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1.
Plasticizers in cap-sealing for bottled foods were analyzed. Twenty-three domestic samples and 80 imported samples, a total of 103 samples, were tested. Among them, 93 contained chloride, and 62 contained di(2-ethylhexyl) phthalate (DEHP), diisodecyl phthalate, O-acetyl tributyl citrate, diacetyllauroyl glycerol, di(2-ethylhexyl) adipate, diisononyl phthalate or dicyclohexyl phthalate. Twelve samples with DEHP-containing caps were further tested for plasticizer levels in the foods. Higher DEHP was detected in oily and fluid food specimens. However, the intake of plasticizers calculated based on usual food consumption did not exceed the tolerable daily intake level in any of the cases. A food sample containing the highest level of DEHP was stored under various conditions, and DEHP that migrated from the cap-sealing into the food was determined. Shaking the bottles increased migration of DEHP into foods.  相似文献   

2.
The presence of plasticizers in PVC toys obtained in October 1998 was investigated. Diisononyl phthalate (DINP), di-2-ethylhexyl phthalate (DEHP), di-n-butyl phthalate (DBP), dinonyl phthalate (DNP), diheptyl phthalate (DHP), and di-2-ethylhexyl adipate (DEHA) were detected. The phthalates were found in all of the 68 samples. The principal phthalate found in toys was DINP, which was present in 48 of 68 samples. The DINP content ranged from 15 mg/g to 580 mg/g, and mean content was 308 mg/g. The highest content was found in a pacifier toy. DEHP was present in 20 of 68 samples and the content ranged from 2.0 mg/g to 380 mg/g. The mean content was 162 mg/g. It was found in 60% of domestic toys.  相似文献   

3.
Duplicate hospital diet samples obtained over 1 week in 2001 were analysed to estimate the daily intake of plasticizers and the results were compared with those obtained in 1999. The plasticizers quantified in this study were: dibutyl phthalate, butylbenzyl phthalate (BBP), di(2-ethylhexyl) phthalate (DEHP), diisononyl phthalate (DINP), di(2-ethylhexyl) adipate (DEHA), diisononyl adipate (DINA) and O-acetyl tributyl citrate (ATBC). Dipropyl, dipentyl, dihexyl and dicyclohexyl phthalate were also analysed but not detected. The analytical procedure for this follow-up study was essentially the same as in the previous one. Detection limits were 0.1-15.6 ng g-1 for each plasticizer. One-week duplicate diet samples provided by three hospitals in three remote prefectures of Japan were analysed as individual meals. DEHP was detected at 6-675 ng g-1 in 62 of 63 meals, significantly lower levels compared with those detected in 1999. Levels of DEHA and DINP also decreased. The mean intake of plasticizers estimated from all samples was 160 μg DEHP day-1, 12.5 μg DEHA day-1, 4.7 μg DINP day-1 and 3.4 μg BBP day-1. Levels of DINA were relatively high in meals from one hospital: in those meals, the average daily intake was 1338 μg day-1. Those of ATBC were also higher in meals from another hospital: the average daily intake was 1228 μg day-1. The sources of DINA and ATBC can be cling-film or sausage packaging.  相似文献   

4.
Plasticizers in total diet samples, baby food and infant formulae   总被引:14,自引:0,他引:14  
The plasticizers di-n-butylphthalate (DBP), butylbenzylphthalate (BBP), di-2-(ethylhexyl)phthalate (DEHP) and di-2-(ethylhexyl)adipate (DEHA) were analysed in 29 total diet samples, in 11 samples of baby food and in 11 samples of infant formulae. In all of the total diet samples the presence of one or more of the plasticizers was demonstrated. Maximum and minimum mean concentrations in the total diet samples were: 0.09-0.19mg DBP/kg, 0.017-0.019mg BBP/kg, 0.11-0.18mg DEHP/kg and 0.13-0.14mg DEHA/kg. One or more of the phthalates was also found in about 50% of the samples of baby food as well as in infant formulae. The calculated mean maximum intakes of the individual compounds from the total diet samples were below 10% of the restrictions proposed by the EU Scientific Committee for Food (SCF), and the spread in individual intakes was considerable. DEHP was the plasticizer determined most frequently and contributed the highest fraction of its tolerable daily intake (TDI). Hence, the maximum calculated intake of DEHP from single samples of the foodstuffs analysed could be up to one-third of the TDI. The calculated mean intake of DEHA was about 1% of the TDI with a maximum value of 13% of the TDI. Violations of the restrictions proposed by the EU Scientific Committee for Food (SCF) in the form of TDI values or specific migration limits were not found in this investigation.  相似文献   

