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2021, 38(5):467-472.doi:10.13213/j.cnki.jeom.2021.20575

Health risk assessment of acrylamide contamination in fried and baked foods from 2009 to 2016 in Shanghai residents


Shanghai Municipal Center for Disease Control and Prevention, Shanghai 200336, China

Received: 2020-12-10;  Accepted:2021-04-06;  Published: 2021-06-07

Fund project: This study was funded

Corresponding Author: WU Chunfeng, Email: wuchunfeng@scdc.sh.cn  

Ethics approval  Obtained

Competng interests  None declared

[Background] Acrylamide has attracted much attention since it was found in food in 2002. Acrylamide is formed in high-temperature fried starch-rich food during the Maillard reaction, and has been identified as a teratogenic, carcinogenic, and neurotoxic compound.

[Objective] This study is designed to assess the health risk of exposure to acrylamide related to the consumption of retail fried and baked foods from Shanghai markets using the food consumption data and the data of acrylamide contamination in these foods.

[Methods] A stratified random sampling method was used to select fried and baked food samples, and gas chromatography-mass spectrometry was used to determine acrylamide in food samples. Food consumption was investigated by food frequency questionnaire (FFQ). Population's probability distributions of acrylamide exposure were assessed by@Risk 7.5 software and Monte Carlo simulation algorithm. According to the dietary intake assessment model, the method of low-dose extrapolation was applied to the carcinogenic and non-carcinogenic risk assessments of exposure to acrylamide related to the consumption of retail fried and baked foods.

[Results] The mean concentration of acrylamide in 1049 fried and baked food samples was 51.88μg·kg-1. Among different types of foods, the fried and puffed foods had the highest concentration of acrylamide (89.43μg·kg-1 in mean). The mean consumption of fried and baked foods by residents in Shanghai was 82.85 g·d-1. Among all investigated age groups, the juveniles (3-17 years old) had the highest consumption with a mean of 96.41g·d-1. The dietary exposure to acrylamide from fried and baked foods in Shanghai residents averaged 0.16 μg·kg-1·d-1 (average level) and the P95 exposure valued 0.41 μg·kg-1·d-1 (high level). Particularly, the average-and high-level exposure estimates for the juveniles (3-17 years old) were 0.24 and 0.59 μg·kg-1·d-1, respectively. In terms of non-carcinogenic effects, the proportions of at-risk residents defined as with an exposure higher than the reference dose were 0.60%, 2.60%, 0.40%, and 0.20% in the all age group, juveniles, young adults, and the elderly, respectively, and no risk in middle-aged adults and pregnant women. In terms of carcinogenic effects, the incremental lifetime cancer risks of the studied population at average level and high level of intake were 1.08×10-4 and 2.28×10-4, respectively.

[Conclusion] The Shanghai residents have a higher risk of impaired health due to exposure to acrylamide from fried and baked foods than residents in other regions of China. Children and adolescents at 3-17 years are at a high risk and should be highly concerned.

Key Words: fried and baked foods;  acrylamide;  population exposure;  risk assessment 

表 1

上海市售油炸焙烤类食品中丙烯酰胺质量分数

Table 1

Acrylamide concentration in retail fried and baked foods in Shanghai 单位(Unit): μg·kg-1

表 2

上海市不同人群对不同种类油炸焙烤类食品的消费量

Table 2

Consumption of fried and baked foods in different groups in Shanghai 单位(Unit): g·d-1

图 1

上海市居民油炸焙烤类食品中丙烯酰胺暴露量分布

Figure 1

Probability distribution of acrylamide intake from fried and baked foods in Shanghai residents

表 3

不同人群油炸焙烤类食品中丙烯酰胺暴露量分布

Table 3

Percentiles of acrylamide intake from fried and baked foods in different groups in Shanghai 单位(Unit): μg·kg-1·d-1

图 2

上海市居民油炸焙烤类食品丙烯酰胺暴露的非致癌性风险概率

Figure 2

Non-carcinogenic health risk of acrylamide intake from fried and baked foods in Shanghai residents

