多壁碳纳米管固相萃取—液/质联用对牛奶中残留抗生素的检测
|
摘要
四环素类抗生素以及磺胺类抗生素已经被广泛应用于预防和治疗食源性动物的疾病,然而过量地使用这些抗生素会导致其在食源性动物产品中的残留,不仅可能污染环境,严重的还可能影响到人类的身体健康,因此,建立一种快速简便的检测动物源性食品中四环素类抗生素及磺胺类抗生素多残留的方法是非常必要的。本研究采用多壁碳纳米管作为一种新型的固相萃取吸附剂自制了固相萃取柱,建立了离线固相萃取的前处理方法对牛奶样品进行前处理,并采用高效液相色谱-质谱联用技术和高效液相色谱法作为检测牛奶中四环素和磺胺类抗生素残留量的分析方法,并且应用所建立的方法对成都市市售的几种牛奶样品进行了检测。
本文以多壁碳纳米管作为固相萃取吸附剂建立了牛奶中四环素类抗生素以及磺胺类抗生素残留的固相萃取-液/质联用检测方法。四环素类抗生素的检测采用Agilent TC C18色谱柱进行色谱分离,A:甲醇:乙腈=1:3(V/V),B:0.01mol/L草酸溶液。A:B=4:6(V/V)作为流动相,流速为0.7mL/min;磺胺类抗生素的检测采用大连依利特YWG C18色谱柱进行色谱分离,0.1%甲酸的水溶液:0.1%甲酸的乙腈溶液(68∶32 V/V)作为流动相,流速为1.0mL/min。两种待测抗生素的线性范围分别为0.1～2.0μg/mL和0.05～1.0μg/mL。
本文采用液液萃取结合固相萃取作为样品前处理方法,对于牛奶样品中四环素类抗生素的检测,采用购自深圳纳米港有限公司的未经浓硝酸氧化处理的多壁碳纳米管(碳纳米管1)作为固相萃取的吸附剂进行前处理,对于磺胺类抗生素的检测,分别采用经过浓硝酸氧化前后的多壁碳纳米管作为固相萃取吸附剂进行样品前处理。
对于牛奶样品中磺胺类抗生素的检测,分别采用碳纳米管1(未经氧化处理的)和碳纳米管2(经过氧化处理的)对样品进行萃取净化,方法回收率分别为70.1%～109.8%和83.3%～110.0%,最后确定使用经过氧化处理的多壁碳纳米管作为固相萃取吸附剂进行样品前处理。该方法检出限0.3μg/L～0.9μg/L,方法精密度4.38%～10.13%,并且采用液质联用对牛奶样品中残留磺胺类抗生素进行检测,探讨了高效液相色谱以及质谱的最佳操作条件。方法检出限远低于欧盟最大残留量的要求。
对于牛奶中四环素类抗生素的检测,本文建立的多壁碳纳米管作为固相萃取的前处理方法回收率在94.4%～101.2%之间,方法检出限0.05mg/L,方法精密度为1.9%～5.0%,并且采用高效液相色谱对牛奶样品中残留的四环素类抗生素进行检测,探讨了高效液相色谱的最佳操作条件。
本方法精确可靠,灵敏度高,适用于牛奶中四环素及磺胺类抗生素的定量和确认分析。另外,本研究所建立的离线前处理方法与在线仪器相比虽然较为耗时,但是仍然具有一定的实用价值。
Tetracycline antibiotics and sulfa antibiotics has been widely used in the prevention and treatment of food-borne animal diseases, but excessive use of these antibiotics will result in food-borne residues in animal products, may not only pollute the environment, serious Also likely to affect human health, therefore, the establishment of a quick and easy way to detect animal-derived food in the tetracycline class antibiotics and sulfa antibiotic residues in many ways is very necessary. This study used multi-walled carbon nanotubes as a new type of solid-phase extraction adsorbent to make a solid phase extraction columns, a solid-phase extraction of offline pre-treatment methods on milk samples before processing and use of high-performance liquid color Spectrum-using mass spectrometry technology and high-performance liquid chromatography as a test of milk in the antibiotics tetracycline and sulfonamides residues in the analysis, and application of the method established by the Chengdu Commercial Several milk samples Were detected.
