8 5 Vol. 8 No. 5 2017 5 Journal of Food Safety and Quality May., 2017 李建辉 1, 张朝晖 1*, 王琳 2, 韩深 1, 程甲 3, 何悦 1, 崔凤云 1, 赵善贞刘韦华 1, 李小林 1, 刘鑫 1, 严华 1, 齐鹤鸣 1 1, 吕东阳 (1., 100026; 2., 100088; 3., 200135) 3, 摘要 :,, 6, 3, -,,, -,, 关键词 : ; ; ; ; ; ; ; Research progress of analysis of illegal additives in weight-reducing dietary supplements LI Jian-Hui 1, ZHANG Zhao-Hui 1*, WANG Lin 2, HAN Shen 1, CHENG Jia 3, HE Yue 1, CUI Feng-Yun 1, ZHAO Shan-Zhen 3, LIU Wei-Hua 1, LI Xiao-Lin 1, LIU Xin 1, YAN Hua 1, QI He-Ming 1, LV Dong-Yang 1 (1. Beijing Entry-Exit Inspection and Quarantine Bureau, Inspection and Quarantine Testing Center, Beijing 100026, China; 2. General Administration of Quality Supervision, Inspection and Quarantine of the People s Republic of China, Research Center for international inspection and Quarantine Standard and Technical Regulation, Beijing 100088, China; 3. Shanghai Entry-Exit Inspection and Quarantine Bureau, Technical Center for Animal Plant and Food Inspection and Quarantine, Shanghai 200135, China) ABSTRACT: After a brief introduction of the definition and risk factors of overweight and obesity, this paper presented and discussed the types, extraction and detection methods of illegal additives in weight-reducing dietary supplements. More than 100 synthetic drugs are adulterated into dietary supplements individually or in combination, including appetite suppressant, energy expenditure enhancer, drugs for preventing digestion and absorption, drugs for influencing lipid metabolism, diuretic and antidepressant. The applicability and limitations of existing analytical methods were summarized. Compared with gas chromatography, thin layer chromatography, enzyme linked 基金项目 : (2015IK012 2016IK021) Fund: Supported by Science and Technology Planning Project of General Administration of Quality Supervision, Inspection and Quarantine (AQSIQ) of P.R. China (2015IK012 and 2016IK021) * 通讯作者 :,,, E-mail: zhangzhh@bjciq.gov.cn *Corresponding author: ZHANG Zhao-Hui, Ph.D, Senior Engineer, Inspection and Quarantine Testing Center, Beijing Entry-Exit Inspection and Quarantine Bureau, No.6 TianshuiyuanJie, Chaoyang District, Beijing 100026, China. E-mail: zhangzhh@bjciq.gov.cn
1586 8 immunosorbent assay and nuclear magnetic resonance, high performance liquid chromatography combined with tandem mass spectrometric detection is the most commonly used technique. For tablets, capsules and granules, liquid solid extraction is the main sample pretreatment method. Although the current analysis methods can basically meet the actual detection requirements, there are some defects in the face of new drugs and high throughput screening, such as simultaneously extracting and pre-treating of the compounds with different polarities and improving the