食品中に残留するクロラムフェニコールを含めた動物用医薬品の一斉

ᲯᲨ᫢ԼɶƴസသƢǔǯȭȩȠȕǧȋdzȸȫǛԃNJƨ
ѣཋဇҔᕤԼƷɟ૪ЎௌඥƷ᧏ႆ
‫ۑ‬ᮏ㒓 ⊛ࠊᶫᮏ ༤அࠊబ⸨ ┾୍㸦༓ⴥ┴⾨⏕◊✲ᡤ㸧
ụ⏣ ᝴㸦ᪧᡤᒓ㸸༓ⴥ┴⾨⏕◊✲ᡤ ⌧ᡤᒓ㸸බ┈㈈ᅋἲே༓ⴥ┴Ꮫᰯ⤥㣗఍㸧
࠙┠ⓗࠚ
∵ࠊ㇜࡞࡝ࡢ␆⏘ື≀ࡸࢧ࣮ࣔࣥࠊ࢚ࣅ࡞࡝ࡢ㣴Ṫ㨶௓㢮ࡢឤᰁ⑕ண㜵ཬࡧ἞⒪ࢆ┠ⓗ
࡜ࡋ࡚ከࡃࡢື≀⏝་⸆ရࡀ౑⏝ࡉࢀ࡚࠸ࡿࠋࡑࡢ୍᪉࡛ࠊ౑⏝ࡉࢀࡓື≀⏝་⸆ရࡀ᭱
⤊〇ရ࡛࠶ࡿ␆Ỉ⏘㣗ရ୰࡟ṧ␃ࡋࠊࡑࡢ㣗ရࢆࣄࢺࡀᦤྲྀࡍࡿࡇ࡜࡟ࡼࡿẘᛶࡸ㐣ᩄ⑕
ㄏⓎࠊ⭠ෆ⣽⳦ྀࡢኚ໬➼ࡀ㣗ရ⾨⏕ୖᙉࡃᠱᛕࡉࢀ࡚࠸ࡿࠋࡑࡢࡓࡵࠊ␆Ỉ⏘㣗ရࡢᦤ
ྲྀ࡟ࡼࡿ೺ᗣ⿕ᐖࢆᮍ↛࡟㜵ࡄ࡟ࡣࠊ㎿㏿࡞୍ᩧศᯒἲ࡟ࡼࡿṧ␃ື≀⏝་⸆ရࡢࣔࢽࢱ
ࣜࣥࢢ᳨ᰝ(ㄪᰝ)ࡀ㔜せ࡛࠶ࡿࠋ
୍ᩧศᯒἲࡣཌ⏕ປാ┬࠿ࡽࠕHPLC ࡟ࡼࡿື≀⏝་⸆ရࡢ୍ᩧヨ㦂ἲϨ㹼Ϫ(␆Ỉ⏘≀)ࠖ
(௨ୗࠊϨἲࠊϩἲࠊϪἲ࡜࠸࠺)ࡢ 3 ✀㢮ࡀ㏻▱ࡉࢀ࡚࠸ࡿ 1)ࠋϨἲࡣࢧࣝࣇ࢓๣ࠊ࢟ࣀࣟ
ࣥ๣➼ከࡃࡢື≀⏝་⸆ရࡀศᯒᑐ㇟࡜ࡉࢀࠊ᧯సࡶ⡆౽࡞ヨ㦂ἲ࡛࠶ࡿࠋࡋ࠿ࡋࠊࢸࢺ
ࣛࢧ࢖ࢡࣜࣥ⣔ᢠ⏕≀㉁(௨ୗࠊTCs ࡜࠸࠺)ࡀᢳฟࡉࢀ࡞࠸ࡇ࡜࠿ࡽࡇࢀࡽࡢᢠ⏕≀㉁࡜ྠ
᫬ศᯒࡍࡿࡇ࡜ࡀᅔ㞴࡛࠶ࡗࡓࠋϪἲࡣࢧࣝࣇ࢓๣࡟ຍ࠼ TCs ࡢศᯒࡀྍ⬟࡛࠶ࡿࡀ࢟ࣀ
ࣟࣥ๣ࡣᑐ㇟࡜ࡉࢀ࡚࠸࡞࠸࡞࡝ࠊϨἲ࡟ẚ࡭ศᯒᑐ㇟ື≀⏝་⸆ရࡀᑡ࡞࠸ࠋࡲࡓࠊ⬡
⫫ࢆ⁐ゎࡋ࡞࠸⁐፹࡟ࡼࡿᢳฟἲࡢࡓࡵ∵⫗࡞࡝⬡⫫ࢆྵࡴᅛయヨᩱ࠿ࡽࡢᢳฟࡀᅔ㞴࡛
࠶ࡾࠊ࠿ࡘ᧯సࡀ↹㞧࡛᫬㛫ࡀ࠿࠿ࡿ࡞࡝ࡢၥ㢟Ⅼࡀ࠶ࡗࡓࠋࡲࡓࠊࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮
ࣝࡣ㣗ရ࡬ࡢṧ␃ᇶ‽ࡣ୙᳨ฟ࡜ࡉࢀࠊ࿌♧࡟ࡼࡾಶูヨ㦂ἲࡀ♧ࡉࢀ࡚࠸ࡿࡇ࡜࠿ࡽ௚
ࡢື≀⏝་⸆ရ࡜ࡣู࡟ヨ㦂ࡍࡿᚲせࡀ࠶ࡗࡓࠋ
ࡑࡇ࡛ࠊᮏ◊✲࡛ࡣࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮ࣝࢆྵࡵࡓࢧࣝࣇ࢓๣ࠊ࢟ࣀࣟࣥ๣ࠊTCs ➼ࡢ୍
ᩧศᯒἲࡢ㛤Ⓨࢆ┠ⓗ࡜ࡋ࡚ࠊᾮయヨᩱ࡛࠶ࡿ㭜༸ࢆᑐ㇟࡜ࡋ࡚ࠊϪἲࢆᨵⰋࡋࡓື≀⏝
་⸆ရࡢ୍ᩧศᯒἲ(௨ୗࠊ㭜༸ヨ㦂ἲ࡜࠸࠺㸧ࢆ㛤Ⓨࡋࠊጇᙜᛶホ౯ࢆ⾜ࡗࡓࠋࡉࡽ࡟∵
⫗➼ࡢ⬡⫫ࢆྵࡴᅛయヨᩱࢆᑐ㇟࡜ࡋ࡚ࠊϨἲࢆᨵⰋࡋࡓື≀⏝་⸆ရࡢ୍ᩧศᯒἲ㸦௨
ୗࠊ㣗⫗࣭㨶௓㢮ヨ㦂ἲ࡜࠸࠺㸧ࢆ᳨ウࡋࡓࠋ
࠙᪉ἲࠚ
㸯 ヨᩱ
ヨᩱࡣ∵⫗ࠊ㭜⫗ࠊ㇜⫗ࠊࢺࣛ࢘ࢺࢧ࣮ࣔࣥ(ࢽࢪ࣐ࢫ)ࠊ㭜༸ࢆ⏝࠸ࡓࠋ∵⫗ࠊ㇜⫗ཬࡧ
㭜⫗ࡣ➽⫗㒊ศࢆ౑⏝ࡋࠊ⬡⫫ࡣྍ⬟࡞㝈ࡾ㝖ཤࡋࡓࠋ
㸰 ヨ⸆➼
ື≀⏝་⸆ရࡢᶆ‽ရࡣࠊ㭜༸ヨ㦂ἲ࡛ࡣ࿴ග⣧⸆ᕤᴗ♫〇ࠊ㛵ᮾ໬Ꮫ♫〇ཬࡧᯘ⣧⸆
ᕤᴗ♫〇ࡢ 45 ✀㢮ࢆ⏝࠸ࡓࠋ㣗⫗࣭㨶௓㢮ヨ㦂ἲ࡛ࡣࡉࡽ࡟ࢧࣝࣇ࢓๣(ࢫࣝࣇ࢓ࣈ࣓ࣟࣔ
㸫 㸫
ࢱࢪࣥࠊࢫࣝࣇ࢓ࢭࢱ࣑ࢻࠊࢫࣝࣇ࢓࢚ࢺ࢟ࢩࣆࣜࢲࢪࣥࠊࢫࣝࣇ࢓ࢺࣟ࢟ࢧࢰ࣮ࣝ)ࢆຍ
࠼ࡓ 49 ✀㢮ࢆ⏝࠸ࡓࠋヨ⸆ࡣ࿴ග⣧⸆ᕤᴗ♫〇ࡢ LC/MS ⏝࢔ࢭࢺࢽࢺࣜࣝࠊ࣓ࢱࣀ࣮ࣝࠊ
ࢠ㓟ࠊ㉸⣧Ỉࢆ⏝࠸ࡓࠋ࣊࢟ࢧࣥࡣṧ␃㎰⸆ヨ㦂⏝ࠊ࣓ࢱࡾࢇ㓟ࠊ㓑㓟ࡣ≉⣭ࢆ⏝࠸ࡓࠋ
n-ࣉࣟࣃࣀ࣮ࣝࡣ㛵ᮾ໬Ꮫ♫〇ࢆ⏝࠸ࡓࠋ
㸱 ⿦⨨ཬࡧ ᐃ᮲௳
LC㸸Prominence UFLC (ᓥὠ〇సᡤ〇) MS/MS㸸3200 QTrap (SCIEX ♫〇)
࣒࢝ࣛ㸸㭜༸ヨ㦂ἲ Atlantis T3 (2.1 mm™150 mm, 3 ȝm, Waters ♫〇)
㣗⫗࣭㨶௓㢮ヨ㦂ἲ InertSustain C18 (2.1 mm™150 mm, 3 ȝm, GL Sciences ♫〇)
࣒࢝ࣛ ᗘ㸸50Υ ⛣ື┦㸸(A)0.1%ࢠ㓟ࠊ(B)࢔ࢭࢺࢽࢺࣜࣝ
