2016—2018年烟台苹果中杀菌剂残留及其膳食暴露风险分析

doi:10.11923/j.issn.2095-4050.cjas20190700139

摘要/Abstract

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。

关键词: 苹果, 农药残留, 杀菌剂, 膳食暴露, 食品安全, 风险

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.

Key words: Apple, Pesticide Residue, Fungicide, Dietary Exposure, Food Safety, Risk

中图分类号:

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[J]. 农学学报, 2020, 10(12): 49-56.

Gong Chunbo, Dong Fengguang, Zheng Zhong, Wang Zhaoxia. Dietary Exposure Safety Survey on Fungicide Residue in Apple: Yantai 2016-2018[J]. Journal of Agriculture, 2020, 10(12): 49-56.

图/表 7

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年度	样本数量	检出率/%
年度	样本数量	苯醚甲环唑	多菌灵	甲基硫菌灵	咪鲜胺	戊唑醇	异菌脲	合计
2016	239	0.42	44.35	10.04	0.00	0.00	0.00	54.81
2017	237	0.42	52.32	14.77	0.42	0.00	0.00	67.93
2018	242	2.48	24.79	9.50	0.41	0.41	0.83	38.43
合计	718	1.11	40.39	11.42	0.28	0.14	0.28	53.62

年度	样本数量	检出率/%
年度	样本数量	苯醚甲环唑	多菌灵	甲基硫菌灵	咪鲜胺	戊唑醇	异菌脲	合计
2016	239	0.42	44.35	10.04	0.00	0.00	0.00	54.81
2017	237	0.42	52.32	14.77	0.42	0.00	0.00	67.93
2018	242	2.48	24.79	9.50	0.41	0.41	0.83	38.43
合计	718	1.11	40.39	11.42	0.28	0.14	0.28	53.62

农药种类	毒性	ADI/[mg/(kg·BW)]	检出频次	均值/(mg/kg)	95% CI/(mg/kg)	数值范围/(mg/kg)	P90/(mg/kg)	P95/(mg/kg)	MRL/(mg/kg)
戊唑醇	低毒	0.03	1	0.00103a	0.000973~0.00108	ND~0.0208	0.00100	0.00100	2
异菌脲	低毒	0.06	2	0.00111a	0.000959~0.00125	ND~0.0406	0.00100	0.00100	5
苯醚甲环唑	低毒	0.01	8	0.00209a	0.000962~0.00127	ND~0.560	0.00100	0.00100	0.5
甲基硫菌灵	低毒	0.08	82	0.00270a	0.00187~0.00352	ND~0.210	0.00410	0.00880	5
咪鲜胺	低毒	0.01	2	0.0138b	-0.010~3.0378	ND~8.800	0.00100	0.00100	2
多菌灵	低毒	0.03	290	0.0154b	0.0124~0.0184	ND~0.544	0.0430	0.0920	5

农药种类	毒性	ADI/[mg/(kg·BW)]	检出频次	均值/(mg/kg)	95% CI/(mg/kg)	数值范围/(mg/kg)	P90/(mg/kg)	P95/(mg/kg)	MRL/(mg/kg)
戊唑醇	低毒	0.03	1	0.00103a	0.000973~0.00108	ND~0.0208	0.00100	0.00100	2
异菌脲	低毒	0.06	2	0.00111a	0.000959~0.00125	ND~0.0406	0.00100	0.00100	5
苯醚甲环唑	低毒	0.01	8	0.00209a	0.000962~0.00127	ND~0.560	0.00100	0.00100	0.5
甲基硫菌灵	低毒	0.08	82	0.00270a	0.00187~0.00352	ND~0.210	0.00410	0.00880	5
咪鲜胺	低毒	0.01	2	0.0138b	-0.010~3.0378	ND~8.800	0.00100	0.00100	2
多菌灵	低毒	0.03	290	0.0154b	0.0124~0.0184	ND~0.544	0.0430	0.0920	5

人群分组	全人群					摄食者
人群分组	人数	体重均值/kg	分布类型	消费量均值/ [kg/(人·d)]	分布类型	人数	体重均值/kg	分布类型	消费量均值/ [kg/(人·d)]	分布类型
2~6岁	19	19.78	Logistic	0.0745	Uniform	11	18.97	Extvalue	0.129	Triang
7~10岁	29	30.46	Triang	0.0598	Uniform	11	29.19	BetaGeneral	0.158	Beta General
11~13岁	24	45.89	Extvalue	0.0800	Beta General	10	44.47	Invgauss	0.192	Beta General
14~17岁	19	63.54	Weibull	0.0704	Ext value	8	66.63	Extvalue	0.167	Beta General
18~49岁男	205	74.19	Invgauss	0.0720	Uniform	85	73.96	Invgauss	0.174	Triang
18~49岁女	205	62.94	Invgauss	0.0823	Gamma	100	62.08	Logistic	0.169	BetaGeneral
50~64岁男	182	72.02	Loglogistic	0.0648	Uniform	68	72.62	Gamma	0.173	Uniform
50~64岁女	199	63.49	Logistic	0.0594	Uniform	71	62.38	BetaGeneral	0.167	Ext value
65~79岁男	77	70.11	Logistic	0.0573	Triang	28	72.04	Extvalue	0.160	Normal
65~79岁女	114	61.73	Logistic	0.0759	Triang	56	63.94	Extvalue(	0.154	Invgauss
≥80岁男	15	67.64	Expon	0.0283	Triang	4	74.73	74.73^*	0.106	0.106^*
≥80岁女	26	50.8	Invgauss	0.0502	Uniform	9	47.86	BetaGeneral	0.145	Beta General
男	538	69.11	Logistic	0.0659	Trian	210	69.37	Logistic	0.169	Normal
女	576	60.78	Logistic	0.0713	Uniform	251	60.27	Logistic	0.164	Weibull
全人群	1114	64.81	Logistic	0.0687	Triang	461	64.42	Logistic	0.166	Triang