合肥市土壤中卤代阻燃剂的赋存特征及风险评估

doi:10.3969/j.issn.1000-5641.2024.06.014

摘要/Abstract

摘要：

在合肥市不同区域采集了31个土壤样品, 利用气相色谱−质谱仪测定土壤中卤代阻燃剂的含量, 并对其组成特征、空间分布、来源进行解析. 研究结果显示, 合肥市表层土壤中总的多溴联苯醚 (polybrominated diphenyl ethers, ∑₂₃PBDEs)、替代型溴代阻燃剂 (alternative brominated flame retardants, ∑₂₂ABFRs) 和得克隆及其类似物 (dechloranes, ∑₁₁DECs) 浓度均值分别为(6.490 ± 13.221)、(26.375 ± 101.928)和(0.815 ± 0.760) ng/g. 十溴二苯乙烷 (DBDPE) 是替代型溴代阻燃剂中最主要的同系物, 占比高达84.4%. 空间分布上, 卤代阻燃剂浓度的高值多位于城市开发区、高新区等制造业集中地. 源解析表明, 其主要来源为商业多溴联苯醚, 其次来源于阻燃剂的生产、运输及其环境降解过程. 基于危险指数法估算的非致癌风险评价结果表明, 研究区内目标物的非致癌风险指数均小于1, 在可接受范围内, 无非致癌风险.

关键词: 土壤, 卤代阻燃剂, 空间分布, 风险评估

Abstract:

The contents of halogenated flame retardants (HFRs) in 31 surface soil samples collected from different areas of Hefei City were measured by gas chromatography-mass spectrometry. Their composition characteristics, spatial distribution, and sources were explored. The results showed that the mean concentrations of ∑₂₃PBDEs, ∑₂₂ABFRs, and ∑₁₁DECs in the surface soils of Hefei City were (6.490 ± 13.221), (26.375 ± 101.928), and (0.815 ± 0.760) ng/g, respectively. DBDPE is the main homologue among alternative flame retardants, accounting for 84.4%. In terms of spatial distribution, the hotspots of HFRs were mostly located in manufacturing concentrated areas, such as urban development zones and high-tech zones. Source analysis revealed that the use of commercial polybrominated diphenyl ethers and alternative flame retardants in the study area were the main emission sources, followed by the production, transportation, and environmental degradation process of HFRs. Non-carcinogenic risk assessment was carried out based on hazard index method. The results showed that the non-carcinogenic risk index of the target objects in the study area were less than 1, which were within the acceptable range, indicating that there was no non-carcinogenic risk.

Key words: soils, halogenated flame retardants, spatial distribution, risk assessment

中图分类号:

X144

杨丁业, 杨静, 金芮合, 丁方方, 张雨欣, 刘敏. 合肥市土壤中卤代阻燃剂的赋存特征及风险评估[J]. 华东师范大学学报（自然科学版）, 2024, 2024(6): 161-177.

Dingye YANG, Jing YANG, Ruihe JIN, Fangfang DING, Yuxin ZHANG, Min LIU. Occurrence characteristics and risk assessment of halogenated flame retardants in soils of Hefei City[J]. Journal of East China Normal University(Natural Science), 2024, 2024(6): 161-177.

图/表 15

图1

表1

合肥市表层土壤卤代阻燃剂的浓度"