ࢢࣛࢪ࢙ࣥࢺ㸸(B) 0 ศ(5%)ĺ6 ศ(30%)ĺ9 ศ-14 ศ(100%)ĺ14.1 ศ(5%)ĺ19 ศ(5%)
ὶ㏿㸸0.4 mL/min ὀධ㔞㸸5 μL ࢖࢜ࣥ໬ἲ㸸ESI(Positive, Negative)
࢖࢜ࣥ※ ᗘ㸸550Υ ᐃ࣮ࣔࢻ㸸Scheduled MRM
ᑐ㇟ື≀⏝་⸆ရࡢศᯒ᮲௳ࢆ⾲㸯࡟♧ࡋࡓࠋ
㸲 ヨ㦂⁐ᾮࡢㄪ〇
1) 㭜༸ヨ㦂ἲ
ヨᩱ 5.0 g ࡟࢔ࢭࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.2%࣓ࢱࡾࢇ㓟(1:1:3)ΰᾮ 80 mL ࢆຍ࠼࡚࣍ࣔ
ࢪࢼ࢖ࢬࡋࠊ3,000 rpm ࡛ 5 ศ㛫㐲ᚰศ㞳ᚋࠊỈᒙࢆศྲྀࡋࡓࠋ㐲ᚰศ㞳ࡋࡓṧ␃≀࡟࢔ࢭ
ࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.2%࣓ࢱࡾࢇ㓟(1:1:3)ΰᾮ 40 mL ࢆຍ࠼࡚෌ᗘ࣍ࣔࢪࢼ࢖ࢬࡋࠊ
3,000 rpm ࡛ 5 ศ㛫㐲ᚰศ㞳ࡋࡓࠋᚓࡽࢀࡓỈᒙࢆྜࢃࡏࠊ50Υ࡛ 30㹼40 mL ࡲ࡛ῶᅽ⃰⦰
ࡋࡓࠋࡇࡢ⁐ᾮࢆ Oasis HLB (200 mg)࣮࢝ࢺࣜࢵࢪ࡟㈇Ⲵࡋࠊ㉸⣧Ỉ 5 mL ࡛Ὑίࡋࠊ࣮࢝
ࢺࣜࢵࢪࢆ஝⇱ࡉࡏࡓᚋࠊ࣓ࢱࣀ࣮ࣝ 5 mL ࡛⁐ฟࡋࡓࠋ⁐ฟᾮࢆῶᅽ஝ᅛࡋࡓᚋࠊ࣓ࢱࣀ
࣮ࣝ-Ỉ(1:4)ΰᾮ 5 mL ࡛ᐃᐜࡋࠊヨ㦂⁐ᾮ࡜ࡋࡓࠋ
2) 㣗⫗࣭㨶௓㢮ヨ㦂ἲ
ヨᩱ 5.0 g ࡟࢔ࢭࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.1%㓑㓟(1:1:2)ΰᾮ 30 mL ཬࡧ࢔ࢭࢺࢽࢺࣜࣝ
㣬࿴ n-࣊࢟ࢧࣥ 20 mL ࢆຍ࠼࡚࣍ࣔࢪࢼ࢖ࢬࡋࠊ3,000 rpm ࡛ 5 ศ㛫㐲ᚰศ㞳ᚋࠊ࢔ࢭࢺࢽ
ࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.1%㓑㓟ᒙࢆศྲྀࡋࡓࠋ㐲ᚰศ㞳ࡋࡓṧ␃≀࡟ṧࡗࡓ n-࣊࢟ࢧࣥᒙཬࡧ
࢔ࢭࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.1%㓑㓟(1:1:2)ΰᾮ 20 mL ࢆຍ࠼࡚෌ᗘ࣍ࣔࢪࢼ࢖ࢬࡋࠊ3,000
rpm ࡛ 5 ศ㛫㐲ᚰศ㞳ࡋࡓࠋn-࣊࢟ࢧࣥᒙࢆᤞ࡚ࠊᚓࡽࢀࡓ࢔ࢭࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.1%
㓑㓟ᒙࢆྜࢃࡏࠊ10,000 rpm ࡛ 5 ศ㛫ࠊ4Υ࡛㐲ᚰศ㞳ࡋࡓࠋࡇࡢ⁐ᾮ࡟ n-ࣉࣟࣃࣀ࣮ࣝ 10
mL ࢆຍ࠼ࠊ50Υ࡛⃰⦰ࡋࠊ⁐፹ࢆ㝖ཤࡋࡓࠋṧ␃≀࡟࢔ࢭࢺࢽࢺࣜࣝ-Ỉ(4:6)ΰᾮ 5 mLࠊ
࢔ࢭࢺࢽࢺࣜࣝ㣬࿴ n-࣊࢟ࢧࣥ 3 mL ࢆຍ࠼࡚㉸㡢Ἴ⁐ゎࡋࡓࠋࡇࡢ⁐ᾮࢆ 10,000 rpm ࡛ 5
ศ㛫ࠊ4Υ࡛㐲ᚰศ㞳ࡋࠊ࢔ࢭࢺࢽࢺࣜࣝ-Ỉᒙࢆヨ㦂⁐ᾮ࡜ࡋࡓࠋ
㸳 ጇᙜᛶホ౯
ཌ⏕ປാ┬ࡼࡾ㏻▱ࡉࢀࡓ㣗ရ୰࡟ṧ␃ࡍࡿ㎰⸆➼࡟㛵ࡍࡿヨ㦂ἲࡢጇᙜᛶホ౯࢞࢖ࢻ
ࣛ࢖ࣥ(௨ୗࠊ࢞࢖ࢻࣛ࢖ࣥ࡜࠸࠺)2)࡟ᇶ࡙ࡁࠊᐇ᪋⪅ 1 ྡ࣭2 ే⾜࣭5 ᪥㛫ࡢᯞศ࠿ࢀヨ㦂
࡟ࡼࡾヨ㦂ἲࡢጇᙜᛶࢆホ౯ࡋࡓࠋῧຍ⃰ᗘࡣ୍ᚊᇶ‽(0.01 ȝg/g)࠾ࡼࡧᇶ‽್࡟㏆࠸⃰ᗘ
㸫 㸫
(0.1 ȝg/g)ࡢ㸰⃰ᗘ࡜ࡋࡓࠋࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮ࣝࡢῧຍ⃰ᗘࡣ࿌♧࡛♧ࡉࢀࡓᐃ㔞㝈⏺್࡛
࠶ࡿ 0.0005 ȝg/g ࡜ࡋࡓࠋ
⾲1䚷MS/MSศᯒ䝟䝷䝯䞊䝍䞊
ື≀⏝
་⸆ရྡ
Positive mode
Sulfacetamide
Sulfisomidine
5-Hydoroxythiabendazole
Albendazole metabolite
