Scientia Agricultura Sinica ›› 2024, Vol. 57 ›› Issue (12): 2454-2466.doi: 10.3864/j.issn.0578-1752.2024.12.014

• FOOD SCIENCE AND ENGINEERING • Previous Articles     Next Articles

Study on Characterization and Interaction Analysis of Co-Contamination of Multi-Mycotoxins in the Flours of Rice, Maize, Soybean and Wheat Flour in Shanghai from 2021 to 2022

ZHU ZuoYin1,2(), ZHAO HanKe1, CHENG HaiSheng1,2, HAN MengYi1, QIU Zhi1, WANG Jie1,2, ZHOU XinLi2(), YANG JunHua1()   

  1. 1 Institut e for Agro-Food Standards and Testing Technology, Shanghai Academy of Agricultural Sciences, Shanghai 201403
    2 School of Health Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093
  • Received:2023-11-10 Accepted:2024-04-08 Online:2024-06-16 Published:2024-06-25
  • Contact: ZHOU XinLi, YANG JunHua

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Abstract:

【Objective】 The co-contamination of multiple mycotoxins in grain food ingredients has become one of most concerned problem of food safety. In this study, the characteristics and interactions of co-contamination of 14 mycotoxins in the flours of rice, maize, soybean and wheat in Shanghai were explored, in order to provide the basic reference for safety assessment, early warning and supervision of mycotoxins, and development of efficient monitoring measures. 【Method】The content of 14 mycotoxins in 621 substrates of rice, maize, soybean and wheat flour from Shanghai were determined by ultra performance liquid chromatography tandem-triple quadrupole mass spectrometry (UPLC-MS/MS). The co-contaminated characteristics and interaction probabilities of multi-mycotoxin was analyzed by the common contamination index (CCEI), correlation cluster analysis (CCA), one-way ANOVA (one-way ANOVA), and the JAVA procedure. 【Result】The main exposure of mycotoxins in the grain ingredients in Shanghai regions included ochratoxin (OTA), deoxynivalenol (DON), aflatoxins (AFs) and fumonisins (FUMs). Among them, rice was mainly contaminated by OTA and DON, maize was mainly contaminated by FUMs and DON, soybean was mainly contaminated by DON and AFs, and wheat flour was mainly contaminated with DON and its derivatives. Based on the safety limit standards of mycotoxins, the total excess rate was lower than 2.09% in four kinds of grain food ingredients, but the co-contamination rate of two or more kinds of mycotoxins were upper than 87.76%. Moreover, there was much higher interaction rates (25.44%) among different mycotoxins, such as FB1+FB2, DON+FB1, OTA+FB1, OTA+DON, AFM2+OTA, and DON+FB1+FB2. Among the higher interaction rates groups, the most of the mycotoxins cooccurrence showed weaker correlations, but the co-combinations of FB1+FB3, AFB1+DON, DON+15-ADON were all showed the significant moderate correlation. 【Conclusion】 The overall contaminated level and excessive rates of mycotoxins in the flours of rice, maize, soybean, and wheat flour from Shanghai was relatively low. However, the proportion of single samples contaminated by multi-mycotoxins was higher, and along with the difference of sample types. As a complex problem of the mycotoxin contamination in the flours of rice, maize, soybean and wheat, this study provided an important reference for the prevention and control of the co-occurrence of multi-mycotoxins in commercially available grain food ingredients in the future.

Key words: mycotoxin, rice, maize, soybean, wheat flour, co-combination, interaction analysis, Shanghai region

Table 1

Sampling distribution of grain food ingredients in 16 districts of Shanghai"

行政区名称 Name of district 大米 Rice (No.) 玉米Maize (No.) 黄豆Soybean (No.) 面粉Wheat flour (No.)
浦东Pudong 20 16 15 19
闵行Minhang 13 12 11 10
松江Songjiang 12 15 12 8
青浦Qingpu 10 9 11 6
普陀Putuo 4 6 3 4
杨浦Yangpu 5 5 5 5
嘉定Jiading 12 11 11 13
奉贤Fengxian 9 11 5 11
徐汇Xuhui 4 4 4 3
静安Jing’an 6 3 2 4
宝山Baoshan 8 11 11 10
金山Jinshan 9 11 11 11
虹口Hongkou 4 3 3 3
长宁Changning 4 2 3 4
黄浦Huangpu 4 4 3 4
崇明Chongming 13 11 8 14
线上Online 32 0 28 40
总计Total 169 134 146 169

Table 2

Mass spectral parameters of 14 mycotoxins in multiple reaction monitoring mode"

真菌毒素
Mycotoxin		 保留时间
Retention period (min)		 母离子
Parent ion (m/z)		 子离子
Daughter ion (m/z)		 碰撞电压
Impulse voltage (eV)		 离子源
Ion source
AFB1 3.32 313.24 241.16*/284.97 36/22 ES+
AFB2 3.17 315.22 287.14*/259.12 28/26 ES+
AFG1 3.18 329.22 243.08*/199.86 42/26 ES+
AFG2 3.03 331.22 189.05*/245.09 40/30 ES+
AFM1 2.83 329.22 273.12*/229.17 38/22 ES+
AFM2 3.04 331.23 284.99*/241.10 42/24 ES+
DON 1.99 297.1 249.10*/231.10 13/10 ES+
3-ADON 2.71 339.23 231.16*/213.15 16/12 ES+
15-ADON 2.66 356.03 339.02*/320.94 12/6 ES+
FB1 2.97 722.39 334.38*/352.38 38/34 ES+
FB2 3.41 706.39 336.39*/354.39 36/32 ES+
FB3 3.23 706.39 336.39*/354.39 36/32 ES+
ZEN 4.19 317.24 175.05*/131.03 26/24 ES-
OTA 2.90 404.29 239.03*/221.03 34/22 ES+