类别	化合物	名称	最小值/(ng/g)	最大值/(ng/g)	平均值/(ng/g)	检出率/%
PBDEs	BDE17	2,2’,4-三溴联苯醚	ND	1.032	0.054 ± 0.181	29.0
	BDE28/33	2,4,4’-三溴联苯醚	ND	0.132	0.027 ± 0.039	83.9
	BDE49	2,2’,4,4’-四溴联苯醚	ND	1.047	0.086 ± 0.183	35.5
	BDE47	2,2’,4,5’-四溴联苯醚	ND	0.327	0.039 ± 0.069	58.1
	BDE66	2,3’,4,4’-四溴联苯醚	ND	0.212	0.012 ± 0.037	51.6
	BDE100	2,2’,3,4,4’-五溴联苯醚	ND	0.398	0.021 ± 0.069	74.2
	BDE99	2,2’,4,4’,5-五溴联苯醚	ND	0.933	0.170 ± 0.257	64.5
	BDE85	2,2’,4,4’,6-五溴联苯醚	ND	0.650	0.061 ± 0.114	74.2
	BDE154	2,2’,3,4,4’,5’-六溴联苯醚	ND	1.985	0.097 ± 0.367	74.2
	BDE153	2,2’,4,4’,5,5’-六溴联苯醚	ND	2.045	0.073 ± 0.360	9.7
	BDE138	2,2’,4,4’,5,6’-六溴联苯醚	ND	1.055	0.060 ± 0.182	16.1
	BDE183	2,2’,3,4,4’,5’,6-七溴联苯醚	ND	3.127	0.121 ± 0.549	83.9
	BDE190	2,3,3’,4,4’,5,6-七溴联苯醚	ND	0.792	0.047 ± 0.138	41.9
	BDE202	2,2’,3,3’,4,4’,5,6’-八溴联苯醚	ND	0.986	0.121 ± 0.168	74.2
	BDE201	2,2’,3,3’,4,4’,6,6’-八溴联苯醚	ND	2.391	0.148 ± 0.417	71.0
	BDE197	2,2’,3,3’,4,5’,6,6’-八溴联苯醚	ND	1.532	0.100 ± 0.264	74.2
	BDE203	2,2’,3,3’,5,5’,6,6’-八溴联苯醚	ND	0.943	0.071 ± 0.161	90.3
	BDE196	2,2’,3,4,4’,5,5’,6-八溴联苯醚	ND	1.277	0.075 ± 0.220	93.5
	BDE208	2,2’,3,3’,4,4’,5,5’,6-九溴联苯醚	ND	1.542	0.123 ± 0.267	71.0
	BDE207	2,2’,3,3’,4,4’,5,6,6’-九溴联苯醚	0.042	2.420	0.254 ± 0.412	100
	BDE206	2,2’,3,3’,4,5,5’,6,6’-九溴联苯醚	0.018	1.944	0.210 ± 0.349	96.8
	BDE209	十溴联苯醚	0.999	51.134	4.520 ± 8.748	100
	Σ₂₂PBDEs	多溴联苯醚 (无BDE209)	0.400	26.742	1.970 ± 4.561
	Σ₂₃PBDEs	多溴联苯醚 (含BDE209)	1.399	77.876	6.490 ± 13.221
ABFRs	TBP	三溴苯酚	0.337	34.728	2.256 ± 6.062	100
	ATE	2,4,6-三溴苯基烯丙基醚	ND	0.171	0.033 ± 0.044	80.6
	TBECH	1,2-二溴乙基环己烷	ND	0.358	0.183 ± 0.077	96.8
	TBPX	2,3,5,6-四溴对二甲苯	ND	0.025	0.006 ± 0.005	51.6
	PBBZ	五溴苯	ND	0.071	0.034 ± 0.016	74.2
ABFRs	TBCO	1,2,5,6-四溴环辛烷	ND	0.092	0.013 ± 0.017	38.7
	TBOCT	四溴邻氯甲苯	0.014	0.490	0.093 ± 0.092	100
	PBT	五溴甲苯	ND	0.038	0.014 ± 0.009	58.1
	PBEB	五溴乙苯	ND	0.034	0.007 ± 0.008	61.3
	HBBZ	六溴苯	0.118	0.292	0.180 ± 0.041	100
	BB101	2,2’,4,5,5’-五溴联苯	ND	0.398	0.017 ± 0.070	22.6
	PBBA	丙烯酸五溴苄酯	ND	0.410	0.030 ± 0.079	45.2
	HCDBCO	六氯二溴辛烷	ND	3.470	0.690 ± 0.860	96.8
	EHTBB	2-乙基己基-2,3,4,5-四溴苯甲酸酯	ND	0.240	0.043 ± 0.047	9.7
	BB153	2,2’,4,4’,5,5’-六溴联苯	ND	2.394	0.166 ± 0.432	6.5
	BTBPE	2,4,6-三溴苯氧基乙烷	ND	1.447	0.080 ± 0.252	51.6
	TBPH	2-乙基己基四溴邻苯二甲酸	ND	0.727	0.104 ± 0.127	87.1
	DBDPE	十溴二苯乙烷	0.871	544.305	22.260 ± 95.702	100
	BATBPE	2-溴烯丙基-2,4,6-三溴苯醚	ND	0.011	0.005 ± 0.003	32.3
	DPTE	2,3-二溴丙基-2,4,6-三溴苯基)醚	ND	0.083	0.033 ± 0.009	3.2
	TBC	三(2,3-二溴丙基)异氰脲酸酯	ND	0.493	0.082 ± 0.096	22.6
	OBIND	八溴-1,1,3-三甲基-3-苯基苯胺	ND	0.152	0.045 ± 0.020	3.2
	Σ₂₂ABFRs	替代型溴代阻燃剂	2.159	582.652	26.375 ± 101.928
DECs	HCPN	1,2,3,4,7,7-六氯-5-苯基-2-降冰片烯	ND	0.406	0.106 ± 0.092	83.9
	DEC-602	得克隆602	ND	1.585	0.106 ± 0.275	83.9
	Cplus	氯丁加	ND	0.115	0.021 ± 0.026	32.3
	DEC-604CB	得克隆604 组分 B	ND	0.107	0.012 ± 0.017	3.2
	DEC-603	得克隆603	ND	0.318	0.030 ± 0.054	38.7
	DEC-604	得克隆604	ND	3.150	0.124 ± 0.553	58.1
	Cl10-DP	Cl10-得克隆	ND	0.460	0.108 ± 0.104	67.7
	DEC-601	得克隆601	ND	0.070	0.010 ± 0.013	29.0
	Syn-DP	顺式得克隆	ND	0.529	0.030 ± 0.092	29.0
	Cl11-DP	Cl11-得克隆	0.035	0.523	0.178 ± 0.132	100
	Anti-DP	反式得克隆	ND	0.644	0.089 ± 0.122	90.3
	Σ₁₁DECs	得克隆及其类似物	0.250	4.217	0.815 ± 0.760