Sulfadiazine
Sulfathiazole
Thiabendazole
Sulfapyridine
Marbofloxacin
Trimethoprim
Norfloxacin
Ofloxacin
Oxytetracycline
Sulfamerazine
Cyprofloxacin
Ormethoprim
Danofloxacin
Tetracycline
Enrofloxacin
Sulfisozole
Orbifloxacin
Sulfadimidine
Sulfamethoxypyridazine
Sarafloxacin
Difloxacin
RT (min)
㭜༸
ヨ㦂⏝
㣗⫗䞉㨶௓㢮
ヨ㦂ἲ
䠉
4.60
5.47
4.90
4.74
5.14
6.43
5.57
6.19
5.66
6.55
6.35
6.94
6.03
6.81
6.34
7.09
6.68
7.08
6.04
7.82
7.26
7.35
8.02
7.85
3.44
3.55
3.60
3.99
4.01
4.25
4.32
4.48
4.56
4.63
4.78
4.83
4.88
4.91
4.96
5.03
5.19
5.28
5.43
5.63
5.64
5.66
5.67
5.98
6.09
MRM for quantitation
ື≀⏝
་⸆ရྡ
156.1
124.1
191.0
133.2
156.0
156.0
175.1
156.2
72.0
230.2
231.0
318.3
426.1
92.1
231.1
122.9
82.1
410.2
316.3
156.1
352.3
124.0
156.0
342.2
299.2
21
26
61
56
36
36
61
41
61
61
41
46
46
41
41
61
56
51
46
31
61
31
41
56
56
13
29
37
41
21
19
35
19
41
33
55
23
25
41
51
35
65
23
23
19
23
33
23
25
39
MRM for quantitation
㣗⫗䞉㨶௓㢮
ヨ㦂ἲ
Piromidic acid
7.22
8.08
7.88
8.39
7.92
8.44
8.40
䠉
䠉
8.33
9.19
8.62
9.46
8.97
9.10
8.84
9.65
9.91
9.71
䠉
10.06
6.21
6.26
6.50
6.68
6.97
7.02
7.13
7.18
7.23
7.40
7.78
7.98
8.14
8.15
8.15
8.15
8.59
8.59
8.66
8.71
9.00
221.2
281.2
285.0
479.2
254.1
249.2
311.2
268.1
295.1
268.2
262.2
277.1
238.2
311.2
301.2
361.2
233.2
314.0
262.2
357.0
289.3
123.0
155.9
156.0
444.1
92.0
177.1
156.1
92.1
156.1
156.1
215.9
156.2
206.0
156.0
156.1
222.2
187.1
282.0
202.1
92.2
243.2
56
41
51
61
36
66
46
36
41
41
36
36
26
51
46
61
26
60
36
46
41
47
23
19
27
37
41
23
39
23
17
41
17
15
27
21
23
35
33
45
49
45
Negative mode
Thiamphenicol
Chloramphenicol
Sulfanitran
6.47
8.96
9.49
5.19
7.79
8.62
354.0
320.9
