2016—2018年烟台苹果中杀菌剂残留及其膳食暴露风险分析

宫春波, 董峰光, 郑重, 王朝霞

农学学报. 2020, 10(12): 49-56

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农学学报 ›› 2020, Vol. 10 ›› Issue (12) : 49-56. DOI: 10.11923/j.issn.2095-4050.cjas20190700139
植物保护

2016—2018年烟台苹果中杀菌剂残留及其膳食暴露风险分析

作者信息 +

Dietary Exposure Safety Survey on Fungicide Residue in Apple: Yantai 2016-2018

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摘要

为了解烟台主产区苹果中杀菌剂残留状况,评估居民苹果来源杀菌剂膳食暴露风险,采用随机采样方法,2016—2018年每年10月于种植、贮存和流通环节共采集718份样本,进行18种杀菌剂检测。基于蒙特卡罗拟合计算危害指数,评估杀菌剂膳食暴露风险。结果表明,苹果中存在6种杀菌剂残留,检出率53.26%,3年检出率分别为38.43%、67.93%、38.43%,年度间差异显著(α=0.01);多菌灵最高40.39%,戊唑醇最低0.14%。6种杀菌剂残留量均值范围1.03~15.4 μg/kg,组间差异显著(α=0.05),戊唑醇、异菌脲、甲基硫菌灵、多菌灵各自最大残留量远小于最大残留限量(maximum residue limit,MRL),存在咪鲜胺和苯醚甲环唑超过MRL情况,超标率0.28%。6种杀菌剂共检出385频次,多菌灵最高290频次;同一样本存在多种杀菌剂残留,最多同一样本5种杀菌剂残留。各人群分组中,6种杀菌剂的日均膳食暴露量(estimated daily intake,EDI)各异,女性大于男性;未成年人组中,6种杀菌剂的EDI均值与年龄呈现负相关。除2~6岁组外,5种杀菌剂的膳食暴露风险商(hazard quotient,HQ)值远小于1;咪鲜胺HQ>1概率值各异,2~6岁风险概率值最大;多菌灵、苯醚甲环唑HQ>1仅存在全人群2~6岁组,其概率值分别为0.01%、0.02%。苹果来源杀菌剂的慢性膳食暴露风险危害概率值为0.30%~66%,女性大于男性,摄食者大于全人群,2~6岁、7~10岁组是高风险膳食暴露组。苹果中杀菌剂残留的总体质量状况处在可接受安全水平,咪鲜胺是苹果来源杀菌剂膳食暴露风险主要危害因子,尤其对于儿童、少年等低龄人群。

Abstract

To investigate the level of fungicide residue in apple of Yantai, and assess the dietary exposure risk to residents, 718 apple samples were randomly selected in October from 2016 to 2018, covering orchards, refrigeration storage and supermarkets, and 18 fungicides were tested. Hazard index was calculated based on Monte Carlo to assess the dietary exposure risk of fungicide residue in apples. The study showed that 6 fungicides were detected in apples of Yantai, the total positive rate was 53.26%, the maximum was carbendazim of 40.39% and minimum was tebuconazole of 0.14%. The positive rate of 2016-2018 was 38.43%, 67.93%, 38.43%, and the year to year difference was significant (α=0.01). The mean value of the 6 fungicides’ residue was from 1.03 μg/kg to 15.4 μg/kg, significantly different between each group (α=0.05). None of the residue of tebuconazole, iprodione, thiophanate-methyl, carbendazim measured exceeded the GB Maximum Residue Limit (MRL), but prochloraz and difenoconazole content of individual sample exceeded MRL, with a ratio of 0.28%. The detect frequency of the six fungicides was 385 times, carbendazim was detected 290 times, which was the highest, multiple fungicides’ residue, at most five, was detected in the same sample. The estimated daily intake (EDI) mean value of the 6 fungicides was different in each population group, higher in female group than that in male group; the EDI had a negative correlation trend with age in children and teenage group, five fungicides’ hazard quotient (HQ) was less than one except in the 2-6 years old group; the probability rate of prochloraz HQ exceeding one varied, which was the highest in the 2-6 years old group, the HQ of carbendazim and difenoconazole exceeding one only found in the 2-6 years old group, which was 0.01% and 0.02%, respectively. In general, the hazard index of long-term dietary exposure risk rate of apple is 0.30%-66%, higher for female than for male, and higher for intake group than for the total, the 2-6 years old group and 7-10 years old group are the most vulnerable one. Fungicides’ residue is relatively low in Yantai apples and belongs to the acceptable level to residents, and prochloraz is the major hazard factor of fungicide dietary exposure risk of apple, particularly to children and teens.