5.
Plasticizers in duplicate diet samples obtained over 1 week were analysed in order to estimate daily intake. The phthalate esters were as follows: diethyl, dipropyl, dibutyl, dipentyl, dihexyl, butylbenzyl, dicyclohexyl, di(2-ethylhexyl), dioctyl, diisooctyl (mixture of isomers) and diisononyl (mixture). Di(2-ethylhexyl) adipate was also determined. Homogenized samples of composite meals were extracted with acetonitrile, lipids were removed by extraction into n-hexane and the acetonitrile layer was cleaned using FlorisilR and R Bondesil PSA dual layer column. Phthalates were determined by GC/MS (SIM). Phthalate recovery from the fortified food mixture by this method was 62.5-140.8%. Quality assurance as assessed by three laboratories indicated coefficient of variance in the levels of detected phthalates in same lot samples as below 10%. Detection limits were 0.1-23ng/g for each phthalate. One-week duplicate diet samples provided by three hospitals in three remote prefectures of Japan were analysed as individual meals. In all 63 samples, DEHP was present at the highest level among all phthalates in the range 10-4400ng/g. The intake of plasticizers estimated from all samples was 519 µ g DEHP/day, 86 µ g DEHA/day, 65 µ g DINP/day, and 4.7 µ g BBP/day. Calculated DEHP in 2-day samples out of 21 days exceeded EU TDI for a person of 50kg body weight (1850 µ g per day). Disposable PVC gloves used during the preparation of meals were suspected as the source of the high DEHP content. One-day intake of the other phthalates and DEHA was below 7% of TDI in all cases. High concentrations of DEHP (5990ng/g) was found in baby food used in quality assurance work. The source of contamination was the PVC-tube used during production and was effectively reduced by replacing the tube by one made of stainless steel.  相似文献   

6.
A sensitive and selective GC-MS method was developed and used for simultaneous analysis of di-(2-ethylhexyl) adipate (DEHA) and 20 selected phthalates in the food samples from the 2013 Canadian Total Diet Study. At least one of the 21 target chemicals was detected in 141 of the 159 different food composite samples analysed. However, only seven of the 21 target chemicals were detected, with di-(2-ethylhexyl) phthalate (DEHP) and DEHA being detected most frequently, in 111 and 91 different food composite samples, respectively, followed by di-n-butyl phthalate (DBP) (n = 44), n-butyl benzyl phthalate (BBzP) (32), di-iso-butyl phthalate (DiBP) (27), di-ethyl phthalate (DEP) (3), and di-cyclohexyl phthalate (DCHP) (1). Levels of DEP (di-ethyl phthalate), DiBP, DBP, BBzP and DCHP were low, in general, with average concentrations of 9.63, 8.26, 23.2, 12.4 and 64.9 ng g–1, respectively. Levels of DEHA and DEHP varied widely, ranging from 1.4 to 6010 ng g–1 and from 14.4 to 714 ng g–1, respectively. High levels of DEHA were found mainly in the composite samples where the individual food items used to prepare the composite were likely packaged in polyvinyl chloride (PVC) wrapping film, while the highest DEHP levels were found in the vegetable and fruit samples.  相似文献   

7.
Packaging materials intended for direct food contact were acquired on the Brazilian retail market and analysed for their plasticizer content. Analyses were carried out by gas chromatography with flame ionization detection. Di-2-ethyl-hexyl adipate (DEHA), di-2-ethyl-hexyl phthalate (DEHP) and di-iso-decyl phthalate (DIDP) plasticizers were identified in films and closure seals in concentrations ranging from 12 to 19% (w/w), 15 to 44% (w/w) and 10 to 11% (w/w), respectively. Brazilian regulations state that for use with foods with a fat content above 5%, the levels of DEHP and DIDP in the plastic material should be no greater than 3%. The results obtained demonstrate a lack of conformity. It would be advisable to include information on the labels of packaging materials about their restrictions of use in order to advise manufacturers and consumers about their proper usage.  相似文献   