334.0
184.6
152.1
135.9
-45
-40
-60
-30
-24
-44
Morantel
215.1
279.2
218.2
240.2
251.2
256.1
202.2
250.1
363.1
291.3
320.2
362.2
461.2
265.1
332.2
275.3
358.2
445.2
360.3
240.2
396.1
279.2
281.2
386.1
400.2
RT (min)
㭜༸
ヨ㦂⏝
Q1 (m/z) Q3 (m/z) DP (V) CE (eV)
Sulfamonomethoxine
Sulfachlorpyridazine
Chlortetracycline
Sulfamethoxazole
Pyrimethamine
Sulfadoxine
sulfatroxazole
Sulfaethoxypyridazine
Sulfisoxazole
Oxolinic acid
Sulfabenzamide
Ethopabate
Sulfadimethoxine
Sulfaquinoxaline
Difurazon
Nalidixic acid
Flubendazole
Flumequine
Sulfabromomethazine
Q1 (m/z) Q3 (m/z) DP (V) CE (eV)
࠙⤖ᯝཬࡧ⪃ᐹࠚ
㸯 㭜༸ヨ㦂ἲ
1) ๓ฎ⌮ἲࡢ᳨ウ
Ϫἲ࡛ࡣ࣍ࣔࢪࢼ࢖ࢬᚋࡢヨᩱࢆࢣ࢖ࢯ࢘ᅵࢆ⏝࠸࡚྾ᘬࢁ㐣ࡍࡿࡀࠊ྾ᘬࢁ㐣ࡢ᧯స
ࡀ↹㞧࡛᫬㛫ࢆせࡍࡿࡇ࡜࠿ࡽࠊ」ᩘ᳨యࡢ᧯సᛶࢆྥୖࡉࡏࡿࡓࡵࠊ
࣍ࣔࢪࢼ࢖ࢬᚋ 3,000
rpm ࡛㐲ᚰศ㞳ࡋᾮ┦ࢆࢁ⣬࡛ࢁ㐣ࡋࡓࠋࢁᾮࡣ 40Υ௨ୗ࡛ 20 mL ࡟⃰⦰ࡋ࡚࠸ࡓࡀࡇࡢ
᧯స࡟᫬㛫ࢆせࡍࡿࡇ࡜࠿ࡽࠊ⃰⦰᪉ἲࢆ 50Υࠊ30㹼40 mL ࡟ኚ᭦ࡋࡓࠋࡇࢀ࡟ࡼࡾ 1 ᳨
య࠶ࡓࡾ⣙ 40 ศ࠿࠿ࡗ࡚࠸ࡓ⃰⦰᫬㛫ࢆ⣙ 20 ศ࡟▷⦰ࡍࡿࡇ࡜ࡀྍ⬟࡛࠶ࡗࡓࠋࡲࡓࠊ
ヨᩱ୰ࡢ࣐ࢺࣜࢵࢡࢫ࡟ࡼࡿᙳ㡪ࢆ☜ㄆࡋࡓ࡜ࡇࢁࠊ45 㡯┠୰ 13 㡯┠࡟࠾࠸࡚࢖࢜ࣥ໬ᢚ
ไཪࡣಁ㐍ࡀㄆࡵࡽࢀࡓࡇ࡜࠿ࡽࠊᐃ㔞ࡣ࣐ࢺࣜࢵࢡࢫῧຍᶆ‽ἲࢆ⏝࠸ࡿࡇ࡜࡜ࡋࡓࠋ
2) ጇᙜᛶホ౯
࢞࢖ࢻࣛ࢖ࣥ࡟ᚑ࠸ࠊ㑅ᢥᛶࠊᐃ㔞㝈⏺ཬࡧ┿ᗘ࣭⢭ᗘ࡟ࡘ࠸࡚┠ᶆ್࡟㐺ྜࡋ࡚࠸ࡿ
࠿ࢆ☜ㄆࡋࡓࠋࣈࣛࣥࢡヨᩱ࡟࠾ࡅࡿ㑅ᢥᛶࡢホ౯ࢆ⾜ࡗࡓ࡜ࡇࢁࠊᐃ㔞ࢆጉᐖࡍࡿࣆ࣮
ࢡࡣ☜ㄆࡉࢀ࡞࠿ࡗࡓࠋḟ࡟ᐃ㔞㝈⏺࡟ࡘ࠸࡚ࠊࣈࣛࣥࢡヨᩱ࡟ࡑࢀࡒࢀ 0.01 ȝg/g ῧຍࡋࠊ
ῧຍ⃰ᗘ࡟┦ᙜࡍࡿྛࣆ࣮ࢡࡀ S/N ẚӍ10 ࡛࠶ࡿࡇ࡜ࢆ☜ㄆࡋࡓࠋࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮ࣝ
ࡣᐃ㔞㝈⏺⃰ᗘ࡛࠶ࡿ 0.0005 ȝg/g ࢆῧຍࡋ☜ㄆࡋࡓࠋࡑࡢ⤖ᯝࠊ☜ㄆࡋࡓື≀⏝་⸆ရ 45
㡯┠ࡣࡍ࡭࡚ῧຍࡋࡓ⃰ᗘ࡟࠾࠸࡚ S/N ẚӍ10 ࢆ‶ࡓࡋࡓࠋࡇࢀࡽࡢື≀⏝་⸆ရ 45 㡯┠
࡟ࡘ࠸࡚ࠊ┿ᗘཬࡧ⢭ᗘࢆホ౯ࡋࡓࠋ⤖ᯝࢆ⾲ 2 ࡟♧ࡍࠋホ౯ࡋࡓື≀⏝་⸆ရ 45 㡯┠୰
41 㡯┠ࡀ┿ᗘ࣭⢭ᗘ࡜ࡶ┠ᶆ್࡟㐺ྜࡋࡓࠋࡋ࠿ࡋࠊᐃ㔞࡟࣐ࢺࣜࢵࢡࢫῧຍᶆ‽ἲࢆ⏝
࠸࡚࠸ࡿࡇ࡜࠿ࡽࠊ㏣ຍ⢭〇➼ࡢ᳨ウ࡟ࡼࡿ࣐ࢺࣜࢵࢡࢫຠᯝࡢపῶ໬ࡀᚲせ࡛࠶ࡿ࡜⪃
㸫 㸫
࠼ࡽࢀࡓࠋ
⾲2䚷㭜༸ヨ㦂ἲ䛾ጇᙜᛶホ౯䛾⤖ᯝ
1)
ື≀⏝
་⸆ရྡ
Sulfabenzamide
1)
0.01 ppm
┿ᗘ
(%)
(%)
87.7
93.9
93.2
89.6
100.5
87.2
96.9
92.5
107.5
90.7
84.8
96.8
88.0
92.1
99.0
91.9
93.4
1)
0.1 ppm
ే⾜⢭ᗘ ᐊෆ⢭ᗘ
(%)
┿ᗘ
(%)
ື≀⏝
་⸆ရྡ
ే⾜⢭ᗘ ᐊෆ⢭ᗘ
(%)
(%)
7.49
