联苯菊酯等3种杀虫剂在茶园茶叶、土壤及降雨径流中的残留

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赵之德^{1, 2,},
李海涛^1,,,
梁涛¹
1.中国科学院地理科学与资源研究所北京 100101
2.中国科学院大学北京 100049
基金项目: 国家重点研发计划项目2016YFD0201208

详细信息

作者简介:赵之德, 主要研究方向为茶园农药残留。E-mail:zhidezhao@qq.com

通讯作者:李海涛, 主要研究方向为环境核算、环境管理评价。E-mail:liht@igsnrr.ac.cn

中图分类号:S481⁺.1

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出版历程

收稿日期:2018-09-03
录用日期:2018-12-18
刊出日期:2019-08-01

Residues of three insecticides in tea leaves, soil and rainwater runoff

ZHAO Zhide^{1, 2,},
LI Haitao^1,,,
LIANG Tao¹
1. Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China
2. University of Chinese Academy of Sciences, Beijing 100049, China
Funds: the National Key R&D Program of China2016YFD0201208

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Corresponding author:LI Haitao, E-mail: liht@igsnrr.ac.cn

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摘要
摘要:为探究杀虫剂联苯菊酯、溴氰菊酯和虫螨腈的常用剂量和减施剂量对绿茶品种‘丰绿’（Camellia sinensis Yutakmitor）的鲜叶和茶园土壤及降雨径流的影响以及可能产生的膳食摄入风险，选择联苯菊酯、溴氰菊酯和虫螨腈的当地常用剂量和减量30%剂量作为处理组，在浙江绍兴富盛镇御茶村茶园进行田间试验，喷药后1 d、3 d、7 d、10 d分别采集试验小区的鲜叶和土壤，喷药后4 d、8 d采集降雨径流，检测样品中的杀虫剂残留并评估3种杀虫剂的膳食暴露风险。试验结果表明：同种杀虫剂常用剂量处理的茶鲜叶中残留虽然高于减施剂量处理，但二者差异不显著，杀虫剂减量30%对减少鲜叶中的残留并无明显效果。经过常用剂量与减施剂量处理的茶鲜叶中联苯菊酯的半衰期分别为5.89 d和4.61 d，溴氰菊酯的半衰期分别为5.75 d和2.55 d，虫螨腈的半衰期分别为3.72 d和2.70 d。3种杀虫剂在土壤中的残留均低于《土壤环境质量标准（GB 15618-1995）》中有机氯杀虫剂六六六的一级标准值（≤ 0.05 mg·kg^-1）。联苯菊酯和虫螨腈在降雨径流中的残留均低于《生活饮用水卫生标准（GB5749-2006）》中有机氯杀虫剂六六六的限值（0.005 mg·L^-1），溴氰菊酯在降雨径流中的残留低于《生活饮用水卫生标准（GB5749-2006）》中溴氰菊酯的限值（≤ 0.02 mg·L^-1）。3种杀虫剂在茶叶中的膳食暴露风险评估结果表明，联苯菊酯、溴氰菊酯和虫螨腈的最大暴露量分别为0.5×10^-4~1.7×10^-4 mg·kg^-1（bw）·d^-1、1.0×10^-6~7.3×10^-6 mg·kg^-1（bw）·d^-1、1.0×10^-5~8.3×10^-5 mg·kg^-1（bw）·d^-1，风险商分别为0.005~0.017、0.000 2~0.001和0.000 2~0.003，使用联苯菊酯、溴氰菊酯和虫螨腈防治茶树虫害，对消费者的膳食暴露的风险均可以接受。与常用剂量相比，减施剂量处理对减少茶叶和环境中的杀虫剂残留的效果不明显。
关键词:杀虫剂残留/
茶/
土壤/
降雨径流/
杀虫剂减量使用
Abstract:Insecticide residues in tea have attracted much attention, and the means to reduce the level of residues in tea and the surrounding environment is a serious issue. Reducing the usage or dose of insecticide may be a viable option to address this problem. We analyzed the possible dietary intake risks and the effects of regular dose versus reduced dose of bifenthrin, deltamethrin, and chlorfenapyr on their residues in fresh tea leaves, soil, and rainwater runoff in tea plantations of the green tea variety 'Fenglv' (Camellia sinensis Yutakmitor). Field trials using bifenthrin, deltamethrin, and chlorfenapyr were conducted in the tea plantations of Yucha Village, Shaoxing City, Zhejiang Province in China. The local regular dose and 30% dose reduction of bifenthrin, deltamethrin, and chlorfenapyr were considered as the experimental