塑料餐盒中邻苯二甲酸酯的迁移风险研究

蓝敏怡; 李会茹; 应光国

doi:10.6054/j.jscnun.2022026

塑料餐盒中邻苯二甲酸酯的迁移风险研究

doi: 10.6054/j.jscnun.2022026

华南师范大学环境学院/广东省化学品污染与环境安全重点实验室/环境理论化学教育部重点实验室，广州 510006

基金项目:

广东省化学品污染与环境安全重点实验室 2019B030301008

详细信息

通讯作者:
应光国，Email：guangguo.ying@scnu.edu.cn

中图分类号: X502
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出版历程
- 收稿日期: 2021-05-10
- 网络出版日期: 2022-05-12
- 刊出日期: 2022-04-25

On the Migration Risk of Phthalates in Plastic Containers

Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety/MOE Key Laboratory of Theoretical Chemistry of Environment/School of Environment, South China Normal University, Guangzhou 510006, China

摘要

摘要: 测定市售的一次性塑料餐盒中邻苯二甲酸酯的质量分数和探究其向食品中的浸出规律，由此评估对人体造成的健康风险。以聚丙烯(PP)塑料餐盒为研究对象，采用气相色谱-质谱法对样品中16种邻苯二甲酸酯(PAEs)的质量分数进行检测；并依据GB/T 23296.1—2009要求，选择水、4%乙酸、10%乙醇和异辛烷为食品模拟物，考察塑料餐盒中PAEs的浸出率随时间和温度的变化情况，运用美国环保署(U.S. EPA)推荐的健康风险评估模型评价由此造成的健康风险。16种PAEs中邻苯二甲酸二乙酯(DEP)、邻苯二甲酸二异丁酯(DIBP)、邻苯二甲酸二丁酯(DBP)、邻苯二甲酸二(2－乙基)己酯(DEHP)、邻苯二甲酸二苯酯(DPhP)、邻苯二甲酸二辛酯(DNOP)的检出率分别为100%、100%、78%、78%、92%、85%，质量分数范围分别为0.140~0.829、0.237~1.676、ND~0.995、ND~2.302、ND~1.714、ND~0.213 mg/g；但在4种食品模拟物浸出实验中仅检出4种PAEs(DEP、DBP、DIBP、DEHP)，浸出率从大到小的顺序为：异辛烷、10%乙醇、4%乙酸、水；温度越高，时间越长，浸出率越大。暴露评估健康风险结果显示：在25、40、55 ℃下，人群对浸出PAEs日暴露量的致癌风险为1.09×10^-8、4.52×10^-8、1.83×10^-7；总非致癌风险分别为1.10×10^-4、3.62×10^-4、1.21×10^-3。结果表明：PAEs可通过与塑料餐盒接触迁移至食物中，但由此造成的健康风险在U.S. EPA推荐的人群可接受水平范围内。
- 塑料食品包装 /
- 邻苯二甲酸酯 /
- 增塑剂 /
- 迁移 /
- 健康风险
Abstract: The content of Phthalates (PAEs) in plastic containers and the migration of PAEs to food were investigated so as to evaluate the health risk for human body. The contents of 16 kinds of PAEs in polypropylene (PP) plastic containers were determined with meteorological chromatography-mass spectrometry. Water, 4% acetic acid, 10% ethanol and Isooctane were selected as food simulants according to the requirements of GB/T 23296.1—2009 to investigate the change of the leaching rate of typical PAEs in plastic containers with time and temperature, and the health risk assessment model recommended by the U.S. Environmental Protection Agency (EPA) was used to evaluate the health risk caused by the migration of PAEs. The detection rates of Diethyl phthalate (DEP), Diisobutyl phthalate (DIBP), Dibutyl phthalate (DBP), Bis(2-ethylhexyl) phthalate (DEHP), Diphenyl phthalate (DPhP) and Di-n-octylphthalate (DNOP) in 16 PAEs were 100%, 100%, 78%, 78%, 92% and 85%, respectively. The concentration ranges were 0.140~0.829, 0.237~1.676, ND~0.995, ND~2.302, ND~1.714 and ND~0.213 mg ·g^-1 respectively. However, only four PAEs (DEP, DBP, DIBP and DEHP) were detected in the leaching experiments of four food simulants, and the leaching rate order was as follows: Isooctane, 10% Ethyl alcohol, 4% Acetic acid and Water. The higher the temperature, the longer the time and the higher the leaching rate. The health risk of exposure assessment showed that the carcinogenic risk of daily exposure of PAEs was 1.09×10^-8, 4.52×10^-8 and 1.83×10^-8 at 25, 40 and 55 ℃ respectively. The total non-carcinogenic risk was 1.10×10^-8, 3.62×10^-8 and 1.21×10^-8 respectively. The results show that PAEs can be transferred to food through contact with plastic food containers, but the health risk is within the range of acceptable levels recommended by the U.S. EPA.
- plastic food packaging /
- phthalates /
- migration /
- health risk /

