5.23% ~ 63.78%和6.95% ~ 85.46%. 91.2%的采样点处γ-HBCD占比低于商业产品中的比例, 表明这些异构体之间存在相互转化. 不同年龄人群∑HBCDs总的日暴露剂量变化范围为3.17 × 10^–4 ~ 1.57 × 10^–1 ng/(kg·d), 其中, 婴儿暴露量最高, 不同年龄人群经口摄入的日暴露剂量大于皮肤接触摄入. HQ结果表明, 当前浓度水平下所有人群总摄入量基本无风险.

关键词: 农田土壤, 六溴环十二烷, 空间分布, 健康风险评估

Abstract:

The spatial distribution characteristics and potential health risks of hexabromocyclododecane (HBCD) in 34 farmland soils in Shanghai were investigated using the variance analysis and hazard quotient (HQ) methods. Three HBCD homologs (α-, β- and γ-HBCD) were detected in all samples. The total concentration of HBCD (∑HBCDs) ranged from 0.30 to 25.4 ng/g, with an average value of 1.78 ng/g. The ∑HBCDs in agricultural soils exhibited significant spatial variation, of which Baoshan District and Jiading District had notably higher average ∑HBCDs compared to other areas (p < 0.05). It was concluded that HBCDs mainly originated from the combined influence of industrial and vehicular emissions. The proportions of α-, β- and γ-HBCD in Shanghai agricultural soils were 2.90% ~ 73.4%, 5.23% ~ 63.8%, and 6.95% ~ 85.5%, respectively. The proportion of γ-HBCD was lower in 91.2% of the sampling sites than in commercial products, indicating the presence of isomeric interconversion. Daily exposure to ∑HBCDs, combining oral and dermal ingestion, ranged from 3.17 × 10^–4 to 1.57 × 10^–1 ng/(kg·d), peaking in infants. Oral ingestion contributed more to daily exposure than dermal contact across age groups. The HQs indicated that the current HBCD concentrations posed a minimal risk to all populations.

Key words: agricultural soils, hexabromocyclododecane, spatial distribution, healthy risk assessment

中图分类号:

X830

杨静, 邬言, 李月, 刘霞, 杨丁业, 陈圆圆, 金芮合, 李晔, 刘敏. 上海农田土壤中六溴环十二烷的赋存特征及健康风险评估[J]. 华东师范大学学报（自然科学版）, 2024, 2024(6): 178-187.

Jing YANG, Yan WU, Yue LI, Xia LIU, Dingye YANG, Yuanyuan CHEN, Ruihe JIN, Ye LI, Min LIU. Occurrence characteristics and healthy risk assessment of hexabromocyclododecane in agricultural soils in Shanghai[J]. Journal of East China Normal University(Natural Science), 2024, 2024(6): 178-187.