7.89
88.2
4.98
5.65
Sulfachlorpyridazine
6.91
6.91
93.8
3.02
4.47
Sulfadiazine
1.85
5.55
91.3
1.58
2.50
Sulfadimethoxine
4.11
4.11
89.4
4.30
5.84
Sulfadimidine
5.93
11.40
97.1
1.52
2.38
Sulfadoxine
4.36
10.40
92.6
2.33
4.67
Sulfamerazine
4.87
6.79
91.3
3.05
5.57
Sulfamethoxazole
7.13
7.13
92.5
3.45
5.37
Sulfamethoxypyridazine
10.35
11.48
97.5
3.33
3.75
Sulfamonomethoxine
8.53
10.06
96.5
6.57
6.60
Sulfanitran
3.07
14.92
88.7
2.54
6.42
Sulfapyridine
3.68
4.31
92.8
3.51
5.25
Sulfaquinoxaline
3.40
9.73
86.3
2.47
4.78
Sulfathiazole
1.10
6.17
89.3
2.66
3.95
Sulfisomidine
1.46
3.97
92.1
2.38
3.66
Sulfisoxazole
3.39
10.87
89.9
7.86
8.41
Sulfisozole
6.60
6.60
90.4
3.45
3.45
2)
34.41
44.73
37.9
31.17
47.98
Cyprofloxacin
25.2
Danofloxacin
84.9
8.48
10.77
91.6
6.99
8.28
Difloxacin
81.3
8.10
15.25
89.5
5.22
5.57
Enrofloxacin
92.3
8.24
10.45
94.0
5.81
6.15
Marbofloxacin
85.6
7.25
13.07
87.5
6.32
6.47
30.46
47.27
39.4
27.15
46.20
Norfloxacin
29.2
1)䚷Chloramphenicol䛿ᐃ㔞㝈⏺⃰ᗘ䛷䛒䜛0.0005 㽀g/g䜢ῧຍ
2)䚷ጇᙜᛶホ౯䛾ᛶ⬟䝟䝷䝯䞊䝍䞊䛻㐺ྜ䛧䛺䛛䛳䛯㡯┠䜢ୗ⥺䛷グ㍕䛧䛯䚹
Ofloxacin
Orbifloxacin
Sarafloxacin
Flumequine
Nalidixic acid
Oxolinic acid
Piromidic acid
Ethopabate
Ormethoprim
Pyrimethamine
Trimethoprim
Thiamphenicol
Albendazole metabolite
Flubendazole
Morantel
5-Hydoroxythiabendazole
Thiabendazole
Difurazon
Chlortetracycline
Oxytetracycline
Tetracycline
Chloramphenicol
1)
0.01 ppm
┿ᗘ
0.1 ppm
ే⾜⢭ᗘ ᐊෆ⢭ᗘ
┿ᗘ
ే⾜⢭ᗘ ᐊෆ⢭ᗘ
(%)
(%)
(%)
(%)
(%)
(%)
89.4
93.2
19.9
89.1
91.3
100.3
85.1
93.5
96.1
73.9
91.4
88.3
81.9
84.0
76.6
109.8
88.6
23.9
71.3
87.1
98.9
89.1
3.44
9.34
41.81
4.36
3.76
2.87
1.22
6.75
6.35
7.03
10.11
5.41
4.23
3.76
6.76
3.80
5.78
11.91