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图 1 PAEs标准品在SIM模式下的色谱图

Figure 1. The chromatogram of PAE solution reference material in the SIM mode

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图 2 塑料餐盒中PAEs相关化合物的贡献率

Figure 2. The proportion of PAEs-related compounds in plastic containers

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图 3 不同食品模拟物中PAEs的迁移率

Figure 3. The migration rate of PAEs in different food simulators

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图 4 不同温度下PAEs的迁移率

Figure 4. The migration rate of PAEs at different temperatures

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表 1 食品模拟物的选择

Table 1. The selection of food simulants

食品类型	食品模拟物
水性食品(pH>4.5)	蒸馏水
酸性食品(pH≤4.5的水性食品)	4%(体积分数)乙酸
酒精食品	10%(体积分数)乙醇
脂肪食品	异辛烷

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表 2 PAEs的保留时间和离子质荷比

Table 2. The retention time and ion mass charge ratio of PAEs

化合物	CAS号	保留时间/min	定量离子质荷比(m/z)	定性离子质荷比(m/z)
DMP	131-11-3	7.37	163	77/194/133
DEP	84-66-2	8.72	149	177/105/222
DIBP	84-69-5	11.51	149	223/205/104
DBP	84-74-2	12.49	149	223/104/167
DMEP	117-82-8	12.85	149	59/149/104/176
BMPP	146-50-9	13.62	149	167/85/251
DEEP	605-54-9	14.01	149	72/104/193
DPP	131-18-0	14.40	149	237/219/104
DHXP	84-75-3	16.23	149	251/104/233
BBP	85-68-7	16.32	149	91/206/104
DBEP	117-83-9	17.38	149	101/85/193
DCHP	84-61-7	17.84	149	167/249/104
DEHP	117-81-7	17.94	149	167/279/113
DPhP	84-62-8	18.09	225	77/104/153
DNOP	117-84-0	19.57	149	279/104/261
DNP	84-76-4	21.09	149	293/167/275