speed of analysis for high throughput screening. Direct analysis in real time-high resolution mass spectrometry has the advantages of high speed, accuracy and efficiency, which can be used to fill the gaps and screen illegal additives in weight-reducing dietary supplements. KEY WORDS: weight-reducing dietary supplements; illegal additive; high performance liquid chromatography; gas chromatography; thin layer chromatography; enzyme linked immunosorbent assay; mass spectrometry; nuclear magnetic resonance 1 引言,,,,,, (over the counter, OTC), ( ) [1],,,,,,,, [2] [3],,, [4],, (1), (solid-liquid extraction, SLE) - (liquid-liquid extraction, LLE) (desorption corona beam ionization, DCBI) QuEChERS(quick, easy, cheap, effective, rugged, safe) ; (2), (thin layer chromatography, TLC) (liquid chromatography, LC) (capillary electrophoresis, CE) (ion mobility spectrometry, IMS) (gas chromatography, GC) X (X-ray diffraction, XRD) (enzyme-linked immunosorbent assay, ELISA) (nuclear magnetic resonance, NMR), 2 非法添加物种类 [2-64], 111 ( 1), [5-7], : (1) ( N- N- ); (2) ( β- ); (3) ( ); (4) ( ); (5) ( ); (6) ( ) 3 检测方法 [2,4,5,7-58], (diode array detector, DAD) [4,31,42,50] (fluorescence detector, FLD) [8,13] (mass spectrometer, MS) [4,24,27,29,30,35,36,40,41,43,44,49,51-55], [4,8,40,54] [12,56] (attenuated total reflectance infrared spectroscopy, ATR-IR) [57] [16] - [3] X [58] [59]
5, : 1587 表 1 111 种违法添加化合物信息表 Table 1 Information of 111 illegal additives CAS 1 althiazide 5588-16-9 C 11 H 14 ClN 3 O 4 S 3 2 acarbose 56180-94-0 C 25 H 43 NO 18 3 amiloride 2016-88-8 C 6 H 8 ClN 7 O 4 diazepam 439-14-5 C 16 H 13 ClN 2 O 5 amfepramone 90-84-6 C 13 H 19 NO 6 amphetamine 300-62-9 C 9 H 13 N 7 bupropion 34911-55-2 C 13 H 18 ClNO 8 triamterene 396-01-0 C 12 H 11 N 7 9 orlistat 96829-58-2 C 29 H 53 NO 5 10 oxethazaine 126-27-2 C 28 H 41 N 3 O 3 11 bambuterol 81732-65-2 C 18 H 29 N 3 O 5 12 phenobarbital 50-06-6 C 12 H 12 N 2 O 3 13 phenylalanine 150-30-1(DL), 63-91-2(L) C 9 H 11 NO 2 14 phenylpropanolamine 14838-15-4 C 9 H 13 NO 15 phentermine 122-09-8 C 10 H 15 N 16 benfluorex 23602-78-0 C 19 H 20 F 3 NO 2 17 phenmetrazine 134-49-6 C 11 H 15 NO 18 phendimetrazine 634-03-7 C 12 H 17 NO 19 phenytoin 57-41-0 C 15 H 12 N 2 O 2 20 isoxsuprine 395-28-8 C 18 H 23 NO 3 21 phenformin 114-86-3 C 10 H 15 N 5 22 ethyl 4-aminobenzoate 94-09-7 C 9 H 11 NO 2 23 bisacodyl 603-50-9 C 22 H 19 NO 4 24 benzfetamine 156-08-1 C 17 H 21 N 25 bendroflumethiazide 73-48-3 C 15 H 14 F 3 N 3 O 4 S 2 26 benzthiazide 91-33-8 C 15 H 14 ClN 3 O 4 S 3 27 probenecid 57-66-9 C 13 H 19 NO 4 S 28 bumetanide 28395-03-1 C 17 H 20 N 2 O 5 S 29 theophylline 58-55-9 C 7 H 8 N 4 O 2 30 acetazolamide 59-66-5 C 4 H 6 N 4 O 3 S 2 31 emodin 518-82-1 C 15 H 10 O 5 32 usnic acid 125-46-2 C 18 H 16 O 7 33 dobutramine 14648-57-8 C 12 H 20 O 34 metformin 657-24-9 C 4 H 11 N 5 35 A sennoside A 81-27-6 C 42 H 38 O 2 0 36 B sennoside B 128-57-4 C 42 H 38 O 2 0 37 C sennoside C 37271-16-2 C 42 H 40 O 19 38 D sennoside D 37271-17-3 C 42 H 40 O 19 39 A sennidin A 641-12-3 C 30 H 18 O 10 40 B sennidin B 517-44-2 C 30 H 18 O 10