图 3

3~15岁人群油炸焙烤类食品中丙烯酰胺暴露量分布

Figure 3

Probability distribution of acrylamide intake from fried and baked foods in 3-15 years age group in Shanghai

图 4

16岁及以上人群油炸焙烤类食品中丙烯酰胺暴露量分布

Figure 4

Probability distribution of acrylamide intake from fried and baked foods in > 16 years age group in Shanghai

图 5

上海市居民油炸焙烤类食品中丙烯酰胺暴露的终生致癌风险累积分布图

Figure 5

Cumulative distribution of incremental lifetime cancer risk of acrylamide intake from fried and baked foods in Shanghai residents

表 4

上海市居民摄食油炸焙烤类食品接触丙烯酰胺终生致癌风险

Table 4

Incremental lifetime cancer risk of acrylamide intake from fried and baked foods in Shanghai residents

Reference

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Food Standards Agency. FSA study of acrylamide in food, background information and research findings[EB/OL]. [2020-10-10]. http://www.food.gov.uk/multimedia/pdfs/acrylamideback.pdf.

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IARC. Some industrial chemicals[R]. Lyon: International Agency for Research on Cancer, 1994.

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WHO. WHO to hold urgent expert consultation on acrylamide in food after findings of Swedish National Food Administration[J]. Cent Eur J Public Health, 2002, 10(4): 162, 173.

 
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WHO. Guidelines for drinking-water quality: fourth edition incorporating the first addendum[R]. Geneva: World Health Organization, 2017.

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LIU Y J, GU D H, PU Y H, et al. Coordination reduction effects on acrylamide formation of potato chips[J]. J Food Saf Qual, 2016, 7(1): 331-337.

 
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ZYZAK D V, SANDERS R A, STOJANOVIC M, et al. Acrylamide formation mechanism in heated foods[J]. J Agric Food Chem, 2003, 51(16): 4782-4787.

DOI: 10.1021/jf034180i
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WANG X Q, WU Y N, CHEN J S. Low-level data processing of food contamination monitoring[J]. Chin J Prev Med, 2002, 36(4): 278-279.

DOI: 10.3760/j:issn:0253-9624.2002.04.022
[8]

Food and Agriculture Organization of the United Nations. Principles and methods for the risk assessment of chemicals in food[M]. Beijing: People's Medical Publishing House, 2012.

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GUO YD, CHEN L, YUAN YH, et al. Dietary exposure and risk assessment of Aflatoxin B1 in corn-based foods in China using probabilistic approach[J]. Food Sci, 2013, 34(11): 24-27.

DOI: 10.7506/spkx1002-6630-201311006
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XIAO X, SUI H X. Study on risk assessment approaches of genotoxic carcinogens in food[J]. Chin J Food Hyg, 2018, 30(4): 425-429.

 
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USEPA. Toxicological review of acrylamide, EPA/635/R-07/009F[R]. Washington: U.S. Environmental Protection Agency, 2010.

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ZHOU P P, ZHAO Y F, LIU H L, et al. Dietary exposure of the Chinese population to acrylamide[J]. Biomed Environ Sci, 2013, 26(6): 421-429.

[13]

WHO. Evaluation of certain contaminants in food[J]. World Health Organ Tech Rep Ser, 2011(959): 1-105.

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WHO. Safety evaluation of certain contaminants in food[EB/OL]. [2020-09-17]. https://apps.who.int/iris/bitstream/handle/10665/276868/9789241660747-eng.pdf.

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EFSA. Results on acrylamide levels in food from monitoring years 2007-2009 and exposure assessment[J]. EFSA J, 2011, 9(4): 2133.

DOI: 10.2903/j.efsa.2011.2133
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WONG W W, CHUNG S W, LAM C H, et al. Dietary exposure of Hong Kong adults to acrylamide: results of the first Hong Kong Total Diet Study[J]. Food AdditContam Part A, 2014, 31(5): 799-805.

 
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LIU Z M, TSE L A, HO S C, et al. Dietary acrylamide exposure was associated with increased cancer mortality in Chinese elderly men and women: a 11-year prospective study of Mr. and Ms. OS Hong Kong[J]. J Cancer Res Clin Oncol, 2017, 143(11): 2317-2326.