4.10
10.25
9.05
12.41
14.04
11.14
86.21
11.82
9.81
12.33
9.06
8.70
11.24
16.33
13.41
12.21
5.69
5.29
7.37
9.62
8.98
25.78
10.20
12.56
17.55
12.51
96.7
92.2
38.7
89.1
88.9
98.9
83.2
91.5
99.2
78.6
97.1
97.4
82.9
84.2
80.6
109.8
91.6
25.1
82.4
88.1
89.5
90.9
2.76
3.64
25.70
3.05
4.10
3.74
1.03
2.05
4.55
7.87
2.55
3.21
2.69
1.45
3.75
2.65
5.25
17.08
3.38
2.21
5.70
12.52
2.76
5.60
39.09
7.91
4.79
5.96
6.69
4.81
5.44
10.55
5.13
3.52
3.60
3.31
7.77
6.04
5.25
33.78
6.47
2.86
8.20
12.52
㸰 㣗⫗࣭㨶௓㢮୰ࡢື≀⏝་⸆ရ୍ᩧศᯒἲ
1) ๓ฎ⌮ἲࡢ᳨ウ
Ϩἲ࡛ࡣᢳฟ⁐፹࡟࢔ࢭࢺࢽࢺࣜࣝࢆ⏝࠸࡚࠸ࡿࡀ TCs ࡀᢳฟࡉࢀ࡞࠸ࡇ࡜࠿ࡽࠊ࢔ࢭ
ࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ(1:1)࡟ኚ᭦ࡋࠊỈࢆᢳฟ⁐፹㔞ࡢ 30%ࠊ40%ࠊ50%ࡢ๭ྜ࡛ຍ࠼ࡓ 3
✀㢮ࡢᢳฟ⁐፹ࢆ᳨ウࡋࡓࠋࡑࡢ⤖ᯝࠊTCs ࡢᅇ཰⋡ࡣỈ 50%ࡢᢳฟ⁐፹ࡀ᭱ࡶ㧗࠿ࡗࡓ
ࡶࡢࡢ 65.2㹼74.7%࡜┿ᗘࡢ┠ᶆ್(70%㹼120%)ࢆୗᅇࡗࡓࠋTCs ࡣ 2 ౯ࡢ㔠ᒓ࢖࢜ࣥ࡜࢟
࣮ࣞࢺࢆ⏕ᡂࡋࡸࡍ࠸ࡇ࡜࠿ࡽࠊᢳฟ⁐፹࡟ῧຍࡍࡿỈࢆ 0.1%㓑㓟࡟ኚ᭦ࡋࡓ࡜ࡇࢁࠊTCs
ࡢᅇ཰⋡ࡀ 76.8%㹼83.7%࡟ྥୖࡋࡓࡇ࡜࠿ࡽᢳฟ⁐፹ࡣ࢔ࢭࢺࢽࢺࣜࣝ-࣓ࢱࣀ࣮ࣝ-0.1%
㓑㓟(1:1:2)ࢆ᥇⏝ࡋࡓࠋࡲࡓࠊᢳฟ⁐፹࡟ 0.1%㓑㓟ࢆῧຍࡋࡓࡇ࡜࡟ࡼࡾ⁐፹ࡢ㝖ཤ࡟᫬
㛫ࢆせࡋࡓࡇ࡜࠿ࡽࠊ㭜༸ヨ㦂ἲ࡜ྠᵝ࡟⁐፹㝖ཤࢆ⾜࠺㝿ࡢ ᗘࢆ 40Υ࠿ࡽ 50Υ࡟ኚ᭦
ࡋࠊ㝖ཤ࡟せࡍࡿ᫬㛫ࢆ▷⦰ࡋࡓࠋḟ࡟ᮏἲ࡟ࡼࡾᢳฟ࣭⢭〇ࡋࡓヨ㦂⁐ᾮ୰࡟ṧᏑࡍࡿ
࣐ࢺࣜࢵࢡࢫ࡟ࡼࡿᙳ㡪ࢆ☜ㄆࡋࡓ࡜ࡇࢁࠊ49 㡯┠୰ 25 㡯┠࡟࠾࠸࡚࢖࢜ࣥ໬ᢚไࡲࡓࡣ
ಁ㐍ࡀㄆࡵࡽࢀࡓࡇ࡜࠿ࡽᐃ㔞ࡣ࣐ࢺࣜࢵࢡࢫῧຍᶆ‽ἲࢆ⏝࠸ࡿࡇ࡜࡜ࡋࡓࠋ
2) ῧຍᅇ཰ヨ㦂
᳨ウࡋࡓヨ㦂ἲ࡟ࡘ࠸࡚ྛ᳨ウヨᩱ n=5 ࡢῧຍᅇ཰ヨ㦂ࢆ⾜࠸ࠊ┿ᗘཬࡧే⾜⢭ᗘࢆホ
౯ࡋࡓ(ῧຍ⃰ᗘ㸸ࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮ࣝ 0.0005 ȝg/gࠊࡑࡢ௚ࡢື≀⏝་⸆ရࡣ 0.01 ȝg/g)ࠋ
⤖ᯝࢆ⾲ 3 ࡟♧ࡍࠋ┿ᗘཬࡧే⾜⢭ᗘࡀ┠ᶆ್(70%㹼120%ࠊ25%ᮍ‶)ࢆ‶ࡓࡍ⤖ᯝࡀᚓࡽ
ࢀࡓື≀⏝་⸆ရࡣ∵⫗ࠊ㇜⫗ཬࡧࢺࣛ࢘ࢺࢧ࣮࡛ࣔࣥ 46 㡯┠ࠊ㭜⫗࡛ 48 㡯┠࡛࠶ࡗࡓࠋ
ࡲࡓࠊ࠸ࡎࢀࡢヨᩱ࡟࠾࠸࡚ࡶࣈࣛࣥࢡヨᩱ࡟ᐃ㔞ࢆጉᐖࡍࡿࣆ࣮ࢡࡣ࡞ࡃࠊ㑅ᢥᛶ࡟ၥ
㢟ࡣ࡞࠿ࡗࡓࠋࡇࡢᡂᯝࢆඖ࡟ࠊ᳨ウࡋࡓヨ㦂ἲࡢጇᙜᛶࢆホ౯ࡍࡿணᐃ࡛࠶ࡿࠋ
㸫 㸫
⾲3 㣗⫗䞉㨶㢮ヨ㦂ἲ䛾ῧຍᅇ཰ヨ㦂⤖ᯝ (n=5)
ື≀⏝
་⸆ရྡ
∵➽⫗
┿ᗘ
(%)
ే⾜⢭ᗘ
Sulfadiazine
Sulfadimethoxine
㇜➽⫗
ే⾜⢭ᗘ
(RSD%)
┿ᗘ
(%)
79.1
4.9
80.2
㭜➽⫗
ే⾜⢭ᗘ
(RSD%)
┿ᗘ
(%)
80.4
9.5
3.7
91.8
12.3
䝖䝷䜴䝖䝃䞊䝰䞁
ే⾜⢭ᗘ
(RSD%)
┿ᗘ
(%)
87.9
5.4
78.4
4.0
96.0