In this paper, a solid-phase extraction-liquid/mass spectrometry detection method which multi-walled carbon nanotubes was used as a solid-phase extraction adsorbent to detect tetracycline antibiotics and sulfa antibiotic residues in milk. Agilent TC C18 column chromatography was used to detection tetracycline antibiotics in milk, A:methanol:acetonitrile=1:3(V/V), B:0.01mol/L oxalic acid solution. A:B=4:6 (V/V) as flow phase; flow rate was 0.7 mL/min; sulfa antibiotics detected by Dalian Gbadolite YWG C18 column for chromatography, flow phase:0.1% formic acid solution: 0.1% formic acid solution of acetonitrile (68:32 V/V); flow rate was 1.0 mL/min. The linear range of two kind of antibiotics under test were 0.1-2.0μg/mL and 0.05-1.0μg/mL.
In this paper, liquid-liquid extraction and solid-phase extraction were used as a sample pre-treatment methods, the milk samples, nano-purchased from Shenzhen Co., Ltd. of Hong Kong without a concentrated nitric acid oxidation of the multi-walled carbon nanotubes ( Carbon Nanotubes 1) were used for solid-phase extraction in the detection of tetracycline antibiotics in milk samples, In sulfa antibiotics testing, multi-walled carbon nanotubes before and after the concentrated nitric acid oxidation were used as a solid-phase extraction absorbent sample pre-treatment.
The milk samples sulfa antibiotics testing, were used carbon nanotubes 1 (without the oxidation process) and carbon nanotubes 2 (after the oxidation process) on the sample extraction purification, recoveries were 70.1%-109.8% and 83.3% -110.0%, after the finalization of the use of multi-walled carbon nanotubes with a solid-phase extraction absorbent sample pre-treatment. The method detection limit of 0.3μg/L-0.9μg/L, the precision of the method was 4.38%-10.13%, and the sulfa antibiotic residues in milk samples were detected with a method of high-performance liquid chromatography and MS and the best operating conditions was discussed. The detection limits was well below the EU maximum residue requirements.
For determination of tetracycline antibiotics in milk, the recovery of the method established in this paper which multi-walled carbon nanotubes was used as a solid-phase extraction absorbent was 94.4%-101.2% and the detection limit was 0.05 mg/L, he precision of the method was 1.9%-5.0%, and high-performance liquid chromatography was used to detect the tetracycline antibiotic residues in milk samples, a high-performance liquid chromatography of the best operating conditions was discussed.
The detection of tetracycline and sulfa antibiotics in several milk samples sold in Chengdu was determined by the method of multi-walled carbon nanotubes SPE-LC/MS which was established in this research.
