% 1% SEM-EDX - X Si Ca SEM-EDX SIMS ppm % M M T 100 % 100 % Ba 1 % 91 % 9 % 9 % 1 % 87 % 13 % 13 % 1 % 64 % 36 % 36 % 1 % 34 46
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1 Review on Hair Analysis in the Wakayama Arsenic Case Jun KAWAI Department of Materials Science and Engineering, Kyoto University Sakyo-ku, Kyoto , Japan Received 6 December 2014, Revised 29 December 2014, Accepted 31 December 2014 I review the hair analysis of Wakayama arsenic poisoning case, and discuss problems in this forensic analysis. (i) It has been said that two pieces of hair were analyzed, but I conclude that only one piece was analyzed. (ii) High concentration arsenic was said to be attached on the hair, but I conclude that the arsenic concentration was same level as those of ordinary Japanese. (iii) It was said that the discrimination of exogenous and endogenous arsenic in hair was possible by the line analysis of hair, but I conclude that the testimony has already been known by the witness to be fault before the death sentence. [Key words] Wakayama curry poisoning case, Hair, Arsenic X Kimura p M M T Adv. X-ray. Chem. Anal., Japan 46, pp (2015) 33
2 % 1% SEM-EDX - X Si Ca SEM-EDX SIMS ppm % M M T 100 % 100 % Ba 1 % 91 % 9 % 9 % 1 % 87 % 13 % 13 % 1 % 64 % 36 % 36 % 1 % 34 46
3 SPring-8 X SEM-EDX SIMS SIMS SPring , 9 SPring-8 KEK PF KEK-PF
4 , I 3 mm ICP-MS a 11 1a I 3 mm 11 ppm , I 11 ppm µg/g 1a KEK-PF 98U
5 10 a / = 80 ppb p = 11 ppm p b p.21 p ppm ppm c 1 a I 3 mm ICP- MS 10 b 16 c
6 p p.23 1a I mm 11 ppm 15 cm 1 mg 18 3 mm 18 mg = 0.02 mg 11 ppm 0.02 mg = g I 1 1a g I g 100, g KEK-PF 4A BL-4A 4 mm X p p cm 1 mg 18 3 a, c 10 cm 50 mg 2N- 2 ml cm 15 cm
7 ppb p ppb 69 ppb 3 32 ppb 37 ppb 3 90 ppb ppb I 1/ ppb 159 ppb ppb 1988 Yamato ppb ppb 3 As III ppb , ppb ppb 53.2 ppm ppb 124 ppm ppb ppb ppb ppb 3 As 3 + attached to the hair through exogenous contamination remains so attached to be slowly oxidized into As ppm 5 39 ppm ppb ppb
8 ppm ppm 3 ppm X 22 ppm 23 DMA DMA p ppm 3 1 ppb ppm 3 10 ppb 19, DMA 10 ppb pp DMA
9 1 I ,000 1c p X 63 SPring-8 SPring p
10 U004 KEK-PF BL-4A U 98U U X X b mm mm MA DMA TMA DMA DMA 42 46
11 a 2 KEK-PF BL-4A a b b 1a 1a I 3 mm 3 mm 1 98U KEK-PF Photon Factory News Photon Factory News 46 43
12 Vol.17 No U004 97G172 Web BL-11B 98G120 BL-4A BL-4A Photon Factory News Vol.16, No Vol.17, No Vol.17, No Vol.17, No Vol.18, No Vol.18, No Vol.18, No A B C D E BL-4A 44 46
13 6 Web 25 97G172 X 98U004 98G G391 00G336 A B C D E 5 A KEK-PF BL-4A p.80 SPring-8 KEK-PF KEK-PF X BL-4A X C a 3a 0 10 cm 10 cm 4 mm X 0 mm 96 mm mm 2 3a mm X ULD LLD 1 X 46 45