8.
Epoxidized soybean oil (ESBO) was surveyed in the 103 samples of cap sealing for bottled foods on the Japanese market. Most of the sealings were made of polyvinyl chloride, while a few were made of polyethylene or acrylic resin. All the sealings contained ESBO in the range of 0.006-42.4%. Sealings for baby food, jam, etc. contained higher levels of ESBO, though those for beverages contained lower levels. Sealings in lug caps and press-on twist caps contained higher levels of ESBO, though that in pilfer-proof caps contained lower levels. Some sealings in screw caps and lug caps also contained other plasticizers, for example, di-2-ethylhexyl phthalate and diisononyl phthalate, and their ESBO contents were 1/10 of those in sealings containing only ESBO. In this survey, ESBO was the most common plasticizer in cap sealing resin for bottled foods on the Japanese market.  相似文献   

9.
Ten samples of retail packed lunches purchased from convenience stores were determined for 11 phthalates and di(2-ethylhexyl) adipate (DEHA) in August 2000, 2 months after the prohibition of DEHP-containing PVC gloves in Japan. Each homogenized sample was extracted with acetonitrile, partitioned with n-hexane, and cleaned up using Florisil and PSA columns. Phthalates in the extract were determined by GC/MS (SIM). The limits of detection were 14.9 ng/g for di(2-ethylhexyl) phthalate (DEHP) and 18.6 ng/g for dibutyl phthalate (DBP). Levels of phthalates in packed lunch samples were 45 to 517 ng DEHP/g (198 ng/g, average), ND to 90 ng DEHA/g, and ND to 10.0 ng BBP/g. Diisononyl phthalate (DINP) was detected in one sample at 76 ng/g. Average DEHP level in ten samples was 4% of that in 1999. The contents of other phthalates were also reduced. DBP was not detected in any sample. Recovery of deuterated isomers added as surrogates was 27.9% for DNP-d4, and 40.6 to 101.5% for the other phthalates.  相似文献   

10.
The levels of dibutyl phthalate (DBP), butylbenzyl phthalate (BBP), di-(2-ethylhexyl) phthalate (DEPHP), di-isononyl phthalate (DINP), di-(2-ethylhexyl) adipate (DEHA) and di-isononyl adipate (DINA) were determined in 50 processed foods (ham and sausage, fried dumpling and shao-mai, fish paste products, croquette and fried fish, bread, noodle, pickles, etc.). DBP, BBP, DEHP, DINP, DEHA, and DINA were contained at nd approximately 47.7, nd approximately 16.6, nd approximately 749, nd approximately 358, nd approximately 57.2 and nd approximately 20,200 ppb, respectively. High-level contamination of DINA was found in fish paste products, croquette and shao-mai, presumably because of migration from plasticized wrapping film using for food packaging. We studied the relationship between DINA migration from wrapped PVC film into fried croquette and its standing time after frying. When the croquette was wrapped immediately after frying, the migration from wrapping film into the croquette was highest (36,400 ng/g). On wrapping after standing for 5 min and 30 min, the migration level was reduced to 1/3.5 and 1/14 of the highest level, respectively.  相似文献   

11.
Foods with at least a few percent of free oil packed in glass jars with metal closures were analyzed for migration of additives, primarily plasticizers, from the gasket of the lid. One hundred and fifty-eight samples were collected in June 2005, i.e., some 10 months after the problem of excessive migration into oily food was communicated to the industry. In a first step, the composition of the additives in the gaskets was determined. Then the compounds found in the lid were measured in the jar content. Sixty-four percent of the gaskets contained epoxidized soy bean oil (ESBO) as principal plasticizer, 22% a phthalate, and 6% substantial amounts of di(2-ethylhexyl) adipate (DEHA). Concentrations in the food reached 1,170 mg/kg for ESBO, 270 mg/kg for diisononyl phthalate (DINP), 740 mg/kg for diisodecyl phthalate (DIDP), 825 mg/kg for di(2-ethylhexyl) phthalate (DEHP), and 180 mg/kg for DEHA. Further, elevated concentrations of plasticizers not authorized by the EU were found: diisononyl-cyclohexane-1,2-dicarboxylate (DINCH), 2-ethylhexyl palmitate and stearate, as well as epoxidized linseed oil (ELO). The few samples complying with the European rules contained little or well emulsified oil; some others were probably of very recent production (beginning of shelf life). It is concluded that there was still no lid reliably complying with the European rules (EU and national legislation).  相似文献   

