Search for Author, Title, Keyword
ORIGINAL ARTICLE
Non-Destructive Quantitative Analysis of Azodicarbonamide Additives in Wheat Flour by High-Throughput Raman Imaging
Xiaobin Wang 1, 2, 3, 4, 5  
,   Chunjiang Zhao 2, 3, 4, 5  
 
More details
Hide details
1
School of Physics and Electronic Information, Nanchang Normal University, Nanchang 330032, China
2
Beijing Research Center of Intelligent Equipment for Agriculture, Beijing 100097, China
3
National Research Center of Intelligent Equipment for Agriculture, Beijing 100097, China
4
Key Laboratory of Agri-informatics, Ministry of Agriculture, Beijing 100097, China
5
Beijing Key Laboratory of Intelligent Equipment Technology for Agriculture, Beijing 100097, China
CORRESPONDING AUTHOR
Xiaobin Wang   

School of Physics and Electronic Information, Nanchang Normal University, 330032, Nanchang, China
Submission date: 2021-04-17
Final revision date: 2021-10-02
Acceptance date: 2021-10-05
Online publication date: 2021-10-26
Publication date: 2021-10-26
 
 
KEYWORDS
TOPICS
ABSTRACT
Azodicarbonamide (ADA) additives are limited or prohibited from being added to wheat flour by various countries because they may produce carcinogenic semicarbazide in humid and hot conditions. This study aimed to realize the non-destructive detection of ADA additives in wheat flour using high-throughput Raman imaging and establish a quantitative analysis model. Raman images of pure wheat flour, pure ADA, and wheat flour-ADA mixed samples were collected respectively, and the average Raman spectra of each sample were calculated. A partial least squares (PLS) model was established by using the linear combination spectra of pure wheat flour and pure ADA and the average Raman spectra of mixed samples. The regression coefficients of the PLS model were used to reconstruct the 3D Raman images of mixed samples into 2D grayscale images. Threshold segmentation was used to classify wheat flour pixels and ADA pixels in grayscale images, and a quantitative analysis model was established based on the number of ADA pixels. The results showed that the minimum detectable content of ADA in wheat flour was 100 mg/kg. There was a good linear relationship between the ADA content in the mixed sample and the number of pixels classified as ADA in the grayscale image in the range of 100 – 10,000 mg/kg, and the correlation coefficient was 0.9858. This study indicated that the combination of PLS regression coefficients with threshold segmentation had provided a non-destructive method for quantitative detection of ADA in Raman images of wheat flour-ADA mixed samples.
FUNDING
This work was supported by the Project supported by the National Natural Science Foundation of China (No. 32160417), the Science and Technology Project of Jiangxi Provincial Department of Education (No. GJJ212605), the Doctoral Research Funds of Nanchang Normal University (No. NSBSJJ2018016), and the Scientific research project of Nanchang Normal University (No. N21KJYB02).
 
REFERENCES (36)
1.
Becalski, A., Lau, B.P.Y., Lewis, D., Seaman, S.W. (2004). Semicarbazide formation in azodicarbonamide-treated flour: A model study. Journal of Agricultural and Food Chemistry, 52(18), 5730-5734. https://doi.org/10.1021/jf0495....
 
2.
Cebi, N., Dogan, C.E., Develioglu, A., Yayla, M.E.A., Sagdic, O. (2017). Detection of L-cysteine in wheat flour by Raman microspectroscopy combined chemometrics of HCA and PCA. Food Chemistry, 228, 116-124. https://doi.org/10.1016/j.food....
 
3.
Chen, W., Shi, W., Li, Z., Ma, H.M., Liu, Y., Zhang, J.H., Liu, Q.J. (2011). Simple and fast fluorescence detection of benzoyl peroxide in wheat flour by N-methoxy rhodamine-6G spirolactam based on consecutive chemical reactions. Analytica Chimica Acta, 708(1-2), 84-88. https://doi.org/10.1016/j.aca.....
 
4.
Che, W.K., Sun, L.J., Zhang, Q., Zhang, D., Ye, D.D., Tan, W.Y., Wang, L.K., Dai, C.J. (2017). Application of visible/near-infrared spectroscopy in the prediction of azodicarbonamide in wheat flour. Journal of Food Science, 82(10), 2516-2525. https://doi.org/10.1111/1750-3....
 
5.
Chen, Z.Q., Chen, L., Lin, L., Wu, Y.N., Fu, F.F. (2018). A colorimetric sensor for the visual detection of azodicarbonamide in flour based on azodicarbonamide-induced anti-aggregation of gold nanoparticles. ACS Sensors, 3(10), 2145-2151. https://doi.org/10.1021/acssen....
 
6.
Czaja, T., Mazurek, S., Szostak, R. (2016). Quantification of gluten in wheat flour by FT-Raman spectroscopy. Food Chemistry, 211, 560-563. https://doi.org/10.1016/j.food....
 
