SUPPLEMENTARY INFORMATION FOR THE ARTICLE: Distribution Profiles of Melamine and its Derivatives in Indoor Dust from Twelve Countries and the Implications for Human Exposure Hongkai Zhu, Kurunthachalam Kannan *,, Wadsworth Center, New York State Department of Health, and Department of Environmental Health Sciences, School of Public Health, State University of New York at Albany, Empire State Plaza, P.O. Box 509, Albany, New York 12201-0509, United States Biochemistry Department, Faculty of Science and Experimental Biochemistry Unit, King Fahd Medical Research Center, King Abdulaziz University, Jeddah 21589, Saudi Arabia *Corresponding author at: Wadsworth Center, Empire State Plaza, P.O. Box 509, Albany, NY 12201-0509, USA Fax: +1 518 473 2895 E-mail: Kurunthachalam.Kannan@health.ny.gov (K. Kannan) Submitted to: Environmental Science & Technology Tables: Figures: S1-S7 S1 References: 2 S1
List of Supporting Information: Table Table S1. Details of indoor dust samples collected from various countries Table S2. MRM conditions for tandem mass spectrometry Table S3. Concentrations of melamine and its derivates in house dust (ng/g) collected from 12 countries Table S4. Correlation analyses of melamine and its derivatives in indoor dust from 12 countries Table S5. The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by the WHO Table S6. The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by the U.S. FDA Table S7. The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by Hsieh et al. Figure Figure S1. Chromatograms of the quantitation MRM transitions for standard (A) and a real dust sample from Kuwait (B) Reference S2
Table S1. Details of indoor dust samples collected from various countries Countries Cities Locations Period China (n = 50) Shanghai (n=4; urban area); Beijing (n=17; urban area); Qiqihaer (n=5; urban area); Nanchang (n=8; urban area); Xinjiang (n=5; urban area); Shandong (n=6; rural area); Guangzhou (n=5; urban area) Homes 2010 2011 Colombia (n = 45) Cartagena (urban area) Homes 2014 Greece (n = 30) Athens, Erateini, Komotini Homes 2014 India (n = 36) Patna (urban area) Homes 2014 Japan (n = 14) Kumamoto, Nagasaki, Fukuoka, Saitama, Saga Homes 2012 Kuwait (n = 24) Kuwait (urban area) Homes 2013 Pakistan (n = 25) Faisalabad (Urban area: n=12; rural area: n=13) Homes 2011 2012 Romania (n = 23) Iasi (urban area) Homes 2012 Saudi Arabia (n = 31) Jeddah (urban area) Homes 2013 South Korea (n = 30) Ansan, Anyang (urban area) Homes 2012 USA (n = 15) Albany (Urban area) Homes 2014 Vietnam (n = 18) Hanoi, Hatinh, Hungyen, Thaibinh Homes 2014 Table S2. MRM conditions for tandem mass spectrometry Compounds Abbreviation Ionization mode Transition (m/z) CE DP CXP EP Melamine 13 C 3, 15 N 3 melamine Ammeline 13 C 3 ammeline Cyanuric acid 13 C 3, 15 N 3 cyanuric acid Ammelide 13 C 3 -AMD MEL 13 C 3, 15 N 3 -MEL AMN 13 C 3 -AMN CYA 13 C 3, 15 N 3 -CYA AMD 13 C 3 -AMD Note: *Quantitation transition ES+ ES- 127 85* 30 30 8 12 127 68 40 25 10 10 133 89* 25 40 8 12 133 72 40 40 10 12 128 86* 20 20 10 15 128 69 40 20 10 10 131 88* 40 20 10 10 131 71 20 20 10 10 128 42* -30-30 -12-12 128 85-20 -15-8 -10 134 44* -35-20 -12-10 134 89-20 -15-12 -12 127 84* -20-25 -8-12 127 42-35 -25-8 -10 130 86* -20-30 -8-8 130 43-30 -25-12 -15 S3
Table S3. Concentrations of melamine and its derivates in house dust (ng/g) collected from 12 countries MEL AMN AMD CYA Total MEL AMN AMD CYA Total 25th 1700 72 46 1200 4800 25th 710 19 23 440 1300 China (n=50) 50th 3,300 220 98 2,500 8000 Kuwait 50th 1400 31 28 800 2300 75th 5900 330 210 4100 11000 (n=24) 75th 2000 45 43 1300 4100 95th 14000 1200 508 16000 22000 95th 5000 74 57 5400 11000 25th 210 16 31 240 520 25th 170 6.0 15 220 460 Colombia (n=45) 50th 730 25 53 460 1300 Pakistan 50th 300 10 31 300 820 75th 1600 57 100 860 3100 (n=25) 75th 730 25 39 430 1800 95th 7300 340 590 11000 20000 95th 1800 30 64 2300 3300 25th 1200 31 39 950 2200 25th 560 21 25 1000 2400 Greece (n=30) 50th 1,500 52 61 1,300 3400 Romania 50th 1800 39 42 1700 4300 75th 2500 70 82 1900 4700 (n=23) 75th 3500 50 64 2300 8000 95th 6000 100 160 3400 11000 95th 10000 85 99 6400 13000 25th 140 4.5 5.4 94 310 25th 56 35 46 1500 2800 India (n=36) 50th 75th 260 410 6.2 8.7 10 17 158 230 430 690 Saud Arabia (n=31) 50th 75th 2200 4000 56 110 45 110 1700 2700 4400 7800 95th 5600 140 85 1100 7200 95th 12000 460 160 7300 17000 25th 2900 47 51 980 5300 25th 7400 160 190 2100 12000 Japan (n=14) 50th 4,600 110 120 1800 8400 USA 50th 12000 210 270 2900 17000 75th 10000 200 200 3700 15000 (n=15) 75th 17000 330 360 4700 22000 95th 15000 560 310 6200 19000 95th 54000 670 1100 7700 62000 25th 2900 62 51 1400 5300 25th 480 4.9 24 310 1000 South Korea (n=30) 50th 4,500 87 80 2200 7300 Vietnam 50th 1300 11 47 650 2300 75th 7100 110 130 2800 10000 (n=18) 75th 2400 22 110 1300 3500 95th 10000 150 180 4000 14000 95th 5400 120 400 4100 9400 MEL: melamine; AMN: ammeline, AMD: ammelide; CYA: cyanuric acid S4