12.
采用气相色谱-三重四极杆串联质谱法(GC-MS/MS)建立了邻苯二甲酸酯(PAEs)的检测方法,并对12种不同香型白酒中的18种PAEs塑化剂的含量进行了测定。结果表明,18种PAEs的分离效果良好,检出限为0.001~0.428 mg/kg,定量限为0.003~1.426 mg/kg。邻苯二甲酸二异壬酯(DINP)的线性范围为0.403~20.150 μg/mL,其余17种PAEs的线性范围为0.020~1.106 μg/mL,相关系数(R2)均>0.999,精密度试验结果相对标准偏差(RSD)均<10%,回收率为82.99%~115.25%;白酒样品检出塑化剂的种类主要为邻苯二甲酸二异丁酯(DIBP)、邻苯二甲酸二正丁酯(DBP)及邻苯二甲酸二(2-乙基)己酯(DEHP),含量分别在0.18~1.53 mg/kg、0.27~1.36 mg/kg、0.18~1.86 mg/kg,其中兼香型白酒样品的DBP含量为1.36 mg/kg,超出国标规定限值。在凤香型白酒样品和馥郁香型白酒样品中检出邻苯二甲酸二甲酯(DMP),含量分别为0.53 mg/kg、0.45 mg/kg,在药香型白酒样品中检出邻苯二甲酸二正辛酯(DNOP),含量为1.42 mg/kg,其余均未检出。  相似文献   

13.
为测定烟用水基型乳胶中的邻苯二甲酸酯,用加有内标物质的正己烷溶液对乳胶样品进行了超声萃取,并采用气相色谱/质谱/选择离子监测法(GC/MS/SIM)测定了144个样品中的7种邻苯二甲酸酯:邻苯二甲酸二甲酯(DMP)、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)、邻苯二甲酸二辛酯(DOP)和邻苯二甲酸丁基苄基酯(BBP).结果表明:①样品中加入2 mL水,超声30 min萃取效果较好;②在标准溶液浓度范围内,7种邻苯二甲酸酯的线性均较好,相关系数达到0.996以上;③低、中、高3种浓度的加标回收率在85% ~ 111%之间,相对标准偏差(RSD)均小于5%;④当前国内烟用水基胶中使用的邻苯二甲酸酯类增塑剂主要集中在D1BP,DBP两种.  相似文献   

14.
选用4种大孔树脂和4种酒类专用活性炭为吸附剂,采用静态吸附法,首先对57%酒精度模拟加标酒样进行吸附实验,以邻苯二甲酸二甲酯(dimethyl phthalate,DMP)、邻苯二甲酸二异丁酯(diisobutyl phthalate,DIBP)、邻苯二甲酸二丁酯(di-n-butyl phthalate,DBP)、邻苯二甲酸二(2-乙基)己酯(diethylhexyl phthalate,DEHP)4种邻苯二甲酸酯类塑化剂的吸附率为指标进行初选。之后用57%酒精度浓香型原酒进行验证,以塑化剂的吸附率和原酒中己酸乙酯、乙酸乙酯、乳酸乙酯、丁酸乙酯4种香气成分的损失率作为指标,筛选出理想的吸附剂。结果表明:1)JT201、JT203酒类专用活性炭对模拟酒样中4种塑化剂的吸附效果较好,平均吸附率为91.01%和87.21%,大孔树脂中非极性的D4006较其他树脂吸附效果好,吸附率达73.67%;极性大孔树脂NKA-Ⅱ和颗粒活性炭的吸附率不足60%,初选JT201、JT203酒类专用活性炭为原酒中塑化剂的吸附剂。2)JT201、JT203酒类专用活性炭吸附后,原酒中DMP、DBP的去除率均达90%以上,JT201对DIBP、DEHP的去除率均达80%以上,JT203对DIBP、DEHP去除率为78%、72%;JT201、JT203吸附处理后原酒中己酸乙酯、乙酸乙酯、乳酸乙酯、丁酸乙酯分别损失7.7%、6.1%、11.9%、11.6%和10.4%、8.6%、33.9%、16.0%,本研究确定JT201酒类专用活性炭为去除浓香型原酒中塑化剂的最佳吸附剂。  相似文献   