Table 3

The detection rates of mycotoxins in different samples of grain food ingredients (Detection rate=number of positives/total number of respective samples)"

真菌毒素
Mycotoxin		 总样品
All sample (%)		 大米
Rice (%)		 玉米
Maize (%)		 黄豆
Soybean (%)		 面粉
Wheat flour (%)
ZEN 18.20 13.61 35.82 12.08 14.20
AFB1 15.94 15.38 17.91 24.83 7.10
AFB2 21.10 13.61 44.78 8.72 20.71
AFG1 20.93 24.26 19.40 26.85 13.61
AFG2 9.82 16.57 14.93 5.37 2.96
AFM1 25.12 28.40 44.03 18.79 12.43
AFM2 35.27 44.38 44.03 30.87 23.08
OTA 47.18 59.17 45.52 51.68 32.54
DON 61.35 36.69 67.91 65.77 76.92
3-ADON 26.73 31.95 26.12 34.23 15.38
15-ADON 15.14 11.24 0.00 22.82 24.26
FB1 29.15 5.92 99.25 16.11 8.28
FB2 23.03 11.83 69.40 13.42 5.92
FB3 30.43 32.54 62.69 12.75 18.34

Table 4

Exceedance rates of mycotoxins in different samples of grain food ingredients"

真菌毒素 Mycotoxin 大米 Rice (%) 玉米 Maize (%) 黄豆 Soybean (%) 面粉 Wheat flour (%)
AFB1 - - - -
AFB1+AFB2+AFG1+AFG2 - - - 0.59 (n=1)
FB1+FB2+FB3 - - - -
OTA 4.14 (n=7) 2.24 (n=3) 0.67 (n=1) 1.18 (n=2)
ZEN - - 2.01 (n=3) -
DON - 1.49 (n=2) - -

Table 5

Levels of mycotoxin contamination in different grain food ingredients"

真菌毒素
Mycotoxin		 大米 Rice 玉米 Maize 黄豆 Soybean 面粉Wheat flour
平均值
Average
(μg∙kg-1)		 污染范围
Rage
(μg∙kg-1)		 平均值
Average
(μg∙kg-1)		 污染范围
Rage
(μg∙kg-1)		 平均值
Average
(μg∙kg-1)		 污染范围
Rage
(μg∙kg-1)		 平均值
Average
(μg∙kg-1)		 污染范围
Rage
(μg∙kg-1)
ZEN 0.48b 0.36-9.76 0.45b 0.34-8.67 5.71a 0.59-97.57 0.29b 0.36-13.52
AFB1 0.11b 0.12-1.84 0.17ab 0.11-2.56 0.23a 0.02-2.81 0.06b 0.22-2.36
AFB2 0.08b 0.12-0.80 0.37a 0.10-2.64 0.06b 0.12-0.97 0.17b 0.11-7.87
AFG1 0.11 0.13-0.64 0.13 0.10-1.57 0.12 0.14-2.15 0.10 0.14-2.36
AFG2 0.08a 0.15-0.79 0.09a 0.15-0.66 0.02b 0.11-0.41 0.02b 0.15-0.36
AFM1 0.13b 0.12-2.24 0.42a 0.12-5.32 0.07b 0.12-0.75 0.04b 0.14-0.36
AFM2 0.14b 0.11-0.78 0.35a 0.10-5.48 0.10b 0.14-0.88 0.11b 0.12-2.37
OTA 1.32a 0.21-41.52 0.71ab 0.15-12.20 0.44b 0.12-9.05 0.27b 0.12-6.86
DON 7.31b 5.00-61.99 110.59a 5.37-2091.52 26.95b 2.56-407.60 53.83a 10.79-698.84
3-ADON 2.01 0.32-56.26 3.91 0.34-93.56 1.54 0.30-26.36 33.61 2.36-1890.20
15-ADON 17.85b 0.60-261.13 0.00 0.00-0.00 78.22a 2.35-890.99 66.74a 25.75-534.56
FB1 0.35b 0.59-16.49 102.59a 1.19-749.38 4.68b 0.56-281.34 1.12b 0.45-78.72
FB2 0.19b 0.56-5.26 18.82a 1.06-167.16 1.81b 0.64-123.74 0.54b 0.64-21.60
FB3 0.24b 0.54-2.56 31.36a 1.02-217.57 3.07b 0.58-168.33 0.61b 0.52-20.15

Fig. 1

Combinated contamination of mycotoxins in different grain food ingredients A: All samples; B: Rice; C: Maize; D: Soybean; E: Wheat flour"

Fig. 2

Heat map for cluster analysis of correlation of 14 mycotoxins in different grain food ingredients A: Rice; B: Maize; C: Soybean; D: Wheat flour. **: Significant correlation (P<0.01)"

Fig. 3

Co-occurrence of mycotoxins and interaction rates in different grain food ingredients A: 2 kinds of mycotoxin combinations; B: 3 kinds of mycotoxin combinations; C: 4 kinds of mycotoxin combinations; D: 5-7 kinds of mycotoxin combinations"

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