本文以多壁碳纳米管作为固相萃取吸附剂建立了牛奶中四环素类抗生素以及磺胺类抗生素残留的固相萃取-液/质联用检测方法。四环素类抗生素的检测采用Agilent TC C18色谱柱进行色谱分离,A:甲醇:乙腈=1:3(V/V),B:0.01mol/L草酸溶液。A:B=4:6(V/V)作为流动相,流速为0.7mL/min;磺胺类抗生素的检测采用大连依利特YWG C18色谱柱进行色谱分离,0.1%甲酸的水溶液:0.1%甲酸的乙腈溶液(68∶32 V/V)作为流动相,流速为1.0mL/min。两种待测抗生素的线性范围分别为0.1～2.0μg/mL和0.05～1.0μg/mL。
本文采用液液萃取结合固相萃取作为样品前处理方法,对于牛奶样品中四环素类抗生素的检测,采用购自深圳纳米港有限公司的未经浓硝酸氧化处理的多壁碳纳米管(碳纳米管1)作为固相萃取的吸附剂进行前处理,对于磺胺类抗生素的检测,分别采用经过浓硝酸氧化前后的多壁碳纳米管作为固相萃取吸附剂进行样品前处理。
对于牛奶样品中磺胺类抗生素的检测,分别采用碳纳米管1(未经氧化处理的)和碳纳米管2(经过氧化处理的)对样品进行萃取净化,方法回收率分别为70.1%～109.8%和83.3%～110.0%,最后确定使用经过氧化处理的多壁碳纳米管作为固相萃取吸附剂进行样品前处理。该方法检出限0.3μg/L～0.9μg/L,方法精密度4.38%～10.13%,并且采用液质联用对牛奶样品中残留磺胺类抗生素进行检测,探讨了高效液相色谱以及质谱的最佳操作条件。方法检出限远低于欧盟最大残留量的要求。
对于牛奶中四环素类抗生素的检测,本文建立的多壁碳纳米管作为固相萃取的前处理方法回收率在94.4%～101.2%之间,方法检出限0.05mg/L,方法精密度为1.9%～5.0%,并且采用高效液相色谱对牛奶样品中残留的四环素类抗生素进行检测,探讨了高效液相色谱的最佳操作条件。
本方法精确可靠,灵敏度高,适用于牛奶中四环素及磺胺类抗生素的定量和确认分析。另外,本研究所建立的离线前处理方法与在线仪器相比虽然较为耗时,但是仍然具有一定的实用价值。
Tetracycline antibiotics and sulfa antibiotics has been widely used in the prevention and treatment of food-borne animal diseases, but excessive use of these antibiotics will result in food-borne residues in animal products, may not only pollute the environment, serious Also likely to affect human health, therefore, the establishment of a quick and easy way to detect animal-derived food in the tetracycline class antibiotics and sulfa antibiotic residues in many ways is very necessary. This study used multi-walled carbon nanotubes as a new type of solid-phase extraction adsorbent to make a solid phase extraction columns, a solid-phase extraction of offline pre-treatment methods on milk samples before processing and use of high-performance liquid color Spectrum-using mass spectrometry technology and high-performance liquid chromatography as a test of milk in the antibiotics tetracycline and sulfonamides residues in the analysis, and application of the method established by the Chengdu Commercial Several milk samples Were detected.
In this paper, a solid-phase extraction-liquid/mass spectrometry detection method which multi-walled carbon nanotubes was used as a solid-phase extraction adsorbent to detect tetracycline antibiotics and sulfa antibiotic residues in milk. Agilent TC C18 column chromatography was used to detection tetracycline antibiotics in milk, A:methanol:acetonitrile=1:3(V/V), B:0.01mol/L oxalic acid solution. A:B=4:6 (V/V) as flow phase; flow rate was 0.7 mL/min; sulfa antibiotics detected by Dalian Gbadolite YWG C18 column for chromatography, flow phase:0.1% formic acid solution: 0.1% formic acid solution of acetonitrile (68:32 V/V); flow rate was 1.0 mL/min. The linear range of two kind of antibiotics under test were 0.1-2.0μg/mL and 0.05-1.0μg/mL.
In this paper, liquid-liquid extraction and solid-phase extraction were used as a sample pre-treatment methods, the milk samples, nano-purchased from Shenzhen Co., Ltd. of Hong Kong without a concentrated nitric acid oxidation of the multi-walled carbon nanotubes ( Carbon Nanotubes 1) were used for solid-phase extraction in the detection of tetracycline antibiotics in milk samples, In sulfa antibiotics testing, multi-walled carbon nanotubes before and after the concentrated nitric acid oxidation were used as a solid-phase extraction absorbent sample pre-treatment.