7.
Dhakal, S., Chao, K.L., Qin, J.W., Kim, M., Chan, D.N. (2016). Raman spectral imaging for quantitative contaminant evaluation in skim milk powder. Journal of Food Measurement and Characterization, 10(2), 374-386. https://doi.org/10.1007/s11694....
 
8.
Esquerre, C., Gowen, A.A., Downey, G., O'Donnell, C.P. (2011). Selection of variables based on most stable normalised partial least squares regression coefficients in an ensemble Monte Carlo procedure. Journal of Near Infrared Spectroscopy, 19(6), 443-450. https://doi.org/10.1255/jnirs.....
 
9.
Gao, S., Sun, L.J., Hui, G.Y., Wang, L.K., Dai, C.J., Wang, J.A. (2016). Prediction of azodicarbonamide in flour using near-infrared spectroscopy technique. Food Analytical Methods, 9(9), 2642-2648. https://doi.org/10.1007/s12161....
 
10.
Hu, J., Liu, Y.D., He, Y., Sun, X.D., Li, B. (2020). Optimization of quantitative detection model for benzoic acid in wheat flour based on CARS variable selection and THz spectroscopy. Journal of Food Measurement and Characterization, 14(5), 2549-2558. https://doi.org/10.1007/s11694....
 
11.
Huang, C.W., Dai, L.K., Dong, X.F. (2011). The application of piecewise direct standardization with SNV in calibration transfer of Raman spectra. Spectroscopy and Spectral Analysis, 31(5), 1279-1282. https://doi.org/10.3964/j.issn....
 
12.
Huang, M., Kim, M.S., Delwiche, S.R., Chao, K., Qin, J.W., Mo, C., Esquerre, C., Zhu, Q.B. (2016). Quantitative analysis of melamine in milk powders using near-infrared hyperspectral imaging, and band ratio. Journal of Food Engineering, 181, 10-19. https://doi.org/10.1016/j.jfoo....
 
13.
Lancelot, E., Fontaine, J., Grua-Priol, J., Le-Bail, A. (2021). Effect of long-term storage conditions on wheat flour and bread baking properties. Food Chemistry, 346, art. no. 128902. https://doi.org/10.1016/j.food....
 
14.
Li, G.L., Tang, C.H., Wang, Y., Yang, J., Wu, H.L., Chen, G., Kong, X.J., Kong, W.H., Liu, S.C., You, J.M. (2015). A rapid and sensitive method for semicarbazide screening in foodstuffs by HPLC with fluorescence detection. Food Analytical Methods, 8(7), 1804-1811. https://doi.org/10.1007/s12161....
 
15.
Li, M.H., Guo, X.Y., Wang, H., Wen, Y., Yang, H.F. (2015). Rapid and label-free Raman detection of azodicarbonamide with asthma risk. Sensors and Actuators B-Chemical, 216, 535-541. https://doi.org/10.1016/j.snb.....
 
16.
Li, Y., Peng, Y.K., Chao, K.L., Qin, J.W., Dhakal, S. (2019). Nondestructive rapid detection of benzoyl peroxide in flour based on Raman hyperspectral technique. Proceedings of SPIE, 11016, art. no. 110160G. https://doi.org/10.1117/12.251....
 
17.
Liu, C., Liu, L., Li, L.M., Hao, C.M., Zheng, X.L., Bian, K., Zhang, J., Wang, X.X. (2015). Effects of different milling processes on whole wheat flour quality and performance in steamed bread making. LWT – Food Science and Technology, 62(1), 310-318. https://doi.org/10.1016/j.lwt.....
 
18.
Lohumi, S., Kim, M.S., Qin, J.W., Cho, B.K. (2017). Raman imaging from microscopy to macroscopy: Quality and safety control of biological materials. TrAC – Trends in Analytical Chemistry, 93, 183-198. https://doi.org/10.1016/j.trac....
 
19.
Lv, J.L., Lu, Y.J., Niu, Y.G., Whent, M., Ramadan, M.F., Costa, J., Yu, L.L. (2013). Effect of genotype, environment, and their interaction on phytochemical compositions and antioxidant properties of soft winter wheat flour. Food Chemistry, 138(1), 454-462. https://doi.org/10.1016/j.food....
 
20.
Noonan, G.O., Warner, C.R., Hsu, W., Begley, T.H., Perfetti, G.A., Diachenko, G.W. (2005). The determination of semicarbazide (N-Aminourea) in commercial bread products by liquid chromatography-mass spectrometry. Journal of Agricultural and Food Chemistry, 53(12), 4680-4685. https://doi.org/10.1021/jf0504....
 
21.
Qin J., Chao K., Kim M.S. (2010). Raman chemical imaging system for food safety and quality inspection. Transactions of the ASABE, 53(6), 1873-1882. https://doi.org/ 10.13031/2013.35796.
 
22.
Qin, J.W., Kim, M.S., Chao, K.L., Bellato, L., Schmidt, W.F., Cho, B.K., Huang, M. (2018). Inspection of maleic anhydride in starch powder using line-scan hyperspectral Raman chemical imaging technique. International Journal of Agricultural and Biological Engineering, 11(6), 120-125. https://doi.org/10.25165/j.ija....
 
