Contamination and health risk assessment of dried bamboo shoots in Zhejiang Province

ZHANG Youqing; LI Kaili; LIU Xingquan; WANG Zhaojun; WU Jun; LU Pin

doi:10.11833/j.issn.2095-0756.2017.01.024

Volume 34 Issue 1

Jan. 2017

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ZHANG Youqing, LI Kaili, LIU Xingquan, WANG Zhaojun, WU Jun, LU Pin. Contamination and health risk assessment of dried bamboo shoots in Zhejiang Province[J]. Journal of Zhejiang A&F University, 2017, 34(1): 178-184. doi: 10.11833/j.issn.2095-0756.2017.01.024

Citation:

ZHANG Youqing, LI Kaili, LIU Xingquan, WANG Zhaojun, WU Jun, LU Pin. Contamination and health risk assessment of dried bamboo shoots in Zhejiang Province[J]. Journal of Zhejiang A&F University, 2017, 34(1): 178-184. doi: 10.11833/j.issn.2095-0756.2017.01.024

Contamination and health risk assessment of dried bamboo shoots in Zhejiang Province

doi: 10.11833/j.issn.2095-0756.2017.01.024

ZHANG Youqing^{1,2
,},
LI Kaili¹,
LIU Xingquan^{1
,
,},
WANG Zhaojun²,
WU Jun³,
LU Pin⁴

1.
Key Laboratory for Quality Improvement of Agricultural Products of Zhejiang Province, Zhejiang A & F University, Lin'an 311300, Zhejiang, China
2.
Lin'an Quality and Measurement Monitoring Center, Lin'an 311300, Zhejiang, China
3.
Lin'an Center for Disease Control and Prevention, Lin'an 311300, Zhejiang, China
4.
Jinhua Quality and Technical Supervision and Inspection Institute, Jinhua 321000, Zhejiang, China

Received Date: 2016-03-08
Rev Recd Date: 2016-04-10
Publish Date: 2017-01-20

Abstract

This study was conducted to determine the current level of heavy metal (arsenic, lead), sulfur dioxide and pesticide residue pollution risks with dried edible bamboo shoots in Zhejiang Province and to provide hygienic standards. Dried bamboo shoots were collected at markets in Zhejiang Province from 2013-2014. Analysis included a comprehensive pollution index for harmful pollutants, a target hazard quotient (THQ), and a human dietary intake risk analysis. Results showed no pesticide residues with an average content (in μg·g^-1) of arsenic (0.09), lead (0.42), and sulfur dioxide (10.58). From the comprehensive pollution index, dried bamboo shoots (Phyllostachys edulis) were within safe levels. The degree of contamination for harmful substances of 165 dried bamboo shoots was Pb > SO₂ > As. The THQ revealed the possibility of human health risks with maximum levels of As and Pb. From TTHQ, dried bamboo shoots may have a negative impact to the human body. The human dietary intake risk analysis showed that overall, dried bamboo shoots were safe in Zhejiang except resident exposure of Pb beyond recommended limits only in a few areas.
- dried bamboo shoots,
- Phyllostachys edulis,
- heavy metals,
- sulfur dioxide,
- risk assessment

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沈阳化工大学材料科学与工程学院沈阳 110142

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新鲜竹笋在采收后常温下放置容易老化，并且营养价值容易降低，所以常常将其加工成笋干制品。毛笋Phyllostachys edulis的笋干肉厚质脆，清香味美，尤其是纤维细嫩且含量丰富，是人们十分喜爱的食品^[1]。二氧化硫超标是现在笋制品质量安全的主要问题之一，时有报道笋制品中的二氧化硫严重超标问题^[2]。二氧化硫作为漂白剂是由于其具有还原性，能与食品中含有的有色物质结合形成不稳定的无色化合物；防腐保鲜，则是由于其可抑制食品中微生物的生长起到防腐保鲜的作用^[3]；抗氧化则主要是因为其抑制酶促褐变与非酶褐变防止食品被氧化褐变^[4-5]。基于二氧化硫的上述作用，在食品保藏和加工中被广泛运用^[6-8]。此外，由于工业“三废”(废水、废气、固体废弃物)及汽车尾气排放、化肥和杀虫剂的使用^[9]，导致重金属进入土壤，经过植物根系吸收并最终在体内富集。长期摄入会影响生长发育并引发多种疾病，严重危害人体健康^[10]。由于竹笋干的质量问题，目前中国竹笋干仅1%的产品销往国外^[11]。浙江省既是中国竹笋干的生产大区，也是消费大区。本研究根据浙江省居民食用竹笋干情况，对检测结果进行风险评估，能够对食用竹笋制品的居民健康提供参考。