Table S4 Correlation analyses of melamine and its derivatives in indoor dust from 12 countries AMN AMD CYA MEL 0.427** 0.303** 0.188* AMN 0.281** 0.200** AMD 0.677** MEL: melamine; AMN: ammeline, AMD: ammelide; CYA: cyanuric acid Table S5 The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by the WHO Hazard Quotients WHO Infant Toddlers Children Teenagers Adults USA 0.000172 0.000400 0.000094 0.000047 0.000038 Greece 0.000092 0.000121 0.000040 0.000022 0.000018 Colombia 0.000090 0.000119 0.000039 0.000021 0.000018 Romania 0.000066 0.000087 0.000028 0.000016 0.000013 Japan 0.000044 0.000058 0.000019 0.000010 0.000009 South Korea 0.000026 0.000060 0.000014 0.000007 0.000006 India 0.000021 0.000050 0.000012 0.000006 0.000005 Vietnam 0.000028 0.000037 0.000012 0.000007 0.000006 Saudi Arabia 0.000026 0.000034 0.000011 0.000006 0.000005 Kuwait 0.000010 0.000024 0.000006 0.000003 0.000002 China 0.000005 0.000007 0.000002 0.000001 0.000001 Pakistan 0.000006 0.000008 0.000003 0.000001 0.000001 S5
Table S6 The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by the U.S. FDA Hazard Quotients U.S. FDA Infant Toddlers Children Teenagers Adults USA 0.000544 0.001270 0.000298 0.000149 0.000119 Greece 0.000292 0.000384 0.000126 0.000069 0.000058 Colombia 0.000286 0.000376 0.000123 0.000067 0.000057 Romania 0.000210 0.000276 0.000090 0.000049 0.000042 Japan 0.000140 0.000184 0.000060 0.000033 0.000028 South Korea 0.000082 0.000190 0.000045 0.000022 0.000018 India 0.000068 0.000159 0.000037 0.000019 0.000015 Vietnam 0.000089 0.000117 0.000038 0.000021 0.000018 Saudi Arabia 0.000083 0.000109 0.000036 0.000020 0.000016 Kuwait 0.000033 0.000076 0.000018 0.000009 0.000007 China 0.000017 0.000022 0.000007 0.000004 0.000003 Pakistan 0.000019 0.000025 0.000008 0.000004 0.000004 S6
Table S7 The calculated hazard quotients for melamine based on the tolerable daily intakes (TDIs) set by Hsieh et al. and Wang et al. Hsieh, D. P. H.; Chiang, C. F.; Chiang, P. H.; Wen, C. P., Toxicological analysis points to a lower tolerable daily intake of melamine in food. Regul Toxicol Pharm 2009, 55, 13-16. Wang, I. J.; Chen, C. C.; Chan, C. C.; Chen, P. C.; Leonardi, G.; Wu, K. Y. A hierarchical Bayesian approach for risk assessment of melamine in infant formula based on cases of related nephrolithiasis in children. Food Addit. Contam., Part A 2011, 28, 384 395. Hazard Quotients Hsieh et al. (2009) 1 and Wang et al. (2011) 2 Infant Toddlers Children Teenagers Adults USA 0.004288 0.010000 0.002350 0.001173 0.000938 Greece 0.002300 0.003025 0.000991 0.000543 0.000456 Colombia 0.002250 0.002963 0.000970 0.000531 0.000446 Romania 0.001650 0.002175 0.000711 0.000389 0.000328 Japan 0.001100 0.001450 0.000474 0.000260 0.000219 South Korea 0.000643 0.001500 0.000351 0.000176 0.000141 India 0.000536 0.001250 0.000293 0.000146 0.000117 Vietnam 0.000700 0.000921 0.000301 0.000165 0.000139 Saudi Arabia 0.000650 0.000855 0.000280 0.000154 0.000129 Kuwait 0.000258 0.000600 0.000141 0.000070 0.000056 China 0.000130 0.000171 0.000056 0.000031 0.000026 Pakistan 0.000150 0.000198 0.000065 0.000035 0.000030 S7
Figure S1. Chromatograms of the quantitation MRM transitions for standard (A) and a real dust sample from Kuwait (B) S8
Reference (1) Hsieh, D. P. H.; Chiang, C. F.; Chiang, P. H.; Wen, C. P., Toxicological analysis points to a lower tolerable daily intake of melamine in food. Regul Toxicol Pharm 2009, 55, 13-16. (2) Wang, I. J.; Chen, C. C.; Chan, C. C.; Chen, P. C.; Leonardi, G.; Wu, K. Y. A hierarchical Bayesian approach for risk assessment of melamine in infant formula based on cases of related nephrolithiasis in children. Food Addit. Contam., Part A 2011, 28, 384 395. S9