treatments group, which included dosages of bifenthrin at 150 mL·hm^-2 and 105 mL·hm^-2, deltamethrin at 750 mL·hm^-2 and 525 mL·hm^-2, and chlorfenapyr at 750 mL·hm^-2 and 525 mL·hm^-2, respectively. Samples of tea leaves and soil were collected on the 1^st, 3^rd, 7^th, and 10^th day after spraying, and rainwater runoff was similarly collected on the 4^th and 8^th day after spraying. The data related to insecticide residues in all the collected samples were used to evaluate the behavioral pattern of residue and risk assessment of the three insecticides. The results indicated that no significantly different residues present in fresh tea leaves was observed sprayed with regular dosage and 30%-reduced dose. The half-lives of bifenthrin in fresh tea leaves sprayed with regular dosage and reduced dosage were 5.89 d and 4.61 d, respectively, and the half-lives of deltamethrin with regular dosage and reduced dosage were 5.75 d and 2.55 d, respectively; and those of chlorfenapyr with regular dosage and reduced dosage were 3.72 d and 2.70 d, respectively. The residue levels of bifenthrin, deltamethrin, and chlorfenapyr in soil were lower than the primary standard value (≤ 0.05 mg·kg^-1) of organochlorine insecticide, hexachlorocyclohexane, as stated in Environmental Quality Standard for Soils (GB15618-1995). The residue levels of bifenthrin and chlorfenapyr in rainwater runoff were lower than the value (≤ 0.005 mg·L^-1) of organochlorine insecticide hexachlorocyclohexane as stated in Standards for Drinking Water Quality (GB5749-2006). The residue levels of deltamethrin in rainwater runoff were lower than the value (≤ 0.02 mg·L^-1) of deltamethrin as stated in Standards for Drinking Water Quality (GB5749-2006). Dietary exposure risk assessment referred to the risk assessment of exposure to insecticides and other harmful substances ingested through food. The results related to the assessment of risk of dietary exposure to the three insecticides in tea indicated that the maximum exposures of bifenthrin, deltamethrin and chlorfenapyr were 0.5×10^-4-1.7×10^-4, 1.0×10^-6-7.3×10^-6, 1.0×10^-5-8.3×10^-5 mg·kg^-1(bw)·d^-1. Risk quotient was expressed as the ratio of maximum exposure to acceptable daily intake. The risk quotients of bifenthrin, deltamethrin and carbonitrile were 0.005-0.017, 0.000 2-0.001, 0.000 2-0.003, respectively, which meant the risk to consumers was within an acceptable range. Reducing sprayed dosages of the above three insecticides in the tea plantations made no significant differences to the residues in tea and the environment.
Key words:Insecticide residues/
Tea/
Soil/
Rainfall-runoff/
Insecticide reduction