The milk samples sulfa antibiotics testing, were used carbon nanotubes 1 (without the oxidation process) and carbon nanotubes 2 (after the oxidation process) on the sample extraction purification, recoveries were 70.1%-109.8% and 83.3% -110.0%, after the finalization of the use of multi-walled carbon nanotubes with a solid-phase extraction absorbent sample pre-treatment. The method detection limit of 0.3μg/L-0.9μg/L, the precision of the method was 4.38%-10.13%, and the sulfa antibiotic residues in milk samples were detected with a method of high-performance liquid chromatography and MS and the best operating conditions was discussed. The detection limits was well below the EU maximum residue requirements.
For determination of tetracycline antibiotics in milk, the recovery of the method established in this paper which multi-walled carbon nanotubes was used as a solid-phase extraction absorbent was 94.4%-101.2% and the detection limit was 0.05 mg/L, he precision of the method was 1.9%-5.0%, and high-performance liquid chromatography was used to detect the tetracycline antibiotic residues in milk samples, a high-performance liquid chromatography of the best operating conditions was discussed.
The detection of tetracycline and sulfa antibiotics in several milk samples sold in Chengdu was determined by the method of multi-walled carbon nanotubes SPE-LC/MS which was established in this research.
引文
[1]A.Gentili,D.Perret,S.Marchese,et al.Liquid chromatography-tandem mass spectrometry for performing confirmatory analysis of veterinary drugs in animal-food products[J].Trend in analytical chemistry,2005,24(7):704-733.
[2]Yi Wen,Ying Wang,Yu-Qi Feng,et al.Simultaneous residue monitoring of four tetracycline antibiotics in fish muscle by in-tube solid-phase microextraction coupled with high-performance liquid chromatography[J].Talanta,2006,70:153-159.
[3]Commission Regulation no.2377/90,Off.J.Eur.Commun.,18 August 1990,no.L224.
[4]The maximum residue limit of veterinary drugs in edible animal food established by Ministry of Agriculture of People's Republic of China,Chin.J.Vet.Drug 37(2003)15.
[5]Guo-Zhen Fang,Jin-Xing He,Shuo Wang,et al.Multiwalled carbon nanotubes as sorbent for on-line coupling of solid-phase extraction to high-performance liquid chromatography for simultaneous determination of 10 sulfonamides in eggs and pork[J],Journal of Chromatography A,2006,1127:12-17.
[6]B.Shao,D.Dan,Y.N.Wu,J.Y.Hu,et al.Simultaneous determination of 17 sulfonamide residues in porcine meat,kidney and liver by solid-phase extraction and liquid chromatography-tandem mass spectrometry[J].Anal.Chim.Acta,2005,546:174.
[7]鲁晓翠,候玉泽,邓瑞广,等.磺胺类药物在动物性食品中的残留与检测[J].动物医学进展,2007,28(2):70-74.
[8]董丹.液相色谱-质谱/质谱测定动物源性食品和水中17种磺胺[D].东北大学理学院,2005:5-10.
[9]L.Verzegnassi,M.-C.Savoy-Perroud,R.H.Stadler,et al.Application of liquid chromatography-electrospray ionization tandem mass spectrometry to the detection of 10sulfonamidesin honey.[J]Journal of Chromatography A,2002,977:77-87.
[10]Nancy T.Malintan,Mustafa Ali Mohd.Determination of sulfonamides in selected Malaysian swine wastewater by high-performance liquid chromatography[J].Journal of Chromatography A,2006,1127:154-160.
[11]沈永聪,李守军,杨林,等.牛奶中抗生素残留检测技术进展[J].食品科学,2006:87-88.
[12]陆勤,林蜂,朱柳明,等.牛奶中磺胺类抗生素的快速检测分析[J].乳品加工报,2006,8(11):51-53.
[13]汤丽芬,张选红.反向液相色谱法同时测定广州部分地区肉类4种抗生素的残留[J].中国卫生检验杂志,2003,14(3):270-271.