1. 材料与方法

1.1. 材料采集及问卷调查

2014年5月初，对浙江省杭州、宁波、丽水等重点生产毛笋干的地区采样。

2014年1月和7月，以面对面问卷询问调查的方法，在竹笋加工产品消费集中的地区进行随机调查，收到有效样本量3 657份，其中食用毛笋干的有效样本量有1 494份。

1.2. 试验方法

二氧化硫检测中，先将笋制品取出一定量用匀浆机磨碎。称取5 g均匀样品采用蒸馏法蒸馏，之后用碘标准滴定溶液(0.01 mol·L^-1)滴定至变蓝色且在30 s内不褪色为止。

本研究检测了砷和铅2种重金属，样品采用硝酸-高氯酸(HNO₃-HClO₄)加热消解，金属元素采用氢化物发生-原子荧光光谱法(Agilent 7500a电感耦合等离子体质谱仪)测定，检测条件参考文献[12]。

依据NY/T 1048-2012《绿色食品笋及笋制品》的要求检测了敌敌畏、甲胺磷、乙酰甲胺磷、氧化乐果、乐果、毒死蜱、甲基对硫磷、马拉硫磷、杀螟硫磷、水胺硫磷、杀扑磷等11种有机磷农药；依据NY/T 761-2008《蔬菜和水果中有机磷、有机氯、拟除虫菊酯和氨基甲酸酯类农药多残留的测定》的规定检测了联苯菊酯、氯氰菊酯、溴氰菊酯、氰戊菊酯、甲氰菊酯、氯氟氰菊酯、氟氯氰菊酯等7种拟除虫菊酯类农药。

1.3. 评价标准

本研究采用GB 2762-2012《食品安全国家标准食品中污染物限量》和NY/T 1048-2012《绿色食品笋及笋制品》中对砷、铅和二氧化硫规定的限值0.5，1.0和200.0 mg·kg^-1作为评价标准。

1.4. 笋制品二氧化硫及重金属污染评价方法

笋制品污染等级评价依据NY/T398-2000《农、畜、水产品污染监测技术规范》规定进行，采用单因子法。目前，该方法已在蔬菜污染评价方面得到应用^[13-14]。

式(1)中：P_i为竹笋干中有害物质的单项污染指数，C_i为竹笋干中有害物质的实际测量值，S_i为竹笋干中有害物质的评价标准。当P_i≤1时，表示笋制品未受污染；P_i＞1时，表示笋制品收到污染，其值越大表示受污染程度越重^[15]。综合污染指数计算方法如下：

式(2)中：P_综合为综合污染指数，P_max为单项污染指数最大值，P_ave为各单项污染指数P_i的平均值。通常设定综合污染指数P_综合≤0.7为安全等级，P_综合=1.0为警戒限，P_综合≤2.0为轻污染，P_综合≤3.0为中污染，P_综合＞3.0为重污染。

1.5. 健康风险评价方法

竹笋加工产品中二氧化硫及重金属的暴露量评估计算公式^[2]：

式(3)中：D_EED为竹笋加工产品中有害物质(即二氧化硫和重金属)的暴露量(μg·kg^-1)，C为竹笋加工产品中有害物质的暴露质量分数(μg·g^-1)，R_FIR为竹笋加工产品的日摄入量(g·d^-1)，P_i为竹笋加工产品的加工处理因子，E_i为竹笋加工产品的可食用部分因子，S_ABS为肠胃对竹笋加工产品的吸收系数，f_EF为食用竹笋加工产品的暴露频率(d·a^-1)，t_ED为食用竹笋加工产品的暴露持续时间(a)，W_BW为样本人群的体重(kg)，t_AT为拉平时间(t_ED×365 d·a^-1)。

1.6. 目标危害系数

目标危害系数Q_THQ是美国环境保护署推荐采用的健康风险评价模型，计算方法^[16]：

式(4)中：Q_THQ为目标危险系数，D_EED为竹笋加工产品中有害物质的暴露量(μg·kg^-1)，D_RfD为口服参考剂量(μg·kg^-1·d^-1)。

污染物对人体健康的影响往往是多种元素共同作用的，用总目标危险系数Q_TTHQ表示为^[17]：

若Q_TTHQ≤1.0，则表示没有明显的负面影响；若Q_TTHQ＞1.0，则表示对人体健康产生负面影响的可能性很大；若Q_TTHQ＞10.0，则表明存在慢性毒性效应^[18]。