关键词

苹果 / 农药残留 / 杀菌剂 / 膳食暴露 / 食品安全 / 风险

Key words

Apple / Pesticide Residue / Fungicide / Dietary Exposure / Food Safety / Risk

引用本文

导出引用
宫春波 , 董峰光 , 郑重 , 王朝霞. 2016—2018年烟台苹果中杀菌剂残留及其膳食暴露风险分析. 农学学报. 2020, 10(12): 49-56 https://doi.org/10.11923/j.issn.2095-4050.cjas20190700139
Gong Chunbo , Dong Fengguang , Zheng Zhong , Wang Zhaoxia. Dietary Exposure Safety Survey on Fungicide Residue in Apple: Yantai 2016-2018. Journal of Agriculture. 2020, 10(12): 49-56 https://doi.org/10.11923/j.issn.2095-4050.cjas20190700139

参考文献

[1]
Bondonno Nicola P, Bondonno Catherine P, Ward Natalie C, et al. The cardiovascular health benefits of apples: Whole fruit vs. isolated compounds[J]. Trends in Food Science & Technology, 2017,69:243-256.
[2]
Fabiani R, Minelli L, Rosignoli P. Apple intake and cancer risk: a systematic review and meta-analysis of observational studies[J]. Public Health Nutrition, 2016,19(14):2603-2617.
OBJECTIVE: Conflicting results on the association between fruit consumption and cancer risk have been reported. Little is known about the cancer preventive effects of different fruit types. The present meta-analysis investigates whether an association exists between apple intake and cancer risk. DESIGN: Relevant observational studies were identified by literature search (PubMed, Web of Science and Embase). A random-effect model was used to estimate the cancer risk in different anatomical sites. Between-study heterogeneity and publication bias were assessed using adequate statistical tests. RESULTS: Twenty case-control (three on lung, five on colorectal, five on breast, two on oesophageal, three on oral cavity, two on prostate and one each on pancreas, bladder, larynx, ovary, kidney and brain cancer) and twenty-one cohort (seven on lung, two on colorectal, three on breast and one each on oesophageal, pancreas, bladder, kidney, endometrial, head-neck, urothelial and stomach cancer) studies met the inclusion criteria. Comparing the highest v. lowest level of apple consumption, the reduction of lung cancer risk was statistically highly significant in both case-control (OR=0.75; 95% CI 0.63, 0.88; P=0.001, I 2=0 %) and cohort studies (relative risk=0.89; 95% CI 0.84, 0.94; P<0.001, I 2=53 %). Instead, in the case of colorectal (OR=0.66; 95% CI 0.54, 0.81; P<0.001, I 2=55%), breast (OR=0.79; 95% CI 0.73, 0.87; P<0.001, I 2=1 %) and overall digestive tract (OR=0.50; 95% CI 0.36, 0.69; P<0.001, I 2=90 %) cancers a significant preventive effect of apples was found only in case-control studies while prospective studies indicated no effect. No evidence of publication bias could be detected for colorectal, oral cavity, oesophageal and breast cancer. However, some confounding effects may be present and related to the consumption of other fruit which have not been considered as adjusting factors. CONCLUSIONS: The present meta-analysis indicates that consumption of apples is associated with a reduced risk of cancer in different anatomical sites.
