Determination of monomethyltin migration from toys by gas chromatography-mass spectrometry and confirmation of its false positive

doi:10.3724/SP.J.1123.2018.06004

Abstract

Abstract:

Based on migration procedures using simulated gastric juice specified in the EU toy Safety Standard EN 71-3:2013/A2:2017, a method was developed for the determination of monomethyltin (MMT) migration from toys by gas chromatography-mass spectrometry (GC-MS). Further, a reliable confirmation method for judgement of a false positive for MMT obtained by GC-MS, was established. After optimizing the migration conditions, derivatization steps and chromatographic parameters, the method yielded a linear range from 0.02 to 1.0 mg/L with a correlation coefficient (R²) of 0.9992. The limits of detection and quantification of the method were 0.11 and 0.32 mg/kg, respectively. The recoveries were 86.2%-104.2% under different spiked levels (0.5, 1.0 and 1.5 μg), and the relative standard deviations were 3.1%-8.2% (n=6). MMT migration ranging from 0.44 to 0.67 mg/kg was detected in the surface coating of tin-plating (Sn-Fe alloy) toy materials, which was subsequently confirmed to be false positive. Therefore, a novel confirmative approach using methanol or acetone as the migration solvent was proposed, aiming at verifying the false positive of MMT. The results showed that the previously positive MMT detected by GC-MS could no longer be detected when treated by these migration solvents.Hence, this approach can be used to confirm false positive detected for MMT after GC-MS detection.

Key words: confirmation, false positive, gas chromatography-mass spectrometry (GC-MS), migration, monometyltin (MMT), toys

CLC Number:

O658

LI Hanke, YI Lezhou, TAN Zhixian, DING Zhiyong, HUANG Ningshan, HUANG Lina, MA Tongmei. Determination of monomethyltin migration from toys by gas chromatography-mass spectrometry and confirmation of its false positive[J]. Chinese Journal of Chromatography, 2018, 36(11): 1181-1188.

References

[1] Moser V C, Barone S, Phillips P M, et al. Neurotoxicology, 2006, 27(3):409
[2] Kruger K, Hiong T, Bensch W, et al. Neurotoxicology, 2007, 28(1):114
[3] European Food Safety Authority (EFSA). EFSA J, 2004, 102:1
[4] EN 71-3:2013
[5] EN 71-3:2013/A2:2017
[6] Cui Z Y, Zhang K G, Zhou Q F, et al. Talanta, 2011, 85(2):1028
[7] Liu J M, Jiang G B, Zhou Q F, et al. Anal Sci, 2001, 17(11):1279
[8] Smitiene V, Semasko I, Vickackaite V. J Sep Sci, 2014, 37(15):1989
[9] Chen B W, Wang T, Yin Y G, et al. Anal Methods, 2012, 4(7):2109
[10] Jitaru P, Infante H G, Adams F C. J Anal At Spectrom, 2004, 19(7):867
[11] Zhai G S, Liu J F, Li L, et al. Talanta, 2009, 77(4):1273
[12] Suyani H, Heitkemper D, Creed J, et al. Appl Spectrosc, 1989, 43(6):962
[13] Li H K, Huang L N, Yi L Z, et al. Chinese Journal of Applied Chemistry, 2016, 33(10):1210 李函珂, 黄理纳, 蚁乐洲, 等. 应用化学, 2016, 33(10):1210
[14] Hobsley M, Whitfield P F. J Physio, 1977, 271(2):57
[15] Van Engelen J G M, Park M V D Z, Janssen P J C M, et al. Chemical in Toys, a General Methodology for Assessment of Chemical Safety of Toys with a Focus on Elements.[2018-03-11]. https://www.rivm.nl/dsresource?objectid=0e8298a9-8490-458d-b9c5-c3be5c5e9a2b&type=org&disposi-tion=inline
[16] Charman W N, Porter C J H, Mithani S, et al. J Pharm Sci, 1997, 86(3):269
[17] Oomen A G, van Twillert K, Hofhuis M F A, et al. Development and Suitability of in Vitro Digestion Models in Accessing Bioaccessibility of Lead from Toy Matrices.[2018-03-11]. https://www.rivm.nl/dsresource?objectid=2590c915-8816-4144-8489-8d9e8fccb8b6
[18] Christensen F N, Davis S S, Hardy J G, et al. J Pharm Pharmacol, 1985, 37(2):91
[19] Degen L P, Phillips S F. Gut, 1996, 39(2):299
[20] GB 6675.4-2014
[21] ISO 8124-3:2010
[22] Oomen A G, Rompelberg C J M, Bruil M A, et al. Arch Environ Contam Toxicol, 2003, 44(3):281
[23] Ruby M V, Davis A, Schoof R, et al. Environ Sci Technol, 1996, 30(2):422
[24] Hamel S C, Buckley B, Lioy P J. Environ Sci Technol, 1998, 32(3):358
[25] Chung S W C, Wu A H T. J Chromatogr A, 2017, 1505(1/2):18
[26] De Smaele T, Moens L, Dams R, et al. J Chromatogr A, 1998, 793(1):99
[27] Leermakers M, Nuyttens J, Baeyens W. Anal Bioanal Chem, 2005, 381(6):1272
[28] Le Gac M, Lespes G, Potin-Gautier M. J Chromatogr A, 2003, 999(1/2):123
[29] Vahcic M, Milacic R, Scancar J. Anal Chim Acta, 2011, 694(1/2):21
[30] Pinel-Raffaitin P, Rodriguez-Gonzalez P, Ponthieu M, et al. J Anal At Spectrom, 2007, 22(3):258
[31] Gu G B, Li P. Inorganic Chemistry. 2nd ed. Beijing:Chemical Industry Press, 2007 古国榜, 李朴. 无机化学. 2版. 北京:化学工业出版社, 2007
[32] Bishop D P, Hare D J, De Grazia A, et al. Anal Methods, 2015, 7(12):5012
[33] Marcic C, Lespes G, Potin-Gautier M. Anal Bioanal Chem, 2005, 382(7):1574
[34] ISO/TS 16179:2012
[35] Kannan K, Tanabe S, Tatsukawa R. Bull Environ Contam Toxicol, 1995, 55(4):510
[36] Lee C C, Wang T, Hsieh C Y. Environ Pollut, 2005, 137(2):198
[37] Wahlen R, Wolff-briche C. Anal Bioanal Chem, 2003, 377(1):140
[38] Xiao Q, Hu B, He M. J Chromatogr A, 2008, 1211(1/2):135