目前，联合国粮农组织(FAO)和世界卫生组织(WHO)对部分重金属提出了人均日摄入可允许限量标准(provisional tolerable daily intake, PTDI)，FAO和WHO食品添加剂联合专家委员会(JECFA)还对部分重金属提出了人体最大允许摄入量限值^[19]。

2. 结果与分析

2.1. 毛笋干中有害物质

检测结果表明：165份毛笋干中均未检测到农药残留，且不同地区之间重金属和二氧化硫之间存在差异。只有杭州地区毛笋干中砷和铅超标，超标率分别为13.16%和7.89%，且最大值分别为限量标准的2.76和15.07倍。具体情况见表 1。

地区	样本数/个	砷/(μg.g^-1)		铅/(μg·g^-1)		二氧化硫/(μg·g^-1)
地区	样本数/个	范围值	均值%标准差	范围值	均值%标准差	范围值	均值%标准差
杭州市	38	0.00~1.38	0.20±0.32	0.00~15.07	0.73±2.43	0.95~29.00	10.77±6.89
宁波市	16	0.01~0.15	0.07±0.04	0.03~0.91	0.39±0.31	7.60~18.00	12.84±3.54
湖州市	23	0.02~0.15	0.06±0.03	0.02~0.99	0.35±0.28	1.00~28.00	6.83±6.32
金华市	11	0.01~0.28	0.06±0.07	0.00~0.99	0.28±0.36	2.00~21.00	11.13±5.55
绍兴市	22	0.02~0.13	0.07±0.04	0.05~1.00	0.35±0.25	0.96~21.00	9.53±5.14
台州市	10	0.02~0.05	0.04±0.01	0.00~0.98	0.18±0.30	4.80~22.00	11.05±5.65
温州市	8	0.02~0.12	0.07±0.04	0.02~0.95	0.52±0.34	3.20~23.00	13.56±8.24
衢州市	18	0.00~0.08	0.04±0.02	0.00~0.93	0.25±0.24	0.86~23.00	8.77±6.84
丽水市	19	0.01~0.25	0.06±0.06	0.03~0.62	0.33±0.17	1.50~24.00	13.92±7.00
总体	165	0.00~1.38	0.09±0.17	0.00~15.07	0.42±1.19	0.86~29.00	10.58±6.49

Table 1. Concentrations of heavy metals and SO₂ in bamboo products in different areas

2.2. 毛笋干中有害物质污染评价

结合式(1)和式(2)，计算得到不同地区毛笋干中各有害物质的单项污染指数均值。从表 2的结果可以看出：杭州、宁波、湖州、金华、绍兴、台州、温州、衢州和丽水等地的毛笋干都没有受到重金属和二氧化硫的污染，且综合指数表明均为安全等级产品。

地区	单项平均污染指数			综合指数
地区	砷	铅	二氧化硫	综合指数
杭州市	0.40	0.73	0.05	0.59
宁波市	0.13	0.39	0.06	0.31
湖州市	0.12	0.35	0.03	0.27
金华市	0.12	0.28	0.06	0.23
绍兴市	0.14	0.35	0.05	0.28
台州市	0.07	0.18	0.06	0.15
温州市	0.14	0.52	0.07	0.41
衢州市	0.07	0.25	0.04	0.20
丽水市	0.11	0.33	0.07	0.26
总体	0.18	0.42	0.21	0.35

Table 2. Single factor index and integrated pollution index of heavy metals and SO₂ of contaminated bamboo products

2.3. 居民健康风险评估

根据调查问卷的统计结果，得到不同地区人群毛笋干的日摄入量。从摄入量平均值看温州地区最多，达81.87 g·d^-1，其次多到少依次为丽水、绍兴、嘉兴、金华、湖州、舟山、宁波、杭州、台州、衢州和省外地区。具体结果见表 3。

地区	样本数/个	日摄入量/(g·d^-1)
地区	样本数/个	范围	均值±标准差	P₅₀	P₇₅	P₉₀
杭州市	172	0.07~757.58	15.05±82.50	0.83	7.14	10.71
宁波市	56	0.83~75.76	23.08±29.24	7.14	25.00	75.76
金华市	208	0.07~454.55	30.96±81.21	2.50	21.43	75.76
丽水市	300	0.14~454.55	37.68±97.03	2.5	5.00	100.00
湖州市	66	0.07~150.00	26.69±44.00	0.83	50.00	50.00
嘉兴市	12	0.07~150.00	36.67±56.52	0.83	50.00	150.00
衢州市	85	0.07~75.76	8.06±18.07	0.28	7.14	21.43
绍兴市	107	0.07~700.00	37.32±102.72	7.14	8.33	100.00
台州市	219	0.07~233.33	14.54±41.13	0.83	5.00	42.86
温州市	133	0.07~757.58	81.87±192.45	7.14	50.00	250.00
舟山市	131	0.07~227.27	24.07±39.62	3.57	50.00	75.76
省外地区	5	0.14~7.14	3.13±3.67	0.83	7.14	7.14
总体	1 494	0.07~757.58	30.62±92.17	2.50	10.71	75.76
说明: P₅₀, P₇₅, P₉₀分别表示第50百分位数，第75百分位数，第90百分位数的摄人量。