14 1 1 XY 4 mm 3 mm X 1 X mm a 0 mm 10 cm cm 1 3a 3c Kα X X b c d 3 a 12 4 mm b 13 1 mm c 12 3a d
15 3c X mm mm X X 3a C 3b 3b 1 mm 2 3a 3 2 mm 52 mm 1 3d 3ab 3 3a B M 97G172 98U C U004 97G mm 12.2 kev 12.9 kev X mm p.40 p.41 A 46 47
16 p b 45 mm 59 mm A C 45 mm b mm mm 7 X 12 X 5 X X D U004 98G187 98G391 E G391 98G mm kev X mm 1 A E 3 97G172 X 98U004 C 98G187 2 E 2000G
17 A E A E KEK-PF 4 / A E 1a 3ab 7 X 7 Web i vi i a X 27 Appendix D 30 X SEM SEM SEM 3a ii 12 A B
18 2 120 iii 5 C B mm 1988 Yamato 20 1 C 12 A 4 mm 1 mm mm 5 C B E A D 2 2 iv 5 6 D 96 v 12 A 5 C 10 E 96 5 X C 98U004 98G187 98U G187 5 vi 98U a X b c 5 3 d 4 mm e X f 1 mm 3 2 d e 50 46
19 f % 28 KEK-PF BL 4A kev X X X 7 4 Kα Kα 2.3 kev 0.1% 7, 9 X 4 5 C A 5 30 X 7 4 Kα 100 ppb < I 10 ppm < 0.1% ppm 1,000, ppb 1,000,000,
20 KEK BL-4A I I 100 ppb 10 ppm 0.1 % g Appendix 2 mm 52 46
21 10 12 g g 3 3 µm 1 11 µm PM 2.5 PM10 PM 2.5 I 10 9 g g ppb ppb X X p.29 SPring KEK-PF 1 SPring-8 1 KEK-PF 46 53
22 1 I 1 1 KEK-PF A BL-4A LC-ICP/MS 1 Y. Kimura: Forensic analysis in the Wakayama Arsenic Case, Forensic Sci. Rev., 26 (2), (2014) (10), (2014) No pp.464 (1)-122 (343) (2003). 4 X X 45, (2014). 5 Anthony T. Tu X 45, (2014). 6 6 No (2014) (2), (2014). PDF/trioc_2014_27_113.pdf http//
23 do?resrchnum= a h t t p : / / m h l w - g r a n t s. n i p h. g o. j p / n i p h / s e a r c h / NIDD02.do?resrchNum= A A do?resrchnum= a do?resrchnum= a 16 X 11 pp (2000). do?resrchnum= a P&G Web 73 (2), (1963) 1 mg/15 cm 80 µm 70 µm 19 Y. Yamaura, H. Yamauchi: Arsenic metabolites in hair, bolood and urine in workers exposed to arsenic trioxide, Industrial Health, 18, (1980). 20 N. Yamato: Concentrations and chemical species of arsenic in human urine and hair, Bull. Environ. Contam. Toxicol., 40, (1988). 21 M. Bissen, F. H. Frimmel: Arsenic - a review. Part II: Oxidation of arsenic and its removal in water treatment, Acta Hydrochim. Hydrobiol., 31 (2), (2003). 22 X X X 45, (2014) PAC X 44, (2013). 28 X 36, (1987) KEK-PE A 46 55
24 Elements Fluor. Y kev X K/L excitation prob. Kα emis. prob. Mass abs. coef. Product S As Appendix ppb ab 90 ppb 3 A 2 mm 15 cm 1 15 cm = 1 mg ppb mm A1 3 As g I g 1 I 1 80 ppb 15 cm g 2 mm 80 ppb 2 mm A2 A I g g 10 1/ g A3 I 10 4 g A g mm KEK-PF 1 3a 1/
25 A As 2O g/cm 3 = As 76% As 2O 3 100% As As 2O 3 A4 A4 d 3a mm 3b mm 4 52 mm Fig.3a mm X 80 ppb KEK-PF BL-4A MDL sub-ppm ppb 48 mm 52 mm 2 As 1 2 As
26 As As ppm As 3a b As KEK-PF
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