DOI: 10.1007/s00432-017-2477-4
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我国各级医疗机构对儿童用基本药物剂型和规格的需求调查

丙烯酰胺易产生聚合作用形成助凝剂聚丙烯酰胺,自20世纪60年代以来,被广泛应用于水质净化处理、纸浆加工以及其他工业用途。丙烯酰胺可通过皮肤黏膜、呼吸道、消化道途径被人体吸收,具有神经毒性、遗传毒性和致癌性[1],早在1994年被国际癌症研究中心(International Agency for Research on Cancer,IARC)列为人类可能致癌物(ⅡA类)[2]。2002年,瑞典、英国等国家率先在一些高温油炸和烧烤的淀粉类食品中检出丙烯酰胺[1, 3],其质量浓度远远超过世界卫生组织(World Health Organization,WHO)规定的饮用水中丙烯酰胺0.5 μg·L-1的最大限值[4]。大量研究表明,食品中的丙烯酰胺主要来源于美拉德反应,在各类油炸、焙烤类高碳水化合物、低蛋白质的植物性食品中检出含量最高[5-6],对人类健康存在潜在危害风险。

我国有关人群膳食中丙烯酰胺暴露量评估的研究较少,但随着饮食结构和消费习惯的转变,尤其是上海地区,居民对于油炸面制品、蛋糕、面包等油炸焙烤类食品摄入量较高,通过食品摄入丙烯酰胺对人体产生的健康风险不容忽视。

1   对象与方法

1.1   污染量调查

1.1.1   样品来源

采用多阶段分层随机抽样的方法,综合考虑上海市各区人口数、地域面积、食品消费情况等因素,选择主要食品供应渠道的大中型超市、农贸市场、各类型餐饮单位为采样点。于2009—2016年间采集各类油炸焙烤类食品样品共1 049件,包括中式面制品(油条、油饼、麻花、方便面等)478件、焙烤食品(面包、饼干、糕点等)398件、油炸膨化小食品(薯条、薯片、膨化食品等)173件。

1.1.2   检测方法

参照GB 5009.204—2014《食品安全国家标准食品中丙烯酰胺的测定》,采用气相色谱-质谱法测定油炸焙烤类食品中丙烯酰胺。对于未检出的食品,检测值以1/2检出限计[7]

1.2   消费量调查

1.2.1   调查对象

采用多阶段分层随机抽样的方法,于2009年按经济水平、地理位置等因素,将上海16个区分为城区和郊区二层,分别从中经多阶段随机抽取常住户籍人口(居住满1年以上)共2325人作为调查样本人群,包括未成年人(3~17岁)701人、青年人(18~44岁)459人(孕妇除外)、中年人(45~59岁) 241人、老年人(> 60岁)525人、孕妇399人。

1.2.2   调查方法

采用统一自行设计的调查问卷,应用食物频率表法,入户调查上海市户籍常住居民油炸焙烤类食品消费量。

1.3   暴露量评估

采用联合国粮农组织和WHO推荐的食品化学物质膳食暴露评估方法[8],建立暴露量评估模型,$m_{\mathrm{EDI}}=m_{\mathrm{C}} \times I_{\mathrm{ad}} \times f_{\mathrm{PF}} \times m_{\mathrm{ing}} \times 10^{3} / \mathrm{m}_{\mathrm{BW}} $。式中:mEDI为暴露量(estimated daily intake,EDI),μg·kg-1·d-1mC为食品中污染量,μg·kg-1Iad为校正系数,无单位;fPF为加工因子,无单位;ming为每天食品消费量,g·d-1mBW为体重,kg。本研究采集的食品样品均为即食食品,不涉及食品烹调、加工等影响因素,研究中直接以样品中丙烯酰胺污染量进行计算,故校正系数与加工因子均取常数1。根据暴露量评估模型,运用@Risk7.5分析软件,分别对油炸焙烤类食品中丙烯酰胺污染量及食物消费量(以单位体重计)数据进行分布拟合。其中,污染量数据选择拟合后的最优函数分布Expon分布,食物消费量符合正态分布。以Monte Carlo原理进行10 000次非参数模拟,抽样方法设定为拉丁超立方抽样[9],分别以均数和第95百分位数作为一般摄入水平和高摄入水平。根据WHO的暴露评估方法,一般摄入水平用污染量和消费量的均数计算,而不推荐用P50,因为 P50往往会低估风险,均值评估结果能保护更大人群。