Table 3. Sample population intake

由表 1得到：毛笋干中砷、铅和二氧化硫质量分数平均值/最大值分别为0.09/1.38，0.42/15.07，10.58/29.00 μg·g^-1。中国男性人均期望寿命为69.6岁，女性为73.3岁，以两者的平均值71.4岁作为期望寿命^[20]；将期望寿命作为暴露年限^[21]，取t_ED=71.4 a，则t_AT=71.4×365 d·a^-1；口服参考计量D_RfD对砷、铅^[22]和二氧化硫分别取0.3，4.0和700.0 μg·kg^-1·d^-1(表 4)。

参数	单位	定义	计算结果
C(竹笋干)	μg·g^-1	笋制品中重金属砷(As)，重金属铅(Pb)和二氧化硫(SO₂)暴露质量分数。	C_As上限值=1.38, C_As平均值=0.09。C_Pb上限值=15.07, C_Pb平均值=0.42。C_SO₂上限值=29.00, C_SO₂平均值=10.58。
P_i		具体食物在从原料加工成食品过程中的转化系数。	笋制品从保鲜竹笋、方便竹笋和竹笋干加工成可以食用的笋时基本无损耗，故P_i=1。
E_i		食品在食用时能完全被人食用部分的系数。	E_i=1。
S_ABS		重金属砷(As)和重金属铅(Pb)随着食品的食用最后能被人体肠胃吸收的系数。	S_ABS=¹。
t_ED	a	暴露年限。	t_ED=71.4。
f_EF	d·a^-1	暴露频率。	f_EF=365。
t_AT	d	拉平时间。	t_AT=71.4×365。
D_RfD	μg.kg^-1·d^-1	口服参考剂量。	D_RfDAs=3×10^-4，D_RfDPb=3×10^-4。

Table 4. The model parameters of sample population risk assessment

由表 3和式(3)以及结合模型(表 4)得出样本人群食用竹笋加工产品的暴露量(表 5和表 6)。

地区	样本数/个	砷/(μg.kg^-1·d^-1)		铅/(μg.kg^-1·d^-1)		二氧化硫/(μg.kg^-1·d^-1)
地区	样本数/个	平均	最大	平均	最大	平均	最大
杭州市	172	0.05	0.36	0.19	3.97	2.84	7.65
宁波市	56	0.04	0.08	0.20	0.46	6.53	9.15
金华市	208	0.03	0.15	0.15	0.53	5.92	11.16
丽水市	300	0.03	0.13	0.17	0.32	7.08	12.20
湖州市	66	0.03	0.08	0.19	0.55	3.77	15.44
嘉兴市	12	0.07	1.07	0.33	11.72	8.23	22.56
衢州市	85	0.01	0.01	0.04	0.14	1.31	3.44
绍兴市	107	0.04	0.08	0.22	0.64	6.06	13.35
台州市	219	0.01	0.01	0.05	0.27	3.05	6.07
温州市	133	0.09	0.16	0.70	1.28	18.21	30.88
舟山市	131	0.03	0.49	0.15	5.36	3.76	10.32
省外地区	5	0.01	0.09	0.03	0.95	0.67	1.84
总体	1 494	0.05	0.75	0.23	8.22	5.77	15.81

Table 5. Exposure of the sample population in different regions

重金属和二氧化硫	暴露量/(μg.kg^-1·d^-1)
重金属和二氧化硫	P₅₀平均	P₅₀最大	P₇₅平均	P₇₅最大	P₉₀平均	P₉₀最大	P₉₅平均	P₉₅最大
砷	0.00	0.05	0.02	0.25	0.12	1.88	0.21	3.18
铅	0.02	0.58	0.08	2.69	0.57	20.55	0.97	34.78
二氧化硫	0.41	1.11	1.89	5.18	14.43	39.55	24.42	66.92