4.8
70.6
ື≀⏝
་⸆ရྡ
∵➽⫗
┿ᗘ
(%)
ే⾜⢭ᗘ
Cyprofloxacin
7.1
㇜➽⫗
ే⾜⢭ᗘ
(RSD%)
┿ᗘ
(%)
93.9
5.7
Danofloxacin
85.3
(RSD%)
㭜➽⫗
䝖䝷䜴䝖䝃䞊䝰䞁
ే⾜⢭ᗘ
(RSD%)
┿ᗘ
(%)
(RSD%)
┿ᗘ
(%)
84.8
4.5
82.8
5.9
85.0
7.0
6.2
94.7
4.9
94.1
4.9
95.7
4.7
ే⾜⢭ᗘ
(RSD%)
Sulfadimidine
78.1
8.0
82.5
6.1
81.4
3.4
86.0
5.1
Enrofloxacin
87.7
2.0
90.9
6.4
93.6
4.1
91.2
4.3
Sulfadoxine
80.0
2.8
91.2
10.4
109.3
6.7
87.4
5.4
Norfloxacin
83.8
4.0
89.5
7.3
88.0
9.6
86.0
13.0
Sulfamerazine
83.5
2.8
93.8
11.3
104.0
5.4
88.2
5.0
Ofloxacin
93.4
1.7
92.7
5.9
92.7
6.2
84.8
9.5
Sulfamethoxazole
74.8
8.1
73.0
7.7
77.9
4.1
72.3
5.1
Difloxacin
84.9
5.7
86.2
6.2
86.8
4.0
86.5
4.8
Sulfamethoxypyridazine
80.3
9.0
80.7
7.2
91.0
5.9
86.6
3.0
Marbofloxacin
95.2
4.9
95.9
6.2
92.0
10.1
88.9
14.0
Sulfamonomethoxine
78.4
8.6
81.9
7.8
93.8
4.8
83.0
5.6
Orbifloxacin
87.3
4.5
99.0
7.1
105.2
4.1
88.8
5.1
Sulfaquinoxaline
85.7
5.9
99.6
16.4
113.4
7.5
80.3
7.9
Sarafloxacin
96.1
7.3
128.6
14.8
111.7
11.3
90.9
4.7
3.9
Sulfathiazole
78.2
5.9
82.3
8.9
94.2
9.6
85.9
4.5
Ethopabate
83.4
10.1
102.6
9.2
100.6
3.3
92.2
Sulfisomidine
86.2
3.3
89.7
4.9
103.9
5.4
81.4
5.5
Ormethoprim
93.1
5.2
97.4
8.0
87.8
6.7
91.9
8.9
Sulfisoxazole
73.8
7.3
86.0
7.3
99.3
6.1
81.7
4.4
Pyrimethamine
81.4
5.2
89.9
6.0
81.2
2.3
88.5
1.2
Sulfisozole
71.9
9.1
79.3
10.2
89.8
8.9
74.0
8.9
Thiamphenicol
91.1
4.8
86.0
9.8
83.3
7.4
86.8
4.0
59.0
Sulfachlorpyridazine 71.0
3.9
69.0
5.6
79.3
7.4
75.9
10.7
Trimethoprim
92.8
5.6
99.5
3.6
101.0
6.0
90.0
12.5
6.4
78.6
6.2
85.0
3.8
80.9
2.0
Albendazole metabolite
89.2
4.7
88.3
4.0
86.2
4.3
86.7
5.8
Sulfanitran
6.9
96.6
18.6
93.8
7.9
84.9
11.6
Flubendazole
78.6
7.4
