Research progress in the application of stable isotope and mineral element analysis in tracing the geographical origin of Chinese medicinal materials

ZHANG, Ticui; LI, Sen; WANG, Yuanhao; HU, Qing; WANG, Chao; YANG, Hua; XU, Naijiao

doi:10.1590/fst.08222

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Food Science and Technology

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Review Article • Food Sci. Technol 42 • 2022 • https://doi.org/10.1590/fst.08222 copy

Research progress in the application of stable isotope and mineral element analysis in tracing the geographical origin of Chinese medicinal materials

Authorship SCIMAGO INSTITUTIONS RANKINGS

Abstract

The Geographical Origin of Chinese medicinal materials plays an important role in guaranteeing the authenticity of Chinese medicinal materials, ensuring the quality and efficacy of Chinese medicinal materials, maintaining the market order, and reducing the risk of medical accidents caused by counterfeit Chinese medicinal materials. In recent years, there have been more and more research papers on tracing Chinese medicinal materials by stable isotope and mineral element analysis combined with chemometrics. Using stable isotope and mineral element analysis to trace traditional Chinese medicinal materials has the advantages of high accuracy and strong reliability. Through chemometrics methods, medicinal materials from different origins can be classified, distinguished, and modeled, and finally the purpose of origin traceability can be achieved. Based on the introduction of the basic principles of stable isotopes and mineral elements, this article systematically analyzes the research and application of relevant stable isotope and mineral element analysis techniques in the origin traceability of Chinese medicinal materials in the past 10 years, and proposes the existing problems in origin traceability of Chinese medicinal materials. This article aims at providing reference for the origin traceability, confirmation and supervision of Chinese herbal medicines, and promoting the establishment and improvement of the traceability technical system of Chinese herbal medicines.

Keywords:
Chinese medicinal materials; geographical origin; stable isotope; mineral element analysis