23.
Qin, J.W., Kim, M.S., Chao, K.L., Gonzalez, M., Cho, B.K. (2017). Quantitative detection of benzoyl peroxide in wheat flour using line-scan macroscale Raman chemical imaging. Applied Spectroscopy, 71(11), 2469-2476. https://doi.org/10.1177/000370....
 
24.
Sun, X.D., Zhu, K., Liu, J.B., Hu, J., Jiang, X.G., Liu, Y.D., Gong, Z.Y. (2019). Terahertz spectroscopy determination of benzoic acid additive in wheat flour by machine learning. Journal of Infrared Millimeter and Terahertz Waves, 40(4), 466-475. https://doi.org/10.1007/s10762....
 
25.
Tian, W.R., Sang, Y.X., Wang, X.H. (2014). Semicarbazide – from state-of-the-art analytical methods and exposure to toxicity: a review. Food Additives and Contaminants Part A-Chemistry Analysis Control Exposure & Risk Assessment, 31(11), 1850-1860. https://doi.org/10.1080/194400....
 
26.
Wang, X.B., Zhao, C.J., Huang, W.Q., Wang, Q.Y., Liu, C., Yang, G.Y. (2017a). Effective detection of benzoyl peroxide in flour based on parameter selection of Raman hyperspectral system. Spectroscopy Letters, 50(7), 364-369. https://doi.org/10.1080/003870....
 
27.
Wang, X.B., Huang, W.Q., Zhao, C.J., Wang, Q.Y., Liu, C., Yang, G.Y. (2017b). Quantitative analysis of BPO additive in flour via Raman hyperspectral imaging technology. European Food Research and Technology, 243(12), 2265-2273. https://doi.org/10.1007/s00217....
 
28.
Wang, X.B., Zhao, C.J., Huang, W.Q., Wang, Q.Y., Liu, C., Yang, G.Y. (2018). Near-infrared hyperspectral imaging for detection and quantification of azodicarbonamide in flour. Journal of the Science of Food and Agriculture, 98(7), 2793-2800. https://doi.org/10.1002/jsfa.8....
 
29.
Wang, Y., Wang, J., Xiang, L., Xi, C., Chen, D., Peng, T., Wang, G., Mu, Z. (2014). Determination of biurea in flour and its products by liquid chromatography-tandem mass spectrometry. Chinese Journal of Chromatography, 32(5), 513-518. https://doi.org/10.3724/SP.J.1....
 
30.
Wei, T.F., Li, G.K., Zhang, Z.M. (2017). Rapid determination of trace semicarbazide in flour products by high-performance liquid chromatography based on a nucleophilic substitution reaction. Journal of Separation Science, 40(9), 1993-2001. https://doi.org/10.1002/jssc.2....
 
31.
Wiercigroch, E., Szafraniec, E., Czamara, K., Pacia, M.Z., Majzner, K., Kochan, K., Kaczor, A., Baranska, M., Malek, K. (2017). Raman and infrared spectroscopy of carbohydrates: A review. Spectrochimica Acta Part A – Molecular and Biomolecular Spectroscopy, 185, 317-335. https://doi.org/10.1016/j.saa.....
 
32.
Xie Y.F., Li P., Zhang J., Wang H.Y., Qian H., Yao W.R. (2013). Comparative studies by IR, Raman, and surface-enhanced Raman spectroscopy of azodicarbonamide, biurea and semicarbazide hydrochloride. Spectrochimica Acta Part A – Molecular and Biomolecular Spectroscopy, 114, 80-84. https://doi.org/10.1016/j.saa.....
 
33.
Yasui, A., Oishi, M., Hayafuji, C., Kobayashi, C., Shindo, T., Ozawa, H., Nakazato, M. (2016). Analysis of azodicarbonamide in wheat flour and prepared flour mixes. Food Hygiene and Safety Science, 57(5), 133-138. https://doi.org/10.3358/shokue....
 
34.
Ye, J., Wang, X.H., Sang, Y.X., Liu, Q. (2011). Assessment of the determination of azodicarbonamide and its decomposition product semicarbazide: investigation of variation in flour and flour products. Journal of Agricultural and Food Chemistry, 59(17), 9313-9318. https://doi.org/10.1021/jf2018....
 
35.
Zhai, C., Peng, Y.K., Li, Y.Y., Zhao, J. (2017). Detection of chemical additives in food using Raman chemical imaging system. Chemical Journal of Chinese Universities, 38(3), 369-375. https://doi.org/10.7503/cjcu20....
 
36.
Zhang, Z.M., Chen, S., Liang, Y.Z. (2010). Baseline correction using adaptive iteratively reweighted penalized least squares. Analyst, 135(5), 1138-1146. https://doi.org/10.1039/b92204....
 
eISSN:2083-6007
ISSN:1230-0322