Table 6. Exposure of the sample population at different point

联合食品添加剂专家委员会(JECFA)和FAO/WHO分别提出砷最大允许摄入量和铅人均日摄入可允许限量(PTDI)分别为2.00 μg·kg^-1·d^-1和200.00 μg·d^-1，以60.0 kg成人体质量计算，得出铅最大允许摄入量为3.33 μg·kg^-1·d^-1。FAO，WHO和JECFA对二氧化硫类物质作为食品添加剂的危险性评估为：二氧化硫的日容许摄入量(ADI)为0~0.70 mg·kg^-1·d^-1，人体少量摄取亚硫酸盐时，会在体内迅速氧化成硫酸盐，排出体外，1 d摄取1.00 g也未发现任何障碍，若摄取4.00~6.00 g，对肠胃有损坏，能造成激烈腹泻、头痛。二氧化硫取700.00 μg·kg^-1·d^-1。结合表 5和表 6从平均值看，样本人群食用毛笋干砷、铅和二氧化硫的暴露量远远低于限量标准。从最大值看，只有杭州、嘉兴和舟山地区铅超出最大允许摄入量，分别为标准的1.2，3.5和1.6倍，且在P₇₅和P₉₀之间暴露量跨越非常明显，表明大致有1/3的人群食用毛笋干存在铅食用过多的危险。

根据上述参数及式(4)和式(5)可以计算得到长期食用这些毛笋干可能带来的身体受损风险(表 7)，其中从有害物质实际检测的平均值来看砷、铅和二氧化硫可造成的目标危害系数Q_THQ总体为0.17，0.06和0.01，总目标危害系数Q_TTHQ为0.24，均不对人体产生任何负面影响。从最大值看，Q_THQ总体为2.50，2.06和0.02，表明毛笋干中的砷和铅可能对人体健康产生影响(即P_i＞1)，其中杭州产毛笋干中的砷为1.20，嘉兴砷和铅分别为3.57和2.93，舟山砷和铅分别为1.63和1.34。从Q_TTHQ最大值来看总体(4.58)，杭州(2.20)，嘉兴(6.53)和舟山(2.98)均可能对人体健康产生负面影响。

地区	样本数/个	^QTHQ平均			^QTHQ最大			^QTTHQ
地区	样本数/个	砷	铅	二氧化碳	砷	铅	二氧化碳	平均	最大
杭州市	172	0.17	0.05	0.00	1.20	0.99	0.01	0.22	2.20
宁波市	56	0.13	0.05	0.01	0.27	0.12	0.01	0.19	0.40
金华市	208	0.10	0.04	0.01	0.50	0.13	0.02	0.15	0.65
丽水市	300	0.10	0.04	0.01	0.43	0.08	0.02	0.15	0.53
湖州市	66	0.10	0.05	0.01	0.27	0.14	0.02	0.16	0.43
嘉兴市	12	0.23	0.08	0.01	3.57	2.93	0.03	0.32	6.53
衢州市	85	0.03	0.01	0.00	0.03	0.04	0.00	0.04	0.07
绍兴市	107	0.13	0.06	0.01	0.27	0.16	0.02	0.20	0.45
台州市	219	0.03	0.01	0.00	0.03	0.07	0.01	0.04	0.11
温州市	133	0.30	0.18	0.03	0.53	0.32	0.04	0.51	0.89
舟山市	131	0.10	0.04	0.01	1.63	1.34	0.01	0.15	2.98
省外地区	5	0.03	0.01	0.00	0.30	0.24	0.00	0.04	0.54
总体	1 494	0.17	0.06	0.01	2.50	2.06	0.02	0.24	4.58

Table 7. Dried bamboo shoots target hazards caused by harmful substances coefficient

3. 结论

在浙江省采样的165份毛笋干中未检测到有农药的残留，且这些毛笋干中只有杭州地区砷和铅超标，超标率分别为13.16%和7.89%，且最大值分别为限量标准的2.76倍和15.07倍，其余均在限量范围之内。

从单项污染指数来看，砷的范围为0.07~0.40，铅的范围为0.18~0.73，二氧化硫的范围为0.03~0.07，综合污染指数为0.15~0.59，均未受到污染。

成人食用毛笋干进入人体的有害物质砷和二氧化硫的暴露量远远低于2.00和700.00 μg·kg^-1·d^-1的限量标准，处于安全范围。铅的最大值表明有部分人群存在铅摄入过量的可能。

毛笋干中有害污染物砷和铅相应的目标危害系数Q_THQ的平均值和最大值对人体具有潜在健康风险(Q_THQ＞1)的可能。从总目标危害系数Q_TTHQ看，毛笋干对人体可能会产生一定负面影响(即Q_TTHQ＞1)。

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Contamination and health risk assessment of dried bamboo shoots in Zhejiang Province

doi: 10.11833/j.issn.2095-0756.2017.01.024