1588 8 续表 1 CAS 41 fenoterol 13392-18-2 C 17 H 21 NO 4 42 phenothiazine 92-84-2 C 12 H 9 NS 43 phenolphthalein 77-09-8 C 20 H 14 O 4 44 phentolamine 50-60-2 C 17 H 19 N 3 O 45 furosemide 54-31-9 C 12 H 11 ClN 2 O 5 S 46 fenfluramine 458-24-2 C 12 H 16 F 3 N 47 fluoxetine 54910-89-3 C 17 H 18 F 3 NO 48 cyclothiazide 2259-96-3 C 14 H 16 ClN 3 O 4 S 2 49 gemfibrozil 25812-30-0 C 15 H 22 O 3 50 methyl amphetamine 537-46-2 C 10 H 15 N 51 methylephedrine 552-79-4 C 11 H 17 NO 52 thyroxine 51-49-0(D), 51-48-9(L) C 15 H 11 O 4 I 4 N 53 caffeine 58-08-2 C 8 H 10 N 4 O 2 54 theobromine 83-67-0 C 7 H 8 N 4 O 2 55 clenpenterol 37158-47-7 C 13 H 20 Cl 2 N 2 O 56 clenbuterol 37148-27-9 C 12 H 18 Cl 2 N 2 O 57 ractopamine 97825-25-7 C 18 H 23 NO 3 58 rimonabant 168273-06-1 C 22 H 21 Cl 3 N 4 O 59 sulbutiamine 3286-46-2 C 32 H 46 N 8 O 6 S 2 60 lorcaserin 616202-92-7 C 11 H 14 ClN 61 chlorphentermine 461-78-9 C 10 H 14 ClN 62 clobenzorex 13364-32-4 C 16 H 18 ClN 63 clorprenaline 3811-25-4 C 11 H 16 ClNO 64 clopamide 636-54-4 C 14 H 20 ClN 3 O 3 S 65 chlorothiazide 58-94-6 C 7 H 6 ClN 3 O 4 S 2 66 chlorthalidone 77-36-1 C 14 H 11 ClN 2 O 4 S 67 spironolactone 52-01-7 C 24 H 32 O 4 S 68 ephedrine 299-42-3 C 10 H 15 NO 69 mabuterol 56341-08-3 C 13 H 18 ClF 3 N 2 O 70 mapenterol 54238-51-6 C 14 H 20 ClF 3 N 2 O 71 mazindol 22232-71-9 C 16 H 13 ClN 2 O 72 metolazone 17560-51-9 C 16 H 16 ClN 3 O 3 S 73 modafinil 68693-11-8 C 15 H 15 NO 2 S 74 nefazodone 83366-66-9 C 25 H 32 ClN 5 O 2 75 paroxetine 61869-08-7 C 19 H 20 FNO 3 76 meperidine 57-42-1 C 15 H 21 NO 2 77 penbutolol 36507-48-9 C 18 H 29 NO 2 78 propranolol 525-66-6 C 16 H 21 NO 2 79 hydroflumethiazide 135-09-1 C 8 H 8 F 3 N 3 O 4 S 2 80 hydrochlorothiazide 58-93-5 C 7 H 8 ClN 3 O 4 S 2
5, : 1589 续表 1 CAS 81 cathine hydrochloride 492-39-7 C 9 H 13 NO 82 salbutamol 18559-94-9 C 13 H 21 NO 3 83 sertraline 79617-96-2 C 32 H 38 N 4 O 12 S 3 84 strychnine 57-24-9 C 21 H 22 N 2 O 2 85 salicin 138-52-3 C 13 H 18 O 7 86 terbutaline 23031-25-6 C 12 H 19 NO 3 87 topiramate 97240-79-4 C 12 H 21 NO 8 S 88 torasemide 56211-40-6 C 16 H 20 N 4 O 3 S 89 tulobuterol 41570-61-0 C 12 H 18 ClNO 90 pseudoephedrine 90-82-4 C 10 H 15 NO 91 penfluridol 26864-56-2 C 28 H 27 ClF 5 NO 92 sibutramine 106650-56-0 C 17 H 26 ClN 93 cimbuterol 54239-39-3 C 13 H 19 N 3 O 94 sildenafil 139755-83-2 C 22 H 30 N 6 O 4 S 95 cimaterol 54239-37-1 C 12 H 17 N 3 O 96 citalopram 59729-33-8 C 20 H 21 FN 2 O 97 synephrine 94-07-5 C 