1.4   健康风险评估

基于遗传毒性物质风险评估方法的适用范围[10],参照美国环境保护署对于丙烯酰胺的风险评估研究[11],采用低剂量外推法分别对经口摄入丙烯酰胺的非致癌性效应及致癌性效应进行风险评估。其中致癌性效应评估仅分为3~15岁和 > 16岁两个区间。实际计算时,将本研究人群暴露量数据按照两个区间整理、拟合、计算。

1.4.1   非致癌性效应风险评估

丙烯酰胺非致癌效应(神经毒性效应)参考剂量(reference dose,Rfd)为2.00 μg·kg-1·d-1(以每kg体重计,余同)[11],按照中国膳食丙烯酰胺暴露量中油炸焙烤类食品的贡献率35.1%[12],上海市居民因食用油炸焙烤类食品而摄入丙烯酰胺的非致癌效应参考剂量为0.702 μg·kg-1·d-1。当暴露量高于该参考剂量时,则认为存在非致癌性效应风险。

1.4.2   致癌性效应风险评估

$ R_{\mathrm{HCR}}=m_{\mathrm{EDI}} \times f_{\mathrm{CSF}} \times f_{\mathrm{ADAF}} \times t_{\mathrm{ED}} \times t_{\mathrm{EF}} / t_{\mathrm{AT}}$。式中:RILCR为人群终生致癌风险(incremental lifetime cancer risk,ILCR),无单位;mEDI为人群暴露量,μg·kg-1·d-1fCSF为致癌斜率因子(carcinogenic slope factor,CSF),(mg·kg-1·d-1)-1fADAF为年龄依赖性调节因子(age dependent adjustment factors,ADAF),无单位;tED为暴露时间(exposure duration,ED),年;tEF为暴露频率(exposure frequency,EF),d· 年-1tAT为平均寿命(average time,AT)[11],年。该公式评估终生持续处于一定丙烯酰胺暴露水平所增加的癌症发生的概率。以引起10% 的实验雄性大鼠甲状腺肿瘤的基准剂量可信下限值(benchmark dose limit,BMDL)作为低剂量外推得到CSF为0.51(mg·kg-1·d-1)-1[12]。对于3~15岁少年儿童 fADAF取值为3,16岁及以上人群 fADAF取值为1。tED取各年龄段划分区间的暴露年数,tEF为365 d· 年-1tAT采用2017年上海市人口预期寿命83岁。参照美国环境保护署对于ILCR的风险判定标准,认为ILCR在1×10-6~ 1×10-4范围内时,其致癌效应风险是低风险;ILCR大于1×10-4时,其致癌效应风险属于具有较高的潜在风险。

1.5   统计学分析

数据由Microsoft Excel 2003录入,采用SAS 9.1.3进行统计分析。正态分布资料的比较采用ANOVA方差分析,两两比较采用SNK法;非正态分布资料的比较采用Kruskal-Wallis H秩和检验,两两比较采用Nemenyi法。检验水准α=0.05。

2   结果

2.1   油炸焙烤类食品中丙烯酰胺污染状况

上海市售1 049件油炸焙烤类食品中,有442件样品检出丙烯酰胺,检出率为42.14%。所有样本丙烯酰胺质量分数(后称:含量)均数为51.88 μg·kg-1,第95百分位数为212.40 μg·kg-1。不同种类食品中丙烯酰胺含量不全相同(χ2=13.02,P < 0.05),油炸膨化小食品中丙烯酰胺质量浓度最高,均数为89.43 μg·kg-1,第95百分位数为453.00 μg·kg-1(表 1)。

表1

上海市售油炸焙烤类食品中丙烯酰胺质量分数

Table1.