87.7
11.2
83.7
3.2
65.5
11.8
Sulfabenzamide
1)
95.3
Sulfapyridine
86.2
7.2
92.1
12.0
107.7
9.0
93.6
12.6
Morantel
88.1
6.2
85.4
10.3
81.4
3.6
76.5
3.9
Sulfabromomethazine
69.2
6.3
80.2
11.1
87.0
3.8
66.4
20.5
5-Hydoroxythiabendazole
79.1
2.2
82.4
6.0
81.1
7.2
74.5
7.4
Sulfacetamide
76.0
5.2
71.3
6.7
88.3
5.3
78.0
7.6
Thiabendazole
87.3
6.8
82.1
5.0
82.2
5.4
80.9
4.9
Sulfaethoxypyridazine
76.2
9.9
83.4
5.2
93.2
4.3
82.1
3.1
Difurazon
51.0
3.7
50.6
25.4
52.5
14.8
31.9
10.8
Sulfatroxazole
71.0
9.6
83.3
8.9
89.5
4.8
80.0
3.3
Chlortetracycline
76.1
8.1
90.9
5.1
81.6
1.5
75.2
2.3
Flumequine
82.2
7.4
94.4
16.7
101.7
6.7
75.4
9.3
Oxytetracycline
85.6
4.8
90.3
7.2
88.2
4.6
89.5
17.0
Nalidixic acid
81.0
6.2
89.2
9.0
95.6
3.9
77.7
7.9
Tetracycline
79.3
2.0
91.0
6.5
77.6
7.4
79.9
4.5
Oxolinic acid
73.3
2.9
88.3
9.9
93.6
2.8
79.6
9.0
Chloramphenicol
74.1
14.0
85.4
9.7
84.6
12.0
100.3
13.2
Piromidic acid
90.7
3.6
99.5
12.3
102.4
3.6
78.4
5.4
1) ┿ᗘཬ䜃ే⾜⢭ᗘ䛜┠ᶆ್(70%䡚120%䚸25%ᮍ‶)䛻㐩䛧䛶䛔䛺䛔㡯┠䜢ୗ⥺䛷グ㍕䛧䛯䚹
࠙ࡲ࡜ࡵࠚ
㣗ရ୰࡟ṧ␃ࡍࡿࢡ࣒ࣟࣛࣇ࢙ࢽࢥ࣮ࣝࢆྵࡵࡓື≀⏝་⸆ရࡢ୍ᩧศᯒἲ࡜ࡋ࡚ࠊϪ
ἲࢆᨵⰋࡋࡓ㭜༸ヨ㦂ἲཬࡧϨἲࢆᨵⰋࡋࡓ㣗⫗࣭㨶௓㢮ヨ㦂ἲࢆ㛤Ⓨࡋࡓࠋࡑࡢ⤖ᯝࠊ
ࡇࢀࡲ࡛㏻▱ἲ࡛ࡣ୍ᩧศᯒࡀᅔ㞴࡛࠶ࡗࡓࢧࣝࣇ࢓๣ࠊ࢟ࣀࣟࣥ๣ࠊTCs ཬࡧࢡ࣒ࣟࣛࣇ
࢙ࢽࢥ࣮ࣝ➼ࡢື≀⏝་⸆ရࡢ୍ᩧศᯒࡀྍ⬟࡜࡞ࡗࡓࠋᮏἲࡣ㣗ရ୰࡟ṧ␃ࡍࡿື≀⏝
་⸆ရ࡟ࡼࡿ೺ᗣ༴ᐖࢆ㜵Ṇࡍࡿࡓࡵࠊከᩘࡢ㣗ရࢆ㎿㏿࠿ࡘຠ⋡ⓗ࡟᳨ᰝࡍࡿୖ࡛᭷⏝
࡞ヨ㦂ἲ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿࠋ௒ᚋࠊ⢭〇➼ࡢ㏣ຍ࡟ࡼࡿ࣐ࢺࣜࢵࢡࢫຠᯝࡢపῶ໬ཬࡧ
ࣁࢳ࣑ࢶࡸ࢚ࣅ࡞࡝ࡢ␆Ỉ⏘≀࡬ࡢ㐺⏝࡟ࡘ࠸᳨࡚ウࢆ⾜࠺ணᐃ࡛࠶ࡿࠋ
࠙ཧ⪃ᩥ⊩➼ࠚ
1) 㣗ရ࡟ṧ␃ࡍࡿ㎰⸆ࠊ㣫ᩱῧຍ≀ཪࡣື≀⏝་⸆ရࡢᡂศ࡛࠶ࡿ≀㉁ࡢヨ㦂ἲ࡟ࡘ࠸࡚
(ᖹᡂ 17 ᖺ 1 ᭶ 24 ᪥௜ࡅ㣗ᏳⓎ➨ 0124001 ྕ)
2) 㣗ရ୰࡟ṧ␃ࡍࡿ㎰⸆➼࡟㛵ࡍࡿヨ㦂ἲࡢጇᙜᛶホ౯࢞࢖ࢻࣛ࢖ࣥࡢ୍㒊ᨵṇ࡟ࡘ࠸
࡚(ᖹᡂ 22 ᖺ 12 ᭶ 24 ᪥௜ࡅ㣗ᏳⓎ 1224 ➨ 1 ྕ)
࠙⤒㈝౑㏵᫂⣽ࠚ
40,284 ෇
ヨ⸆(ᶆ‽ရࠊ᭷ᶵ⁐፹➼)
LC-MS/MS ⏝ศᯒ࣒࢝ࣛ
143,786 ෇
๓ฎ⌮⏝ᾘ⪖ရ(ᅛ┦ᢳฟ࣒࢝ࣛ➼)
115,106 ෇
864 ෇
᣺㎸ࡳᡭᩘᩱ
ྜィ(㈓㔠฼ᜥ 40 ෇ྵࡴ)
300,040 ෇
㸫 㸫