15.
ABSTRACT: Phthalates are a group of diesters of ortho‐phthalic acid (dialkyl or alkyl aryl esters of 1,2‐benzenedicarboxylic acid). Higher‐molecular‐weight phthalates, such as di‐2‐ethylhexyl phthalate (DEHP), are primarily used as plasticizers to soften polyvinyl chloride (PVC) products, while the lower‐molecular‐weight phthalates, such as diethyl phthalate (DEP), di‐n‐butyl phthalate (DBP), and butyl benzyl phthalate (BBzP), are widely used as solvents to hold color and scent in various consumer and personal care products. Phthalates have become ubiquitous environmental contaminants due to volatilization and leaching from their widespread applications, and thus contamination of the environment has become another important source for phthalates in foods in addition to migration from packaging materials. Human exposure to phthalates has been an increased concern due to the findings from toxicology studies in animals. DEHP, one of the important and widely used phthalates, is a rodent liver carcinogen. DEHP, DBP, BBzP, and several phthalate metabolites, such as monobutyl phthalate, monobenzyl phthalate, and mono‐(2‐ethylhexyl) phthalate, are teratogenic in animals. Since foods are the major source of exposure to phthalates, information on levels of phthalates in foods is important for human exposure assessment. The objective of this review is to identify the knowledge gaps for future investigations by reviewing levels of a wide range of phthalates in a variety of foods, such as bottled water, soft drinks, infant formula, human milk, total diet foods, and others, migration of phthalates from various food‐packaging materials, and traditional and new methodologies for the determination of phthalates in foods.  相似文献   

16.
Plasticizer contamination of foods sold in retail packed lunches and set lunches in restaurants was determined by GC/MS. The phthalate esters were as follows: diethyl, dipropyl, dibutyl, dipentyl, dihexyl, butylbenzyl, dicyclohexyl, di(2-ethylhexyl), dioctyl, diisooctyl (mixture of isomers) and diisononyl (mixture). Di(2- ethylhexyl) adipate was also determined. Sixteen packed lunches and ten set lunches were analysed, and in all samples the concentration of di(2-ethylhexyl) phthalate (DEHP) was the highest, at 0.80-11.8 mg/ kg in packed lunches and 0.012-0.30 mg/kg in set lunches. The DEHP content of five packed lunches exceeded 1.85 mg, which is the EU tolerable daily intake (TDI) for a person of 50 kg body weight. Foodstuffs that were components of the packed lunches were taken from the factory at each step of preparation and phthalates were determined. For example, chicken contained 0.08 mg/kg DEHP when uncooked, 13.1 mg/ kg after frying and 16.9 mg/kg after packing. Disposable PVC gloves used in the preparation of foods were apparently the source of high DEHP concentrations. The gloves used during cooking or packaging were sprayed with 68% (w/w) ethanol to sterilize them. PVC gloves from the factory contained 22 or 41% by weight of DEHP. To confirm the link with the contamination problem, samples of boiled rice, croquette and boiled dry radish were handled in the laboratory with PVC gloves containing 30% (w/w) DEHP. DEHP migration levels of 0.05 mg/kg in rice or 0.33 mg/kg in croquette, and 11.1 mg/kg in radish were found. The alcohol sprayed onto the gloves increased the migration of DEHP to 2.03 mg/kg in rice, 2.45 mg/ kg in croquette, and 18.4 mg/kg in radish.  相似文献   

17.
Retail samples of Canadian butter and margarine wrapped in aluminium foil-paper laminate were found to contain dibutyl, butyl benzyl and/or di-2-ethylhexyl phthalate (DBP, BBP, DEHP) as packaging migrants at levels up to 10.6, 47.8 and 11.9 micrograms/g, respectively. These phthalates were determined by capillary gas chromatography with flame ionization detection (GC-FID) after clean-up of the separated oil by sweep co-distillation. The phthalate esters found in the contacted butter or margarine were also found in the contacting wrappers. They were determined in wrapper extracts by liquid chromatography with diode array detection or by GC-FID. Analysis of unused wrappers showed 76-88% of the total DBP and DEHP to be present on the foil (outer) surface as a component of the protective coating (washcoat). The remainder of the DBP and DEHP was found on the food-contacting paper surface, presumably by transfer from the outer to inner surface during storage in tightly wound rolls, although transfer of phthalate esters, if present in the paper-foil adhesive, cannot be ruled out. Food-contacting surface concentrations of DBP and DEHP were found to be 2.4 to 4.7 and 2.8 to 3.6 micrograms/cm2, respectively. Samples of each packaging component: paper, foil, adhesive, washcoat and inks were analysed for phthalate esters and only the washcoat was found to contain phthalate esters.  相似文献   