samples	sources	key variables	statistical method	results	reference
Panax notoginseng	Guangxi, Yunnan,	δ¹³C, δ¹⁵N, δ²H, δ¹⁸O	ANOVA, SDA, Fisher discriminant analysis	overall discrimination rate about 84%;	Liang et al. (2021)Liang, S. W., He, Z. J., Xiong, J. F., & Hong, C. Q. (2021). Study on the root discrimination of spring sanqi root origin based on stable isotopic fingerprint. Chinese Traditional Chinese Medicine, 46(3), 560-566. http://dx.doi.org/10.19540/j.cnki.cjcm20201121.103. PMid:33645020. http://dx.doi.org/10.19540/j.cnki.cjcm20...
Ginseng	China, Korea,	δ¹³, δ¹⁵N, δ²H,	F-test, boxplot	good distinction;	Horacek et al. (2010)Horacek, M., Min, J.-S., Heo, S.-C., & Soja, G. (2010). Discrimination between ginseng from Korea and China by light stable isotope analysis. Analytica Chimica Acta, 682(1-2), 77-81. http://dx.doi.org/10.1016/j.aca.2010.09.046. PMid:21056718. http://dx.doi.org/10.1016/j.aca.2010.09....
Dendrobium officinale	Guangdong, Guangxi, Guizhou, Yunnan, Zhejiang,	δ¹³C, δ¹⁵N, δ²H, δ¹⁸O, ⁸⁷Sr/⁸⁶Sr	PCC, PCA, One-way ANOVA,	PCA can distinguish; Dendrobium officinale from different habitats;	Yang et al. (2018a) Yang, J., Wu, H., Lu, C. G., Wang, S. X., Zhang, B., Yang, G., Guo, L. P., & Huang, L. Q. (2018a). Study on the identification of dendrobium based on stable isotope. Chinese Traditional Chinese Medicine, 43(6), 1118-1123. http://dx.doi.org/10.19540/j.cnki.cjcmm.20180109.006. PMid:29676117. http://dx.doi.org/10.19540/j.cnki.cjcmm....
Panax japonicus	Akita, Hubei, Yunnan, Sichuan, Guizhou,	δ¹³C, δ¹⁵N, δ²H, δ¹⁸O	SVM, LDA, BPN, One-way ANOVA,	accuracy of LD and BPN is 100%;	Zhang et al. (2020)Zhang, W. L., Wu, H., Mei, Y. C., Yang, Z. X., He, S. M., & He, Z. G. (2020). Study on the identification of Panax japonicus joint production site based on stable isotope technology. Chinese Herbal Medicines, 51(23), 6070-6076. http://dx.doi.org/10.7501/j.issn.0253-2670.2020.23.021. http://dx.doi.org/10.7501/j.issn.0253-26...
Amomum villosum	Guangdong, Guangxi, Yunnan,	δ¹³C, δD, δ¹⁵N	OPLS-DA, LDA	the accuracy of discriminant model is 89.7%	Zhong et al. (2021)Zhong, H. Y., Huang, H. B., Chen, Y. E., & Qing, T. H. (2021). Analysis of Yangchun sand origin based on stable isotope performance. Guangzhou University of Traditional Chinese Medicine, 38(10), 2224-2230.
Lycium barbarum L.	Qinghai, Ningxia, Xinjiang,	δ¹³C, δ¹⁵N, δ²H, δ¹⁸O, δ³⁴S	PCA, LDA, SVM, One-way ANOVA	the discrimination effect of SVM model is better than that of LDA model;	Lian et al. (2022)Lian, S. Y., Zhu, S. S., Zhang, Z. J., Xie, Y. J., Fan, C. L., Chen, H., & Wang, M. L. (2022). Characteristic analysis and discrimination of Lycium barbarum from different places based on stable isotope ratio. Shipin Yu Fajiao Gongye, 48(1), 1-8.
Lycium barbarum L.	Gansu, Ningxia, Qinghai,	δ¹³C	ANOVA, LDA	LDA can distinguish Lycium barbarum L. from different provinces;	Meng et al. (2019)Meng, J., Liu, Z., Gou, C. L., Rogers, M. K., Yu, W. J., Zhang, S. S., Yuan, Y. W., & Zhang, L. (2019). Geographical origin of Chinese wolfberry (goji) determined by carbon isotope analysis of specific volatile compounds. Journal of Chromatography. B, Analytical Technologies in the Biomedical and Life Sciences, 1105, 104-112. http://dx.doi.org/10.1016/j.jchromb.2018.12.011. PMid:30580182. http://dx.doi.org/10.1016/j.jchromb.2018...