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表 3 塑料餐盒中PAEs的质量分数

Table 3. The concentration of PAEs in plastic containers mg/kg

样品	DMP	DEP	DIBP	DBP	DMEP	BMPP	DEEP	DPP	DHXP	BBP	DBEP	DCHP	DEHP	DPhP	DNOP	DNP
1	ND	0.177±0.013	1.676±0.861	0.190±0.038	ND	ND	ND	ND	ND	ND	ND	ND	0.201±0.033	1.327±0.162	0.121±0.013	ND
2	ND	0.642±0.022	1.032±0.321	0.254±0.006	ND	ND	ND	ND	ND	ND	ND	ND	0.131±0.011	1.094±0.055	0.115±0.012	ND
3	ND	0.436±0.048	0.944±0.639	ND	ND	ND	ND	ND	ND	ND	ND	ND	0.162±0.020	1.653±0.081	0.094±0.037	ND
4	ND	0.576±0.042	0.761±0.224	ND	ND	ND	ND	ND	ND	ND	ND	ND	ND	1.301±0.202	ND	ND
5	ND	0.829±0.062	0.237±0.398	ND	ND	ND	ND	ND	ND	ND	ND	ND	ND	1.664±0.138	0.038±0.003	ND
6	ND	0.140±0.017	1.113±0.276	0.238±0.019	ND	ND	ND	ND	ND	ND	ND	ND	0.851±0.053	1.714±0.062	0.147±0.012	ND
7	ND	0.385±0.008	0.773±0.555	0.244±0.047	ND	ND	ND	ND	ND	ND	ND	ND	0.092±0.012	0.843±0.059	0.060±0.006	ND
8	ND	0.198±0.012	0.943±0.549	0.276±0.076	ND	ND	ND	ND	ND	ND	ND	ND	0.148±0.042	0.957±0.060	0.105±0.027	ND
9	ND	0.257±0.014	1.115±0.482	0.138±0.010	ND	ND	ND	ND	ND	ND	ND	ND	0.509±0.045	ND	0.075±0.005	ND
10	ND	0.313±0.009	0.681±0.060	0.560±0.067	ND	ND	ND	ND	ND	ND	ND	ND	0.561±0.055	0.611±0.039	0.101±0.009	ND
11	ND	0.204±0.010	0.675±0.093	0.812±0.117	ND	ND	ND	ND	ND	ND	ND	ND	0.554±0.004	0.761±0.060	0.092±0.003	ND
12	ND	0.217±0.021	1.609±0.129	0.995±0.060	ND	ND	ND	ND	ND	ND	ND	ND	2.302±0.602	1.018±0.102	ND	ND
13	ND	0.186±0.016	0.842±0.075	0.227±0.022	ND	ND	ND	ND	ND	ND	ND	ND	1.239±0.168	0.685±0.089	0.213±0.028	ND
14	ND	0.193±0.029	0.523±0.037	0.040±0.020	ND	ND	ND	ND	ND	ND	ND	ND	0.305±0.129	0.416±0.015	0.112±0.020	ND
注：“ND”表示样品中未检出PAEs类化合物。表中数据为平均值±标准差(n=3)。

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表 4 不同温度下36 h时PAEs在不同食品模拟物中的浸出率

Table 4. The migration rate of PAEs in different food simulators at different temperatures for 36 h %

温度/℃	食品模拟物	DEP	DIBP	DBP	DEHP
25	水	0.13	0.08	0.59	0.06
	4%乙酸	0.14	0.09	0.98	0.07
	10%乙醇	0.21	0.33	1.58	0.13
	异辛烷	0.36	0.11	5.49	0.09
40	水	0.41	0.80	1.3	0.27
	4%乙酸	0.45	1.18	1.44	0.26
	10%乙醇	0.59	1.84	2.22	0.28
	异辛烷	1.85	3.67	11.84	0.35
55	水	1.39	0.87	1.29	0.11
	4%乙酸	1.32	1.15	1.57	0.08
	10%乙醇	1.41	0.94	2.08	0.12
	异辛烷	5.24	21.32	75.76	7.34

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表 5 6种优先控制PAEs的TDI

Table 5. The TDI of 6 PAEs under priority control

PAEs	DMP	DEP	DBP	BBP	DEHP	DNOP
CAS号	131-11-3	84-66-2	84-74-2	85-68-7	117-81-7	117-84-0
参考剂量/(μg·(kg·d)^-1)	10 000	800	100	200	20	3 000

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表 6 塑料餐盒中PAEs的日暴露量

Table 6. The daily exposure of PAEs in plastic containers

PAEs	EDI/(ng·L^-1)
PAEs	25 ℃	40 ℃	55 ℃
DMP	0.242	0.544	1.292
DEP	0.186	0.767	2.353
DIBP	0.668	15.621	32.775
DBP	10.338	20.556	87.976
DEHP	0.782	3.226	13.073
总计	12.216	40.714	137.469

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表 7 塑料餐盒中PAEs的健康风险

Table 7. The health risk of PAES in plastic containers

健康风险	PAEs	温度条件
健康风险	PAEs	25 ℃	40 ℃	55 ℃
非致癌	DIBP	6.68×10^-6	1.56×10^-4	3.28×10^-4
	DBP	1.03×10^-4	2.06×10^-4	8.80×10^-4
	DEHP	3.91×10^-5	1.61×10^-4	6.54×10^-4
致癌	DEHP	1.09×10^-8	4.52×10^-8	1.83×10^-7

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