[3]
Lozowicka, Bozena. Health risk for children and adults consuming apples with pesticide residue[J]. Science of The Total Environment, 2015,502:184-198.
[4]
Manolis Tzatzarakis, Ioanna Katsikantami, Elena Vakonaki, et al. Monitoring of pesticide residues in apples from the Greek market[J]. Toxico L Lett, 2017,280(S1):177.
[5]
Bożena Łozowicka, Piotr Kaczyński. Pesticide Residues in Apples (2005-2010)[J]. Arch Environ Prot, 2011,37(3):43-54.
Fruit and vegetables constitute an essential part of human diet and that is why they should be "safe". Chemical contaminants of plant origin in food, including the pesticide residues, are defined as critical differentiators of quality and food safety. Pesticide residues are found in fruits, vegetables, cereals and herbs chemically protected at low concentrations, but they are one of the elements that affect the quality of healthcare.
The aim of this study was to assess the pesticide residues in apples from the north-eastern Poland (Lubelskie, Podlaskie and Warminsko-Mazurskie provinces) and get an answer whether any contamination in fruit from the region is similar to that in other countries and whether it can lead to exposure of consumer's health. Also assessed compliance of used pesticides with applicable law and found residues were compared with the Maximum Residue Levels (MRLs). The study showed that 59% of the samples of apples from the north-eastern Poland contain pesticide residues below the MRL, and 7% above the limits. The estimated dietary intake has shown the chronic dietary exposure of the most vulnerable groups - ildren and adults to the pesticide residues in Polish apples was relatively low and does not constitute a health risk to. The results show that apples from north-eastern Poland are safe.
[6]
李志霞, 聂继云, 闫震, 等. 基于点评估方法的渤海湾产区苹果中农药残留膳食暴露风险研究[J]. 农药学学报, 2015(6):715-722.
[7]
刘永明, 葛娜, 崔宗岩, 等. 2012—2014年青岛、深圳、大连三口岸282份进口水果和蔬菜中农药残留监测[J]. 中国食品卫生杂志, 2016,28(4):511-515.
[8]
田利光, 姜召涛, 曹新芳. 烟台苹果产业发展现状与建议[J]. 烟台果树, 2018(2):1-3.
[9]
庞荣丽, 成昕, 谢汉忠, 等. 我国水果质量安全标准现状分析[J]. 果树学报, 2016(5):612-623.
[10]
2015年烟台统计年鉴[EB/OL].(2019-09-24). http://tjj.yantai.gov.cn/art/2018/3/29/art_118_935455.html.
[11]
China Health and Nutrition Survey. Survey Data-Longitudinal [EB/OL]. (2019-07-12). http://www.cpc.unc.edu/projects/china/data/datasets/data_downloads/longitudinal.
[12]
国家食品安全风险评估中心. 2016年国家食品污染物和有害因素风险监测工作手册[M]. 北京:国家食品安全风险评估中心, 2016:285-297.
[13]
中华人民共和国国家卫生和计划生育委员会, 中华人民共和国农业部, 国家食品药品监督管理总局. GB 2763—2016,食品安全国家标准食品中农药最大残留限量. 北京: 中国标准出版社, 2016:16,23,33,39-41,57,79-80,93,98,108,135,141,164.
[14]
刘沛, 吴永宁. 构建中国膳食暴露评估模型提升我国食品安全风险评估水平[J]. 中华预防医学杂志, 2010,44(3):181-183.
[15]
Szpyrka E, Kurdziel A, SLOwik-Borowiec M, et al. Consumer exposure to pesticide residues in apples from the region of south-eastern Poland[J]. Environmental Monitoring and Assessment, 2013,185(11):8873-8878.