samples	sources	key variables	statistical method	results	reference
Pueraria thomsonii	Shaanxi, Hubei, Guangxi	Mg, P, Co, Rb, Sr	PCA, SLDA, HCA	the overall accuracy rates of back substitution test and cross test are 97.7% and 93.0%, respectively;	He et al. (2021)He, Y. Y., Sun, Q. Q., Guo, B. L., & Zhang, L. (2021). Research on powder growth of fingerprint based on mineral element. Nuclear Agriculture, 35(7), 1565-1573.
Medulla Tetrapanacis	Guangxi, Sichuan, Guizhou, Yunnan	Sn, Be, Na, As, Mg, Al, K, Ca, Mn, Fe, Co, Cu, Zn, Se, Si, Sb, Ba, Ti, Pb, Zr, Sr	PCA, DA, SLDA, K-NN	the correct resolution of KNN model training set and validation set are 100% and 93.33%;	Li et al. (2014)Li, H., Yao, S., Liu, Y., Bai, F. R., Zha, C. J., & Chen, C. (2014). Application of stable isotope carbon, nitrogen in the identification of Cordyceps sinensis. Shipin Yu Fajiao Gongye, 40(7), 173-176. http://dx.doi.org/10.13995/j.cnki.11-1802/ts.2014.07020. http://dx.doi.org/10.13995/j.cnki.11-180...
Salvia miltiorrhiza	Shandong, Shanxi, Henan, Anhui	Na, K, Ca, V, Fe, Ni, Cu, As, Se, Mo, Cd, Pb, Th, U, Sc, Y, La, Eu	ANOVA, LDA, PCA	the accuracy of LDA regression and the success rate of cross validation are 100% and 85.5%;	Zhao et al. (2017)Zhao, H. Q., Zhang, M. M., Zhao, Z. G., Geng, Y. L., Huang, L. Q., & Wang, X. (2017). Multi-element analysis combined with multivariate statistical analysis for the traceability of Danshen Origin. Research and Development of Natural Products, 29(10), 1752-1758.
Lycium barbarum L.	Ningxia, Gansu, Xinjiang	Mg, Fe, Ca, Zn, Cu, Mn, Al, Sr, Rb, Mo, Tb, Cd, Co, V, As, Cs, Pr, Dy, Gd	ANOVA, PCA, LDA	the accuracy rates of original group and cross validation group are 95.7% and 85.7%;	Zhang et al. (2016)Zhang, S., Wei, Y., Wei, S., Liu, H., & Guo, B. (2016). Authentication of Zhongning wolfberry with geographical indication by mineral profile. International Journal of Food Science & Technology, 52(2), 457-463. http://dx.doi.org/10.1111/ijfs.13301. http://dx.doi.org/10.1111/ijfs.13301...
Lycium barbarum L.	5 regions of Zhongning, Ningxia	Cd, Ce, Co, Cu, Gd, Hg, Mg, Se, Zn, P	ANOVA, PCA, PLS-DA, Fisher	OPLS-DA is better than Fisher;	Kai et al. (2021)Kai, J. R., Shi, X. C., Li, H., Yang, C. X., & Wang, C. X. (2021). Discriminant analysis of Lycium barbarum L. in different production area based on mineral element technology. Food & Fermentation Industry. In press.
Panax notoginseng	5 regions of Yunnan	Cu, Fe, Mn, Na, Cd, Pb, As	FA, PCA, CA, CDA	CA discrimination accuracy is 90%;	Zhang et al. (2021)Zhang, P., Zhang, X., Yang, X. Y., Liu, Y. L., Liu, R., Long, M., Tian, X. J., Zhang, F. M., Chen, S. E., & Ma, Z. R. (2021). Analysis of Sanqi origin and identification of main and lateral roots based on the trace element. Zhejiang Agricultural Journal, 33(7), 1300-1308.