18.
利用气相色谱模拟分离软件,测定火腿肠及其肠衣中的塑化剂邻苯二甲酸二甲酯、邻苯二甲酸二乙酯、 邻苯二甲酸二丁酯、邻苯二甲酸二环己酯、邻苯二甲酸二(2-乙基)己酯和邻苯二甲酸二正辛酯的含量。对比超声 提取和索式提取2 种前处理方法对样品中塑化剂的提取效果,确定了程序升温条件,采用外标法定量。结果表明: 6 种标准物质的标准曲线R2为0.996 7~0.998 8,最小检出限为0.04 mg/kg,相对标准偏差为5.0%~9.3%;索式提取 法的提取效果更显著,某些火腿肠和火腿肠肠衣中含有高含量的生殖致癌物邻苯二甲酸酯类物质。  相似文献   

19.
Phthalic acid and phthalate esters are of growing interest due to their significant usage and potential toxicity. Polyethylene terephthalate (PET) and glass are both widely used materials for bottled drinking water. In this study, phthalic acid (PhA), bis(2-ethylhexyl) phthalate (DEHP), dimethyl phthalate (DMP), diethyl phthalate (DEP), diisobutyl phthalate (DiisoBP) and dibutyl phthalate (DBP) were analysed in a large number of Italian bottled water samples. These samples showed different concentrations of phthalates are nearly 20 times higher in samples bottled in PET than those from glass bottles with total levels of phthalates of 3.52 and 0.19 µg l-1, respectively. However, the observed levels do not represent a significant exposure pathway when considering the US Environmental Protection Agency (USEPA) reference dose (an estimate of a daily oral exposure to the human population, including sensitive subgroups, that is likely to be without an appreciable risk of deleterious effects during a lifetime). In addition, no significant correlation was found between the phthalate concentrations and the physicochemical properties of the different water samples, apart from the still/sparkling water parameter for the PET samples. In this instance, slightly higher concentrations were observed for the PET bottled still water samples than for the sparkling water samples, although no explanation has been found yet.  相似文献   

20.
Soft PVC children's products are usually plasticized with phthalates. As young children suck and chew on toys, they extract and ingest certain quantities of the plasticizers. Some phthalates are suspected to affect the kidneys and liver and cause testicular damage. Therefore, the EC has prohibited the sale of toys and childcare articles intended to be placed in the mouth by children <3 years of age made of soft PVC containing >0.1% by weight of six phthalates (1999/815/EC). The aim was to study the materials and plasticizers used in soft children's products. In February 2001, a market surveillance was performed in The Netherlands and 62 soft toys were sampled. Forty-seven of these toys contained plasticized PVC. Diisononylphthalate (DINP) and di(2-ethylhexyl)phthalate (DEHP) were the predominant plasticizers and were usually found in concentrations between 30 and 45% by weight. One teething ring was made of PVC plasticized with 45% by weight of DINP and was not in compliance with Decision 1999/815/EC. The DINP and DEHP migration was determined in saliva simulant using the 'Head over Heels' agitation method. All toys complied with the Scientific Committee on Toxicity, Ecotoxicity and the Environment (SCTEE) guidance release value of 6.7 microg min(-1) 10 cm(-2). The DEHP migration of six toys exceeded the SCTEE guidance release value of 1.7 microg min(-1) 10 cm(-2). Substitutes found for phthalates plasticizers are acetyltributylcitrate, tributylcitrate and diisononyladipate. In addition, other plasticizers and additives were found in minor amounts. The toxicity and the migration behaviour of these substances is less known and requires more attention. To ensure the safety of PVC toys, these substances should also be regulated.  相似文献   

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