The production of apples in Poland is the largest among the countries of the European Union, and therefore, the consumption of these fruits is high in our country. The aim of this study was to determine the presence of pesticide residues in Polish apples and to assess if these residues pose a risk to the health of the consumer. Furthermore, compliance with legal regulations concerning the use of plant protection products in crop cultivation was ascertained. Pesticide residues were found in 192 samples (61.5 % of tested samples). In six samples (1.9 %), residues exceeded maximum residue limits. Violations concerned the insecticides: indoxacarb, diazinon and fenitrothion. The highest long-term consumer exposure was found in the case of consumption of apples with diazinon residue for both groups, adults and toddlers [4 % acceptable daily intake (ADI), adults; 21 % ADI, toddlers]. The highest values of short-term exposure were obtained in the case of consumption of apples with indoxacarb [5 % acute reference dose (ARfD), adults; 27 % ARfD, toddlers] and fenitrothion (4 % ARfD, adults; 23 % ARfD, toddlers). Although fungicides are the pesticides found most often in apples, the consumption of apples with insecticide residues constitutes the greatest hazard to human health.
[16]
杨桂玲, 陈晨, 王强, 等. 农药多残留联合暴露风险评估研究进展[J]. 农药学学报, 2015,17(2):119-127.
[17]
Xu G, Nie J, Wu Y, et al. The effects of fruit bagging on residue behavior and dietary risk for four pesticides in apple[J]. Scientific Reports, 2018,8(1):1-6.
Zika virus (ZIKV) has recently caused a pandemic disease, and many cases of ZIKV infection in pregnant women resulted in abortion, stillbirth, deaths and congenital defects including microcephaly, which now has been proposed as ZIKV congenital syndrome. This study aimed to investigate the in situ immune response profile and mechanisms of neuronal cell damage in fatal Zika microcephaly cases. Brain tissue samples were collected from 15 cases, including 10 microcephalic ZIKV-positive neonates with fatal outcome and five neonatal control flavivirus-negative neonates that died due to other causes, but with preserved central nervous system (CNS) architecture. In microcephaly cases, the histopathological features of the tissue samples were characterized in three CNS areas (meninges, perivascular space, and parenchyma). The changes found were mainly calcification, necrosis, neuronophagy, gliosis, microglial nodules, and inflammatory infiltration of mononuclear cells. The in situ immune response against ZIKV in the CNS of newborns is complex. Despite the predominant expression of Th2 cytokines, other cytokines such as Th1, Th17, Treg, Th9, and Th22 are involved to a lesser extent, but are still likely to participate in the immunopathogenic mechanisms of neural disease in fatal cases of microcephaly caused by ZIKV.
[18]
Policy R F, Fao N D, Guidelines for the study of dietary intakes of chemical contaminants[J]. Who Offset Publication, 1985(87):1-102.
[19]
聂继云, 李志霞, 刘传德, 等. 苹果农药残留风险评估[J]. 中国农业科学, 2014,47(18):3655-3667.
