中国居民小麦粉和玉米制品中脱氧雪腐镰刀菌烯醇和玉米赤霉烯酮暴露水平评估

Probabilistic assessment of dietary exposure to both deoxynivalenol and zearalenone from cerealbased products in Chinese populations

目的分析中国小麦粉和玉米制品中脱氧雪腐镰刀菌烯醇（DON）和玉米赤霉烯酮（ZEN）的污染水平，以及人群DON和ZEN的暴露情况。方法于2009年，按照分层整群随机抽样原则，选取中国13个省份44个市（区、县）的107个超市或市场为采样点，分别采集小麦粉和玉米制品样品292、347份。采用超高效液相色谱-串联质谱法方法检测样品中DON和ZEN污染水平。结合2002年“中国居民营养与健康状况调查”的3～13、≥14岁的68959名调查对象的数据，采用有放回地随机抽样方法以及蒙特卡罗（Monte Carlo）法得到调查对象每日DON和ZEN暴露量的P1～P99及其分布，将DON和ZEN暴露量的P1～P99分别与暂定最大每日耐受摄入量（PMTDI）和每日耐受摄入量（TDI）进行比较，分析超过健康指导值的最小暴露量百分位数及其分布，采用t检验比较不同年龄组调查对象DON和ZEN暴露量差异。结果小麦粉和玉米制品中DON污染阳性率分别为100．O％（292／292）、97．4％（338／347），高于限量标准（1μg·kg^-1·d^-1）的样品分别占1．7％（5／292）、4．6％（16／347）；小麦粉和玉米制品中ZEN污染阳性率分别为53．4％（156／292）、87．6％（304／347），玉米制品中ZEN高于限量标准（0．25μg·kg^-1·d^-1）的样品占15．6％（54／347），小麦粉样品中ZEN均未超过限量标准（0．25μg·kg^-1·d^-1）。3～13岁组DON的P50、P75、P90、P95、P975和P。的面（95％CI）分另0为0．170（0．170～0．171）、0．762（0．759～0．765）、2．066（2．038～2．069）、3．515（3．501～3．530）、5．342（5．314～5．372）和9．220（9．155～9．279）μg·kg^-1·d^-1，均高于≥14岁组的贾（95％CI）[0．131（0．130～0．131）、0．500（0．498～0．501）、1．280（1．276～1．285）、2．138（2．128～2．147）、3．510（3．494～3．527）和5．512（5．474～5．546）μg·kg^-1·d^-1]（t值分男0为87．19、163．87、164．66、157．78、105．47和96．31，P值均〈0．001），3—13岁组ZEN的P50、P75、P90、P95、P97．5和R9暴露量分别为0．001（0．001～0．001）、0．006（0．006～0．006）、0．039（0．038～0．039）、0．101（0．100～0．101）、0．195（0．194～0．197）和0．378（0．374～0．381）μg·kg^-1·d^-1，均高于≥14岁组的元（95％CI）[0．001（0．001～0．001）、0．004（0．004～0．004）、0．026（0．026～0．026）、0．061（0．060～0．061）、0．115（0．115～0．116）和0．232（0．231～0．235）μg·kg^-1·d^-1]（t值分男0为151．11、73．80、96．81、100．81、91．93和76．13，P值均〈0．001）。3—13岁组超过PMTDI的DON最小暴露水平为P76，其P99为1．03μg·kg^-1·d^-1，≥14岁组超过PMTDI的DON最小暴露水平为P84，P95为1．01μg·kg^-1·d^-1。3～13岁组超过TDI的ZEN最小暴露水平为％，其如为Q25μg·kg^-1·d^-1，≥14岁组超过TDI的ZEN最小暴露水平为P98，其P90为0．26μg·kg^-1·d^-1。结论中国小麦粉和玉米制品中DON和ZEN的污染水平较低；人群膳食DON和ZEN暴露风险较低；3～13岁组对DON和ZEN的膳食暴露量均高于≥14岁组，是膳食暴露DON和ZEN的高危人群。