9 H 13 NO 2 98 brombuterol 41937-02-4 C 12 H 18 Br 2 N 2 O 99 nicotinamide 98-92-0 C 6 H 6 N 2 O 100 bergenin 477-90-7 C 14 H 16 O 9 101 ethacrynic acid 58-54-8 C 13 H 12 Cl 2 O 4 102 indapamide 26807-65-8 C 16 H 16 ClN 3 O 3 S 103 yohimbine 146-48-5 C 21 H 26 N 2 O 3 104 L-carnitine 541-15-1 C 7 H 15 NO 3 105 zonisamide 68291-97-4 C 8 H 8 N 2 O 3 S 106 2,4-2,4-dinitrophenol 51-28-5 C 6 H 4 N 2 O 5 107 3,3,5-3,3,5 -triiodo-l-thyronine 6893-2-3 C 15 H 12 I 3 NO 4 108 3,3,5-3,3,5-triiodo-l-thyronine 5817-39-0 C 15 H 12 I 3 NO 4 109 3,5-3,5-diiodo-l-thyronine 1041-01-6 C 15 H 13 I 2 NO 4 110 N- n-di-desmethyl sibutramine 262854-36-4 C 15 H 22 ClN 111 N- n-mono-desmethyl sibutramine 84467-94-7 C 17 H 26 CIN 3.1 样品前处理, ( )3,,,,,,,, 3.1.1 固 - 液萃取 - 2 :
1590 8 -,,,,, -,,,,,, (3600 g, 5 min) (16000 g, 3 min)2, (liquid chromatography-mass spectrometry, LC-MS) [10], HPLC [2], 30 min, 22 4000 r/min 5 min, 2000 5000, 0.22 μm [60] 3.1.2 液 - 液萃取 - ( ),, : (9:1, V:V) (3600 g, 5 min),,, (16000 g, 3 min), LC-MS [10] -, 3.1.3 解吸附电晕束电离 (atmosphere pressure chemical ionization, APCI),,,,,,, (DCBI-MS), [59] 3.1.4 QuEChERS, QuEChERS, (solid phase extraction, SPE),,, β-, 6 (cleanert alumina-n cleanert C18 florisil cleanert pestic carb cleanert NH 2 cleanert PSA), cleanert pestic carb, [61] 3.1.5 其他前处理,,,, [12], 0.45 μm, HPLC [2], T4,, T4, [62],, T4 ELISA, T4,,, LC-MS 3.2 分离和检测方法,,,,, LC-MS NMR 11-desisobutyl-11-benzylsibutramine [18] 3.2.1 薄层色谱法, ; [4,40,54,63], 3, ; 30 min 60 min [4], 225 nm - - (10:1:0.1, V:V:V), ( 60 F254), 250~2000 ng [8] - - (9:1:0.3, V:V:V),,, 1~6 mg, 190 ng 634 ng [63] [40],, (254 nm), (2 μg),, (0.4 μg) [25], 254 nm 20 cm 10 cm HPTLC, 60F254, - - (10:1:0.1, V:V:V ) 3 250~2000 ng [8] 3.2.2 液相色谱法,
5, : 1591 HPLC, [4,13,20,30,31,42,50,64] [8] MS [2,4,24,27,29,30,35,36,40,41,43,44,49,51,52-55,64,65],,,,, 200~500 nm, 219.2 nm 221.5 nm 222.7 nm ; 200 nm, 222 nm [42], HPLC-DAD,, Alltina C 18 : Ⅰ -0.02 mol/l ( 0.1% )(12:88, V:V), Ⅱ -0.02 mol/l ( 0.1% ) (60:40, V:V) 215 nm, 550 nm, 190~600 nm [50] Agilent Zorbax SB C 18 (200 mm 4.6 mm, 5 μm), 0.02 mol/l ( 0.1% )- (20:80, V:V),, 225 nm, [25] UHPLC-DAD ph 5.0, Vision HT C 18 -B(2 mm 100 mm, 1.5 μm) [13],, 225 nm [50], 275 nm [31],,,, [30] 3.2.3 毛细管电泳, [12,55] Cianchino [12] 4, 4,,, 2%,,,,,, [56] 3.2.4 离子淌度光谱法, [14,16], [14], (limit of detection, LOD) 2 ng IMS,,, 3.2.5 气相色谱法,, Parr - (gas chromatography-mass spectrometer, GC-MS) [3] 30 μg, (, 30 μg 3 ) (20 μg) 4 3.2.6 X 射线衍射 X, (coulometric electrode array, CEAD) (time-of-flight mass spectrometry, TOF-MS), X (X-ray powder diffraction, XRPD) [58] X [64] 3.2.7 酶联免疫法 (ELISA) ELISA,, ELISA,, [62] 3.2.8 核磁共振,, diffusion ordered spectroscopy (DOSY) 1 H-nuclear magnetic resonance (NMR) DOSY-COSY
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