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参考文献 25

1	CAO X, LU Y, ZHANG Y, et al.. An overview of hexabromocyclododecane (HBCDs) in environmental media with focus on their potential risk and management in China. Environmental Pollution, 2018, 236, 283- 295.
2	COVACI A, GERECKE A C, LAW R J, et al.. Hexabromocyclododecanes (HBCDs) in the environment and humans: A review. Environmental Science & Technology, 2006, 40 (12): 3679- 3688.
3	LI L, WEBER R, LIU J, et al.. Long-term emissions of hexabromocyclododecane as a chemical of concern in products in China. Environment International, 2016, 91 (5): 291- 300.
4	GAO S, WANG J, YU Z, et al.. Hexabromocyclododecanes in surface soils from e-waste recycling areas and industrial areas in South China: Concentrations, diastereoisomer-and enantiomer-specific profiles, and inventory. Environmental Science & Technology, 2011, 45 (6): 2093- 2099.
5	WU M H, HAN T, XU G, et al.. Occurrence of hexabromocyclododecane in soil and road dust from mixed-land-use areas of Shanghai, China, and its implications for human exposure. Science of the Total Environment, 2016, 559 (7): 282- 290.
6	ZHANG Y Q, LU Y L, WANG P, et al.. Transport of hexabromocyclododecane (HBCD) into the soil, water and sediment from a large producer in China. Science of the Total Environment, 2018, 610, 94- 100.
7	HUANG H L, WANG D, WAN W, et al.. Hexabromocyclododecanes in soils and plants from a plastic waste treatment area in North China: Occurrence, diastereomer-and enantiomer-specific profiles, and metabolization. Environmental Science and Pollution Research, 2017, 24 (27): 21625- 21635.
8	杨昭, 王莹莹.. 农田土壤中六溴环十二烷的污染过程以及生物修复方法研究进展. 农业环境科学学报, 2021, 40 (9): 1839- 1850.
9	WANG T, HAN SL, RUAN T, et al.. Spatial distribution and inter-year variation of hexabromocyclododecane (HBCD) and tris-(2, 3-dibromopropyl) isocyanurate (TBC) in farm soils at a peri-urban region. Chemosphere, 2013, 90 (2): 182- 187.
10	夏炎, 韩伟立, 马安德.. 广东省农耕土壤中四溴双酚A与六溴环十二烷的含量调查及其蓄积水平估算. 环境化学, 2017, 36 (6): 1328- 1334.
11	生态环境部. 环境监测分析方法标准制修订技术导则: HJ 168—2010 [S]. 北京: 中国环境出版集团, 2010.
12	国家环境保护总局. 土壤环境监测技术规范 [EB/OL]. (2004-12-19)[2024-07-02]. https://www.mee.gov.cn/image20010518/5406.pdf.
13	施旭荣. 上海市宝山区挥发性有机化合物排放治理效果评价与对策研究 [D]. 乌鲁木齐: 新疆大学, 2019.
14	TANG J F, FENG J Y, LI X H, et al.. Levels of flame retardants HBCD, TBBPA and TBC in surface soils from an industrialized region of East China. Environmental Science−Processes & Impacts, 2014, 16 (5): 1015- 1021.
15	MENG X Z, DUAN Y P, YANG C, et al.. Occurrence, sources, and inventory of hexabromocyclododecanes (HBCDs) in soils from Chongming Island, the Yangtze River Delta (YRD). Chemosphere, 2011, 82 (5): 725- 731.
16	嘉定区人民政府. 2017年上海市嘉定区国民经济和社会发展统计公报 [EB/OL]. (2018-02-11)[2024-07-02]. http://www.jiading.gov.cn/publicity/jxxgk/zdly1/ggjg/tjsj82/tjgb__publicity/fdzdgknr/tjsj97/tjgb97/93880.
17	ZHU Z C, CHEN S J, ZHENG J, et al.. Occurrence of brominated flame retardants (BFRs), organochlorine pesticides (OCPs), and polychlorinated biphenyls (PCBs) in agricultural soils in a BFR manufacturing region of North China. Science of the Total Environment, 2014, 481, 47- 54.
18	BARONTINI F, COZZANI V, PETARCA L, et al.. Thermal stability and decomposition products of hexabromocyclododecane. Industrial & Engineering Chemistry Research, 2001, 40, 3270- 3280.
19	UENO D, ALAEE M, MARVIN C, et al.. Distribution and transportability of hexabromocyclododecane (HBCD) in the Asia-Pacific region using skipjack tuna as a bioindicator. Environmental Pollution, 2006, 144, 238- 247.
20	USEPA. Supplemental guidance for developing soil screening levels for superfund sites [R]. Washington DC: Office of Emergency and Remedial Response U. S. Environmental Protection Agency, 2002.
21	USEPA. Exposure Factors Handbook (2011 Edition): EPA/600/R-09/052F [S]. Washington DC: Office of Research and Development, United States Environmental Protection Agency, 2011.
22	GUO Y, KANNAN K.. Comparative assessment of human exposure to phthalate esters from house dust in China and the United States. Environmental Science & Technology, 2011, 45, 3788- 3794.
23	QI H, LI W L, LIU L Y, et al.. Levels, distribution and human exposure of new non-BDE brominated flame retardants in the indoor dust of China. Environmental Pollution, 2014, 195, 1- 8.
24	BESIS A, CHRISTIA C, POMA G, et al.. Legacy and novel brominated flame retardants in interior car dust- implications for human exposure. Environmental Pollution, 2017, 230, 871- 881.
25	LU J F, HE M J, YANG Z H, et al.. Occurrence of tetrabromobisphenol a (TBBPA) and hexabromocyclododecane (HBCD) in soil and road dust in Chongqing, western China, with emphasis on diastereoisomer profiles, particle size distribution, and human exposure. Environmental Pollution, 2018, 242, 219- 228.

区域	采样点描述	采样年份	样品数	检出率/%	浓度范围/(ng/g)	平均值/(ng/g)	参考文献
上海全域	郊区农田土壤	2017	34	100	0.30 ~ 25.41	1.78	本研究
宝山			3	100	2.10 ~ 25.41	11.56
奉贤			5	100	0.45 ~ 1.06	0.65
嘉定			2	100	0.93 ~ 5.69	3.31
金山			6	100	0.31 ~ 1.17	0.58
闵行			2	100	0.49 ~ 0.64	0.56
浦东			5	100	0.30 ~ 1.19	0.71
青浦			6	100	0.44 ~ 2.27	0.88
松江			5	100	0.42 ~ 0.63	0.54
上海嘉定	居住、农业混合区土壤	2012	7	100	0.30 ~ 8.28	1.87	[5]
北京	城市边缘农田土壤	2010	12	100	0.17 ~ 34.52	2.97	[9]
广东全域	农耕土壤	2014	360	98	ND ~ 4.64	0.68	[10]
山东寿光	HBCD生产厂周边农田土壤	2015	2	100	38.53 ~ 232.72		[6]
河北定州	塑料废物回收厂周边农田土壤	2014	8	100	5.86 ~ 55.52		[7]
浙江宁波	农田土壤	2012	26	97	ND ~ 47.43	7.75	[14]
上海崇明	郊区农田土壤	2009	9		ND ~ 0.03	0.02	[15]

人群	摄入率/ (mg/d)	暴露频率/ (d/a)	暴露持续时间/a	平均体重/ kg	平均暴露时间/d	吸收率	接触土壤的表面积/cm²	土壤附着因子/ (mg/(cm²·d))	经口参考剂量/ (ng/(kg·d))
婴儿	30	350	1	5	1 × 365	0.03	801	0.096	200
幼儿	50	350	3	19	3 × 365	0.03	2564	0.096	200
儿童	50	350	7	29	7 × 365	0.03	3067	0.096	200
青少年	50	350	8	53	8 × 365	0.03	3692	0.096	200
成人	100	225	25	63	25 × 365	0.03	3300	0.096	200
参考文献	[20−21]	[20]	[20−21]	[22]	[20−21]	[23]	[20,22]	[22]	[24]
参数表示	IGR, 记为R_ingestion	EF, 记为F	ED, 记为D	BW, 记为W	AT, 记为T	ABS, 记为C_ABS	SA, 记为A	AF, 记为C_AF	RfD, 记为D_Rf

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上海农田土壤中六溴环十二烷的赋存特征及健康风险评估

Occurrence characteristics and healthy risk assessment of hexabromocyclododecane in agricultural soils in Shanghai

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