Acrylamide concentration in retail fried and baked foods in Shanghai 单位(Unit): μg·kg-1

2.2   油炸焙烤类食品人群消费水平

上海市常住居民油炸焙烤食品消费量均数为82.85 g·d-1,第95百分位数为211.82 g·d-1。居民对不同油炸焙烤类食品消费量不全相同(F=384.85,P < 0.05),中式米面制品消费量最高,焙烤食品次之,油炸膨化小食品消费量最低。

未成年人(3~17岁)、青年人(18~44岁)、中年人(45~59岁)、老年人(> 60岁)、孕妇油炸焙烤类食品消费量均数分别为96.41、83.59、69.67、72.97、79.14 g·d-1,不同人群油炸焙烤类食品消费量不全相同(F=7.14,P < 0.05),且未成年人(3~17岁)油炸焙烤类食品消费量最高,其他人群之间差异无统计学意义;此外,未成年人(3~17岁)对于焙烤食品、油炸膨化小食品的消费量高于其他人群(F=9.46,P < 0.05;F=46.81,P < 0.05)(表 2)。

表2

上海市不同人群对不同种类油炸焙烤类食品的消费量

Table2.

Consumption of fried and baked foods in different groups in Shanghai 单位(Unit): g·d-1

2.3   油炸焙烤类食品中丙烯酰胺暴露量评估

通过模拟计算得到上海市居民因食用油炸焙烤类食品而摄入丙烯酰胺的均数为0.16 μg·kg-1·d-1,第95百分位数为0.41 μg·kg-1·d-1(图 1)。不同人群因食用油炸焙烤类食品而摄入丙烯酰胺的概率分布也有所不同,经模拟计算未成年人(3~17岁)、青年人(18~44岁)、中年人(45~59岁)、老年人(> 60岁)、孕妇摄入丙烯酰胺的均数分别为0.24、0.14、0.08、0.11、0.10 μg·kg-1·d-1 (表 3)。

图 1

上海市居民油炸焙烤类食品中丙烯酰胺暴露量分布

Figure1.

Probability distribution of acrylamide intake from fried and baked foods in Shanghai residents

表3

不同人群油炸焙烤类食品中丙烯酰胺暴露量分布

Table3.

Percentiles of acrylamide intake from fried and baked foods in different groups in Shanghai 单位(Unit): μg·kg-1·d-1

2.4   丙烯酰胺暴露的健康风险评估

2.4.1   非致癌效应的健康风险评估

根据暴露量概率评估结果及非致癌效应参考剂量,上海市全人群中有99.40% 的居民油炸焙烤类食品丙烯酰胺的暴露水平低于0.702 μg·kg-1·d-1,而0.60% 的居民存在引起非致癌性效应的风险(图 2)。

图 2

上海市居民油炸焙烤类食品丙烯酰胺暴露的非致癌性风险概率

Figure2.

Non-carcinogenic health risk of acrylamide intake from fried and baked foods in Shanghai residents

其中,有2.60% 的未成年人(3~17岁)、0.40% 的青年人(18~44岁)以及0.20% 的老年人(60岁以上)经油炸焙烤类食品摄入丙烯酰胺的暴露水平过高,存在引起非致癌性效应的风险;中年人(45~59岁)和孕妇的丙烯酰胺暴露水平尚无造成非致癌性效应的健康风险。

2.4.2   致癌效应的健康风险评估

3~15岁、16岁及以上人群通过油炸焙烤类食品对丙烯酰胺的暴露量分布图 34

图 3

3~15岁人群油炸焙烤类食品中丙烯酰胺暴露量分布

Figure3.

Probability distribution of acrylamide intake from fried and baked foods in 3-15 years age group in Shanghai

图 4

16岁及以上人群油炸焙烤类食品中丙烯酰胺暴露量分布

Figure4.

Probability distribution of acrylamide intake from fried and baked foods in > 16 years age group in Shanghai

按照ILCR计算方法,分别以均数和第95百分位数作为一般摄入水平和高摄入水平。上海市一般摄入水平人群因食用油炸焙烤类食品而摄入丙烯酰胺的终生致癌风险为1.08×10-4,即每10万人中多增加约11个癌症病例的风险;高摄入水平人群终生致癌风险为2.28×10-4,即每10万人中多增加约23个癌症病例的风险(图 5表 4)。

图 5

上海市居民油炸焙烤类食品中丙烯酰胺暴露的终生致癌风险累积分布图

Figure5.