表1

图2

图3

图4

图5

图6

图7

图8

图9

表2

表3

图10

表4

图11

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目标物	PC1	PC2	PC3	PC4	PC5
BDE28/33	0.389	–0.139	0.048	0.033	0.708
BDE47	0.698	–0.052	0.043	0.314	0.398
BDE66	0.976	–0.041	0.075	0.063	0.168
BDE100	0.982	–0.041	0.061	0.038	0.133
BDE99	0.440	–0.118	0.301	0.191	0.568
BDE85	0.933	–0.034	0.078	–0.051	0.197
BDE154	0.941	0.285	0.041	0.067	0.093
BDE183	0.984	–0.048	0.041	0.039	0.131
BDE202	0.933	0.134	0.112	0.052	0.109
BDE201	0.979	0.104	0.042	0.078	0.087
BDE197	0.985	–0.015	0.047	0.048	0.068
BDE203	0.983	–0.057	0.039	0.040	0.119
BDE196	0.987	–0.028	0.038	0.050	0.092
BDE208	0.963	0.098	0.049	0.112	0.123
BDE207	0.934	0.007	0.230	0.081	0.175
BDE206	0.910	0.047	0.027	0.141	0.155
BDE209	0.966	–0.067	0.051	0.072	0.081
TBP	0.018	0.940	–0.008	0.191	–0.122
ATE	0.485	0.041	0.063	–0.034	0.633
TBECH	0.156	0.026	0.092	0.439	0.346
TBPX	–0.036	–0.005	0.914	0.087	0.136
PBBZ	0.018	0.266	0.235	0.805	–0.058
TBOCT	0.709	–0.046	0.100	–0.035	0.513
PBT	0.392	0.353	0.705	0.253	–0.050
PBEB	0.115	–0.055	0.855	0.030	0.070
HBBZ	0.150	0.079	0.291	0.196	–0.340
HCDBCO	0.544	–0.171	–0.135	–0.104	0.266
BTBPE	0.984	–0.061	0.049	0.039	0.079
TBPH	0.903	–0.104	–0.008	0.030	0.147
DBDPE	0.051	0.953	–0.011	0.118	–0.089
HCPN	–0.041	0.030	0.223	0.501	–0.061
DEC-602	0.057	–0.076	–0.062	–0.134	–0.084
DEC-604	0.987	–0.037	0.043	0.045	0.125
Cl10-DP	–0.135	0.767	0.132	–0.382	0.075
Cl11-DP	0.203	–0.112	0.023	0.849	0.113
Anti-DP	0.096	0.244	–0.091	–0.035	0.024

人群	年龄/岁	DIR/(g/d)	BSA/cm²	BW/kg	SAS/(mg/(cm²·d))	AF/%	OEF/%
成人	≥ 20	0.05	4615	62.9	0.096	3	12.5
青少年	[12,19]	0.05	3692	52.0	0.096	3	12.5
儿童	[6,11]	0.05	3067	25.2	0.096	3	20.8
幼儿	[1,5]	0.10	2564	16.0	0.096	3	20.8
婴儿	< 1	0.02	801	5.0	0.096	3	12.5

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