Objective To elucidate the dietary exposure to deoxynivalenol （DON） and zearalenone （ZEN） from cereal-based products in Chinese populations using the probabilistic assessment approach. Methods A total of 292 wheat flours and 347 corn-based products were collected from sampling sites of 107 supermarkets or farmers markets, which were randomly selected from 44 cities of 13 provinces in 2009 by the stratified cluster random sampling method. Then, DON and ZEN contamination levels in these samples above analyzed by UPLC-MS/MS in combination with the food consumption data of 68 959 respondents, who were divided into group 1 aged 3 to 13 years old, and group 2 aged 14 and over 14 years old （ ≥14 years old）, obtained by China National Nutrition and Health Survey in 2002 were investigated. A probabilistie assessment model using Monte Carlo simulation was applied to derive the intake distribution of P1-P99 percentile of dietary exposure to DON and ZEN. Meanwhile, all parameters related to dietary exposure to both toxins were compared with either the provisional maximum tolerable daily intake （PMTDI） of 1 μg·kg^-1·d^-1 for DON, or the tolerable.daily intake （TDI） of 0.25 μg·kg^-1·d^-1 for ZEN in order to evaluate the risk of dietary intake of two toxins and find the minimum percentile of dietary exposure to these two toxins. The statistical differences of dietary exposure to these two toxins between two groups were achieved by t test. Results The detection frequencies of DON in wheat flours and corn-based products were 100% （292/292） and 97.4% （338/347） , respectively. A total of 21 out of 639 samples （wheat flours： 5/292, corn-based products： 16/347） were positive for DON at the levels exceeding the Chinese regulatory limit of 1 000 μg/kg for DON. And the detection frequencies of ZEN in wheat flours and corn-based products were 53.4% （156/292） and 87.6% （304/347）, respectively. 54 out of 347 corn-based products and no wheat flours were positive for ZEN at the levels exceeding the Chinese regulatory limit of 60 txg/kg for ZEN. Meanwhile, the mean values （95% CI） of the P50 ,P75 ,P90 ,P95 ,P97.5 and P99 percentile of dietary exposure to DON in populations of 3 to 13 years old were 0. 170 （0. 170 - 0. 171 ）, 0. 762 （0. 759 - 0. 765 ） , 2.066（2.038-2.069）, 3.515 （3.501 -3.530）, 5.342 （5.314-5.372）, and 9.220 （9. 155-9.279） μg·kg^-1·d^-1 , which were higher than those in populations of ≥14 years old （0. 131 （0. 130 -0. 131）, 0.500 （0.498 -0.501）, 1.280 （1.276 -1.285） , 2. 138 （2. 128 -2.14）, 3.510 （3.494 -3.527）, and 5.512 （5. 474 - 5. 546）μg·kg^-1·d^-1 ）, with t values of 87.19, 163.87, 164.66, 157.78, 105.47 and 96.31, and all P values less than 0. 001. And the mean values （95% C1） of the P50 ,P75 ,P90 ,P95 , P97.5 and P99 percentile of dietary exposure to ZEN in populations of 3 to 13 years old were 0. 001 （0. 001 - 0.001）, 0.006 （0.006 -0.006）, 0.039 （0.038 -0.039）, 0. 101 （0. 100 -0. 101）, 0. 195 （0. 194 - 0. 197） and 0.378 （0. 374 -0. 381 ）μg·kg^-1·d^-1 , which were also higher than those in populations of ≥14 years old （0. 001 （0. 001 - 0. 001 ）, 0. 004 （0. 004 - 0. 004）, 0. 026 （0. 026 - 0. 026）, 0. 061 （0.060-0.061）,0.115 （0.115-0.116） and0.232 （0.231-0.235） μg·kg^-1·d^-1） with T-values of 151.11, 73.80, 96.81, 100.81, 91.93 and 76.13, and all P values less than 0. 001. Besides, the minimum percentile of dietary exposure to DON in populations of 3 to 13 years old and ≥ 14 years old exceeded the corresponding PMTDI of 1μg·kg^-1·d^-1 was found in the probability distribution of P76 （99% percentile = 1.03 μg·kg^-1·d^-1 ） and P81 （95% percentile = 1.01 μg·kg^-1·d^-1 ） percentile, respectively. And the minimum percentile of dietary exposure to ZEN in populations of 3 to 13 years old and ≥14 years old exceeded the corresponding TDI of 0.25 μg·kg^-1·d^-1 was found in the probability distribution of P97 （95% percentile =0.25 μg·kg^-1·d^-1） and P1 （90% percentile =0.26 μg·kg^-1·d^-1） percentile, respectively. Conclusion The contamination levels of DON and ZEN in wheat flours and corn-based products and the risk of dietary exposure to both DON and ZEN in populations in Chinese populations were at relatively low levels. The dietary exposure to both DON and ZEN in populations of 3 to 13 years old was higher than those in populations of ≥ 14 years old . Populations of 3 to 13 years old were the populations at the high risk of dietary exposure to both mycotoxins.