Cumulative distribution of incremental lifetime cancer risk of acrylamide intake from fried and baked foods in Shanghai residents

表4

上海市居民摄食油炸焙烤类食品接触丙烯酰胺终生致癌风险

Table4.

Incremental lifetime cancer risk of acrylamide intake from fried and baked foods in Shanghai residents

3   讨论

联合国粮农组织和WHO下的食品添加剂联合专家委员会(Joint FAO/WHO Expert Committee on Food Additives,JECFA)于2005年收集各国相关数据,得出全球一般摄入水平和高摄入水平人群对丙烯酰胺的暴露水平分别为1.00 μg·kg-1·d-1和4.00 μg·kg-1·d-1[13-14]。欧洲各国2011年的暴露评估得出18岁以上成年人一般摄入水平和高摄入水平人群对丙烯酰胺的暴露水平分别为0.31~1.10 μg·kg-1·d-1和0.58~2.30 μg·kg-1·d-1[15]。中国香港地区2013年的暴露评估得出20岁以上一般摄入水平和高摄入水平人群对丙烯酰胺的暴露水平分别为0.21 μg·kg-1·d-1和0.54 μg·kg-1·d-1[16-17]。中国大陆地区2013年的暴露评估得出15岁以上一般摄入水平和高摄入水平人群对丙烯酰胺的暴露水平分别为0.29 μg·kg-1·d-1和0.49 μg·kg-1·d-1[12]

按照中国膳食丙烯酰胺暴露量中油炸焙烤类食品(谷类、薯类)的贡献率为35.1%[12]推算,上海市居民一般摄入水平和高摄入水平人群对丙烯酰胺的膳食暴露水平分别为0.46 μg·kg-1·d-1和1.17 μg·kg-1·d-1。与国内外相关研究结果相比,对于一般摄入水平人群,上海市居民丙烯酰胺的膳食暴露水平低于JECFA 2005年的评估结果及欧洲地区2011年的评估结果,略高于我国香港地区2013年的评估结果和大陆地区2013年的评估结果。而对于高摄入水平人群,上海市居民丙烯酰胺的膳食暴露水平低于JECFA评估结果,与欧洲地区接近,明显高于我国香港地区和大陆地区,尤其是3~17岁未成年人暴露水平较高。

本次食品中丙烯酰胺暴露评估采用概率评估的方法,虽然评估过程中油炸焙烤类食品贡献率是基于全国数据计算得到,可能与本市膳食结构不同而存在一定的不确定性,但应用@Risk软件反复模拟计算上万次得到人群丙烯酰胺暴露水平的概率分布,很大程度上降低了极值的影响。另外,对于丙烯酰胺暴露的健康风险评估建立在丙烯酰胺的危害强度参数(Rfd、BMDL、CSF等)和人群暴露水平数据之上,计算过程均引用了国际权威机构推荐和被广泛使用的参数和模型,评估结果具有较好的科学性,与国内外相关研究结果具有良好的可比性,也直观反映出本市居民食用油炸焙烤类食品而摄入丙烯酰胺所带来的健康风险。

鉴于上海市居民食用油炸焙烤类食品摄入丙烯酰胺的暴露水平较我国总体水平偏高,存在的健康效应风险也偏高,尤其是未成年人等高摄入水平人群风险较高。建议居民平衡膳食,做到饮食均衡多样化,烹饪时减少高温油炸和烘烤,避免长期摄入高温或连续长时间烹调加工的淀粉类及薯类食品;未成年人应当减少油炸膨化小食品、焙烤食品的食用量;同时,建议进一步完善食品中丙烯酰胺限量标准,加强监测与监督管理,改进油炸焙烤食品加工工艺和操作流程,降低食品中丙烯酰胺含量,有效减少和控制人群膳食丙烯酰胺暴露水平及其引起的健康危害。

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