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图1喷施后不同时间不同施用剂量联苯菊酯、溴氰菊酯和虫螨腈在茶鲜叶中的残留
不同小写字母表示喷药后同一天常用剂量和减施剂量处理间差异显著(P < 0.05)。
Figure1.Residues of bifenthrin (A), deltamethrin (B) and chlorfenapyr (C) with different spraying doses in fresh tea leaves in different times after spraying
Different lowercase letters for the same days after spraying show significant differences between treatments of common dose and reduced dose (P < 0.05).

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图2喷药后不同时间不同施用剂量联苯菊酯(A)、溴氰菊酯(B)和虫螨腈(C)在茶鲜叶中的残留相比喷药后1 d的消解率
不同小写字母表示喷药后同一天常用剂量和减施剂量处理间差异显著(P < 0.05)。
Figure2.Residue reduction rates of bifenthrin (A), deltamethrin (B) and chlorfenapyr (C) with different spraying doses in fresh tea leaves in different times after spraying compared to the first day after spraying
Different lowercase letters for the same days after spraying show significant differences between treatments of common dose and reduced dose (P < 0.05).

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表1径流采集期间试验区气温和降雨量
Table1.Temperature and rainfall in the study area during runoff collection periods of the experiment

	联苯菊酯Bifenthrin		溴氰菊酯Deltamethrin		虫螨腈Chlorfenapyr
	喷药后4 d 4 days after spraying	喷药后8 d 8 days after spraying	喷药后4 d 4 days after spraying	喷药后8 d 8 days after spraying	喷药后4 d 4 days after spraying	喷药后8 d 8 days after spraying
最高气温 Maximum temperature (℃)	31.6	22.1	26.0	27.2	34.1	36.2
最低气温 Minimum temperature (℃)	22.7	19.3	21.9	22.2	28.4	26.8
降雨量Rainfall (mm)	4.4	11.0	7.3	13.7	12.6	5.1

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表2喷药后不同施用剂量联苯菊酯、溴氰菊酯和虫螨腈在茶鲜叶中的消解动力学参数
Table2.Dissipation dynamic parameters of bifenthrin, deltamethrin and chlorfenapyr with different spraying doses in fresh tea leaves

杀虫剂 Pesticides	处理 Treatment	动态方程 Dynamic equation	相关系数R² Correlation coefficient	半衰期 Half-life period (d)
联苯菊酯 Bifenthrin	减施剂量Reduced dose	$C_{t}=0.622 \mathrm{e}^{-0.1504 t}$	0.993 4	4.61
联苯菊酯 Bifenthrin	常用剂量Common dose	$C_{t}=0.792 \mathrm{e}^{-0.1177 t}$	0.981 4	5.89
溴氰菊酯 Deltamethrin	减施剂量Reduced dose	$C_{t}=0.021 \mathrm{e}^{-0.1206 t} $	0.954 6	5.75
溴氰菊酯 Deltamethrin	常用剂量Common dose	$ C_{t}=0.031 \mathrm{e}^{-0.2714 t} $	0.895 1	2.55
虫螨腈 Chlorfenapyr	减施剂量Reduced dose	$ C_{t}=0.230 \mathrm{e}^{-0.2565 t}$	0.949 0	2.70
虫螨腈 Chlorfenapyr	常用剂量Common dose	$ C_{t}=0.341 \mathrm{e}^{-0.1865 t}$	0.928 2	3.72

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表3喷药后不同时间不同施用剂量联苯菊酯、溴氰菊酯和虫螨腈后茶鲜叶的膳食暴露量、风险商和风险概率
Table3.Dietary exposure, risk quotient and risk probability of bifenthrin, deltamethrin and chlorfenapyr with different spraying doses in fresh tea leaves in different times after spraying

杀虫剂 Pesticides	处理 Treatment	喷药后天数 Days after spraying (d)	茶鲜叶残留量 Residue in fresh tea leaves (mg·kg^-1)	估计暴露量 Estimated exposure dose [mg?kg^-1(bw)?d^-1]	风险商 Risk quotient	风险概率 Risk probability (%)
联苯菊酯 Bifenthrin	减施剂量 Reduced dose	1	0.652	1.39E-04	0.014	1.391
	减施剂量 Reduced dose	7	0.238	5.08E-05	0.005	0.508
	常用剂量 Common dose	1	0.808	1.72E-04	0.017	1.724
	常用剂量 Common dose	7	0.442	9.43E-05	0.009	0.943
溴氰菊酯 Deltamethrin	减施剂量 Reduced dose	1	0.024	5.12E-06	0.001	0.010
	减施剂量 Reduced dose	7	0.005	1.07E-06	0.000 2	0.002
	常用剂量 Common dose	1	0.034	7.25E-06	0.001	0.015
	常用剂量 Common dose	7	0.009	1.92E-06	0.000 4	0.004
虫螨腈 Chlorfenapyr	减施剂量 Reduced dose	1	0.270	5.76E-05	0.002	—
	减施剂量 Reduced dose	7	0.032	6.83E-06	0.000 2	—
	常用剂量 Common dose	1	0.390	8.32E-05	0.003	—
	常用剂量 Common dose	7	0.048	1.02E-05	0.000 4	—
风险商 < 1, 对人体的慢性风险可接受; 风险概率 < 100%, 对人体的急性风险可接受。Risk quotient < 1, the chronic risk to the human body is acceptable; Risk probability < 100%, the acute risk to the human body is acceptable.