目的】开展苹果农药残留风险评估研究,为苹果消费、农药残留监管和农药最大残留限量(MRLs)制修订提供科学依据。【方法】对采自主产区的200个苹果样品进行农药残留检测,分别用%ADI%ARfD进行农药残留慢性膳食摄入风险评估和急性膳食摄入风险评估,用ADI值、大份餐和体重计算最大残留限量估计值(eMRL),借鉴英国兽药残留委员会兽药残留风险排序矩阵进行农药和样品风险排序。【结果】⑴ 检测的102种农药中26种农药检出残留,检测的200个样品中189个样品检出农药残留,仅有1个样品农药残留超标(超标农药为氧乐果);⑵ 检出残留的26种农药,其慢性膳食摄入风险(用%ADI表示)在0.00%—1.07%,平均值为0.13%;其急性膳食摄入风险(用%ARfD表示)在0.18%—22.41%,平均值为4.12%;⑶ 根据残留风险得分,检出残留的26种农药可划分为3类,即高风险农药(8种)、中风险农药(10种)、低风险农药(8种);⑷ 以风险指数排序,风险高的样品仅占1.5%,风险中、低和极低的样品占98.5%;⑸ 在检出残留的26种农药中,灭幼脲可不制定MRL,氟硅唑等6种农药的MRLs过严,乐果等5种农药的MRLs过松,建议矮壮素、苯醚甲环唑、虫酰肼、二嗪磷、氟硅唑、甲基硫菌灵、乐果、联苯菊酯、氯氟氰菊酯、氰戊菊酯、炔螨特、噻嗪酮、三氯杀螨醇、杀扑磷、戊唑醇、烯唑醇、亚胺硫磷和抑霉唑的MRLs分别设定为4、1、2、0.5、0.6、7、0.2、1、2、2、1、0.8、0.2、0.1、3、0.5、1和3 mg·kg-1。【结论】苹果农药残留检出率相对较高,但99.5%的苹果样品其农药残留量均低于MRLs。苹果农药残留慢性膳食摄入风险和急性膳食摄入风险均很低。苹果应重点关注氧乐果、磷胺、杀扑磷、毒死蜱、二嗪磷、联苯菊酯、亚胺硫磷和乐果残留。建议修订或制定苹果中矮壮素等18种农药的MRLs。
[20]
叶孟亮, 聂继云, 徐国锋, 等. 苹果中4种常用农药残留及其膳食暴露评估[J]. 中国农业科学, 2016(7):1289-1302.
【目的】对国产苹果中多菌灵、甲基硫菌灵、吡虫啉和灭幼脲4种常用农药残留及其膳食暴露进行评估,明确并量化中国居民食用苹果途径的上述4种常用农药膳食摄入风险水平,为苹果安全生产、消费及质量安全监管提供依据。【方法】基于渤海湾(辽宁、山东、河北)和西北黄土高原(陕西、山西、河南)两大苹果优势主产区采集的282份苹果样品,运用专业风险评估软件@Risk,尝试构建非参数概率评估模型,对中国居民食用苹果途径的农药膳食摄入(暴露)风险进行概率评估。首先对282份苹果样品中上述4种农药残留检测值进行分布拟合,拟合度运用Chi-Squared、Anderson-Darling、Kolmogorov-Smirnov 3种统计方法进行检验,综合考虑3种评估拟合结果,确定最佳拟合分布。STMR、HR取最佳分布拟合值,%ADI和%ARfD分别表示慢性膳食摄入风险和急性膳食摄入风险。【结果】参试的282份苹果样品,255份(占90.4%)苹果样品中检出了农药残留。在检出的4种常用农药中,多菌灵的检出率最高,达到81.9%;其次为甲基硫菌灵和吡虫啉,分别为52.1%和39.0%;灭幼脲的检出率最低,仅为31.2%。绝大多数苹果样品中农药残留量处于较低水平,最大检出浓度为0.9251 mg·kg-1(多菌灵),但仍远低于最大残留限量值3.0 mg·kg-1。样品中4种常用农药残留量均值依次为多菌灵(0.1042 mg·kg-1)>灭幼脲(0.0182 mg·kg-1)>甲基硫菌灵(0.0082 mg·kg-1)>吡虫啉(0.0050 mg·kg-1)。样品中4种常用农药残留量离散程度有异,变异系数分别达到232.8%(甲基硫菌灵)、214.8%(吡虫啉)、174.1%(灭幼脲)和136.4%(多菌灵)。282份苹果样品农药残留量分布规律较明显,随着农药残留浓度的升高,样品所占的比例均呈逐渐降低的趋势。27份(占9.6%)苹果样品中未检出上述4种常用农药,198份(占70.2%)苹果样品中检出2种及以上农药残留,19份(占6.7%)苹果样品甚至检出4种农药残留。不同年龄组人群食用苹果途径的上述4种常用农药慢性膳食摄入风险(%ADI)分别为0.2120%—35.1100%(多菌灵)、0.0051%—0.8240%(吡虫啉)、0.0049%—0.1710%(甲基硫菌灵)和0.0004%—0.0152%(灭幼脲);急性膳食摄入风险(%ARfD)分别为0.1940%—16.0500%(多菌灵)和0.0122%—0.9400%(吡虫啉)。幼儿(2—6岁)和儿童(7—13岁)2个年龄组人群由于体重较轻,而苹果摄入量相对较高,膳食摄入风险明显高于其他年龄组人群,为重点监控对象。不同年龄组人群之间,随着年龄的增加,农药膳食摄入风险整体呈逐渐下降趋势;同一年龄组人群,选取的百分位点值越高,农药膳食摄入风险越大。【结论】中国苹果中多菌灵、甲基硫菌灵、吡虫啉和灭幼脲这4种常用农药检出率较高,但所有样品农药残留量均低于最大残留限量。中国居民食用苹果途径的上述4种常用农药慢性和急性膳食摄入风险均很低,幼儿和儿童2个年龄组人群膳食摄入风险明显高于其他年龄组人群,需重点关注。
[21]
李志霞, 聂继云, 闫震, 等. 基于点评估方法的渤海湾产区苹果中农药残留膳食暴露风险研究[J]. 农药学学报, 2015(6):715-722.
[22]
兰丰, 刘传德, 周先学, 等. 山东省主产区苹果农药残留水平及累积急性膳食摄入风险评估[J]. 食品安全质量检测学报, 2015,6(7):2595-2602.
[23]
Manuela Olga Pogăcean, Hlihor R M, Gavrilescu M. Monitoring pesticides degradation in apple fruits and potential effects of residues on human health[J]. J Environ Eng Landsc, 2014,22(3):1171-1182.
[24]
李耘, 钱永忠, 陈晨, 等. 混合化学物风险评估技术及研究进展[J]. 农产品质量与安全, 2013(6):42-48.
[25]
吕萍萍, 徐晓曦. 农药残留对食品安全的影响及其检测新技术的研究进展[J]. 农学学报, 2012,2(6):65-67.
农药残留对食品质量安全的影响越来越明显,对食品农药残留的检测方法及技术提出了更高的要求。本研究主要阐述了中国食品中农药残留的来源和危害,并对食品中农药残留的检测新技术进行综述,以期为食品中农药残留的检测及新技术发展提供参考依据。

基金

2017年烟台市科学技术发展计划项目“基于蒙特卡罗模拟的烟台居民食物中化学污染物膳食暴露危害评估”(2017WS118)

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烟草种植与生产

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