samples	sources	key variables	statistical method	results	reference
Coptis chinensis franch	Sichuan, Shaanxi, Yunnan, Hubei, Chongqing	δ¹⁵N, δ¹³C, Al, Sn, Mg	PCA, LDA, OPLS‐DA	LDA and OPLS-DA classification accuracy are both 100%	Du et al. (2020)Du, H., Tang, B., Cao, S., Xi, C., Li, X., Zhang, L. G., Wang, M. G., Lai, Y., & Chen, Z. (2020). Combination of stable isotopes and multi-elements analysis with chemometric for determining the geographical origins of Rhizoma Coptidis. Microchemical Journal, 152, 104427. http://dx.doi.org/10.1016/j.microc.2019.104427. http://dx.doi.org/10.1016/j.microc.2019....
Angelica sinensis	Gansu, Sichuan, Yunnan	δ¹³C, δ¹⁵N, Mg, Mo,Cr, Mn, Fe, Ni, Zn	One-way ANOVA, FLDA	the accuracy of FLDA is 100%, the accuracy of cross validation is 91%, and the accuracy of external sample prediction is 100%;	Yang et al. (2020)Yang, Y., Liu, F., & Li, X. B. (2020). Analysis of origin traceability of Chinese angelica based on stable isotope ratio and trace elements content difference. Chinese Herbal Medicines, (11), 2650-2656. http://dx.doi.org/10.13863/j.issn1001-4454.2020.11.008. http://dx.doi.org/10.13863/j.issn1001-44...
Polygonum multiflorum thumb	Anhui, Hubei, Sichuan	δ¹³C, δ¹⁵D, δ¹⁸O,Sc, V, Zn, Rb, Cd	One-way ANOVA, PCA, OPLS-DA, FLDA, CHAID	the accuracy of back substitution test, cross validation and external sample test for decision tree CHAID modeling analysis reaches 100%.	Yang et al. (2018b) Yang, J., Wu, H., Yang, G., Wang, S., Zhang, X. B., Guo, L. P., & Huang, L. Q. (2018b). Identification of Polygonum multiflorum origin based on stable isotope ratio and element analysis technology. Chinese Traditional Chinese Medicine, 43(13), 2676-2681. http://dx.doi.org/10.19540/j.cnki.cjcmm.20180307.012. http://dx.doi.org/10.19540/j.cnki.cjcmm....
Atractylodes macrocephala	Anhui, Sichuan, Chongqing, Hunan,	δ¹⁸O, δ³⁴S, Li, Dy, Sm, Er	one-way ANOVA, PCA, LDA	classification accuracy is 100%	Fu et al. (2020)Fu, H. Y., Hai, C. Y., Chen, H. Y., Yang, X. L., & Yang, J. (2020). Application of stable isotope and element fingerprint analysis in provenance traceability of Atractylodes macrocephala. Nuclear Agricultural Journal, 34(S1), 69-78.
Polygonatum sibiricum	Anhui,Shanxi, Hebei,Guizhou, Sichuan,Yunnan	δ¹³C, δ¹⁵N, δ²H, δ¹⁸O, Sr, Be, U	one-way ANOVA,PCA,OPLS‐DA	the accuracy of comprehensive discrimination is 100%;	Fu et al. (2021)Fu, H. Y., Wei, L. N., Chen, H. Y., Yang, X. L., Kang, L. P., Hao, Q., Zhou, X. L., Zhan, Z. L., Liu, Z., Yang, J., & Guo, L. P. (2021). Combining stable C, N, O, H, Sr Isotope and multi-element with chemometrics for identifying the geographical origins and farming patterns of Huangjing Herb. Journal of Food Composition and Analysis, 102, 103972. http://dx.doi.org/10.1016/j.jfca.2021.103972. http://dx.doi.org/10.1016/j.jfca.2021.10...
Lonicera japonica	Henan, Shandong, Hebei, Chongqing	δ¹³C, δ¹⁵N, δ¹⁸O, Cd, Cr, As, Hg, Se, Co, Ni, Sr, Fe	ANOVA, PCA, LDA	LDA cross validation accuracy is 95.7%;	Fan et al. (2018)Fan, L., Chen, L., Ding, R., Wang, L., & Zhang, B. (2018). Geographical discrimination of honeysuckle (Lonicera japonica Thunb.) from China by characterization of the stable isotope ratio and multielemental analysis. Analytical Letters, 51(16), 2509-2516. http://dx.doi.org/10.1080/00032719.2018.1446973. http://dx.doi.org/10.1080/00032719.2018....
Semen Cassiae	Zhejiang,Hebei, Shandong,Shaanxi, Sichuan, Anhui, Hunan, Guangxi, Hainan	δ¹³C, δ¹⁵N, Ca, Mn, Y, Nd, Gd, Pr, La, Al, V, Li, As, Ba	one-way ANOVA, PCA, ANN	the overall accuracy of ANN model for the analysis of origin discrimination is higher than 90%;	Wang et al. (2020)Wang, Y. Y., Kang, L. P., Lv, C. G., Zhou, L., Gao, F., Yang, J., & Guo, L. P. (2020). Origin characteristics and traceability discrimination of Semen Cassiae based on stable isotopes and mineral elements. Nuclear Agricultural Journal, 34(S1), 28-36.

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