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表4喷药后不同时间不同施用剂量联苯菊酯、溴氰菊酯和虫螨腈在土壤中的残留
Table4.Residues of bifenthrin, deltamethrin and chlorfenapyr with different spraying doses in soil in different times after spraying

mg·kg^-1
杀虫剂 Pesticides	处理 Treatment	土壤深度 Soil depth (cm)	喷药前 Before spraying	喷药后1 d 1 day after spraying	喷药后3 d 3 days after spraying	喷药后7 d 7 days after spraying	喷药后10 d 10 days after spraying
联苯菊酯 Bifenthrin	减施剂量 Reduced dose	0~20	ND	ND	ND	ND	ND
	减施剂量 Reduced dose	20~40	ND	ND	ND	ND	ND
	常用剂量 Common dose	0~20	ND	ND	ND	ND	ND
	常用剂量 Common dose	20~40	ND	ND	ND	ND	ND
	空白对照 Control	0~20	ND	ND	ND	ND	ND
	空白对照 Control	20~40	ND	ND	ND	ND	ND
溴氰菊酯 Deltamethrin	减施剂量 Reduced dose	0~20	ND	0.005±0.001a	0.005±0.001a	0.003±0.001a	0.005±0.001a
	减施剂量 Reduced dose	20~40	ND	0.003±0.001a	0.005±0.001a	0.006±0.001a	0.004±0.001a
	常用剂量 Common dose	0~20	ND	0.004±0.001a	0.005±0.001a	0.004±0.001a	0.005±0.001a
	常用剂量 Common dose	20~40	ND	0.008±0.002a	0.004±0.001a	0.007±0.001a	0.005±0.001a
	空白对照 Control	0~20	ND	ND	ND	ND	ND
	空白对照 Control	20~40	ND	ND	ND	ND	ND
虫螨腈 Chlorfenapyr	减施剂量 Reduced dose	0~20	ND	0.007±0.001a	0.006±0.001a	0.012±0.003a	0.007±0.001a
	减施剂量 Reduced dose	20~40	ND	0.011±0.002a	0.006±0.002a	0.004±0.001a	0.007±0.003a
	常用剂量 Common dose	0~20	ND	0.003±0.001a	0.004±0.001a	0.031±0.006b	0.008±0.002a
	常用剂量 Common dose	20~40	ND	0.011±0.002a	0.005±0.001a	0.007±0.002a	0.001±0.001a
	空白对照 Control	0~20	ND	ND	ND	ND	ND
	空白对照 Control	20~40	ND	ND	ND	ND	ND
ND表示未检出, 同列同一种杀虫剂不同小写字母表示不同处理间差异显著(P < 0.05)。ND indicates not detected. Different lowercase letters in the same column for the same pesticides indicate significant differences among different treatments (P < 0.05).

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表5喷药后不同时间不同施用剂量联苯菊酯、溴氰菊酯和虫螨腈在降雨径流中的残留
Table5.Residues of bifenthrin, deltamethrin and chlorfenapyr with different spraying doses in rainfall-runoff in different times after spraying

mg·L^-1
杀虫剂 Pesticides	处理 Treatment	喷药前 Before spraying	喷药后4 d 4 days after spraying	喷药后8 d 8 days after spraying
联苯菊酯 Bifenthrin	减施剂量 Reduced dose	ND	0.002±0.003a	0.002±0.001a
	常用剂量 Common dose	ND	0.002±0.001a	0.002±0.001a
	空白对照 Control	ND	ND	ND
溴氰菊酯 Deltamethrin	减施剂量 Reduced dose	ND	0.001±0.001a	0.001±0.001a
	常用剂量 Common dose	ND	0.001±0.001a	0.002±0.001a
	空白对照 Control	ND	ND	ND
虫螨腈 Chlorfenapyr	减施剂量 Reduced dose	ND	ND	0.001±0.001a
	常用剂量 Common dose	ND	ND	ND
	空白对照 Control	ND	ND	ND
ND表示未检出, 同列同一种杀虫剂不同小写字母表示不同处理间差异显著(P < 0.05)。ND indicates not detected. Different lowercase letters in the same column for the same pesticides indicate significant differences among different treatments (P < 0.05).

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