[14]刘清,刘军.鲜牛奶中磺胺类兽药残留检测调查[J].职业与卫生,2003,19(9):41-42.
[15]侯为道,傅小鲁.动物性食品中兽药残留水平及膳食安全性评价[J].现代预防医学,2004,31(1):47-49.
[16]李翠枝,刘艳辉,郭军,等.抗生素和其他兽药残留的危害[J].中国乳品工业,2004,32(10):17-22.
[17]徐士新.食品法典工作法规[M].北京:中国农业科学技术出版社,2004,169.
[18]丁志刚,王静,高红梅,等.抗生素残留检测技术的研究进展[J].食品与发酵工业,2005,31(6):112-115.
[19]Kroner K.H,Hustedt H.New techniques for Solid-Liquid Separation in enzyme recovery-aqueous two-Phase extraction and cross-floe filtration[J].Royal Flemish Soc of Engineers,1986,2:1021-1033.
[20]苏仲毅,陈猛,袁东星,等.固相萃取-超高压液相色谱-串联质谱法分析海水中9种磺胺类抗生素[J].厦门大学学报(自然科学版),2007,46(增刊1):72-76.
[21]谭建华,唐才明,余以义,等.高效液相色谱法同时分析城市河水中的多种抗生素[J].色谱,2007,25(4):546-549.
[22]刘虹,张国平,刘丛强,等.固相萃取-色谱测定水、沉积物及士壤中氯霉素和3种四环素类抗生素[J].分析化学,2007,35(3):315-319.
[23]徐锦忠,吴斌,丁涛,等.高效液相色谱-电喷雾串联质谱法测定蜂蜜中的林可胺类抗生素残留[J].色谱,2006,24(4):436-439.
[24]刘玉春,徐维海,余莉莉,等.固相萃取液相色谱-兽约质谱/质谱联用测定河水中大环内酯类抗生素[J].分析测试学报,2006,25(2):1-5.
[25]贾秀红.碳纳米管吸附性能的研究进展[J].炭素技术,2004,23(3):25-30.
[26]韩宝武,范必威.固相萃取-高效液相色谱法同时检测牛奶中四环素类抗生素残留[J].广州化工,2007,5:39-40.
[27]Cai Y Q,Jiang G B,Liu J F,et al.Multi-walled carbon nanotubes packed cartridge for the solid-phase extraction of several phthalate esters from water samples and their determination by high performance liquid chromatography[J].Anal.Chim.Acta,2003,494:149-156.
[28]Cai Y Q,Cai Y E,Mou S F,et al.Multi-walled carbon nanotubes as a solid-phase extraction adsorbent for the determination of chlorophenols in environmental water samples [J].J.Chromatogr.A,2005,1081:245-247.
[29]Arthur C,Pawliszyn J.Solid phase microextraction with thermal desorption using fused silica optical fibers[J].Anal Chem,1990,62:2145-2148.
[30]McClure,Evelyn L.Wong,Charles S,et al.Solid phase microextraction of macrolide,trimethoprim,and sulfonamide antibiotics in wastewaters[J].Journal of Chromatography A, 2007,1169(1/2):53-62.
[31]Barker S.A.Long A.R.Short C.R.Isolation of drug residues from tissues by solid phase dispersion[J].Journal of Chromatography A,1989,475(1):353-361.
[32]Barker,S.A.Matrix solid-phase dispersion[J].Journal of Chromatography A,2000,885(1):115-127.
[33]Barker S.A.Applications of matrix solid-phase dispersion in food analysis[J].Journal of Chromatography A,2000,880:63-68.
[34]耿志明,李鹏,陈明,等.基质固相分散-高效液相色谱法测定鱼肉中磺胺类药物残留[J].江苏农业学报,2006,22(3):310-312.
[35]罗瑞峰,马小宁.柱后衍生高效液相色谱法测定猪肉中的链霉素残留[J].化学分析计量,2006,15(3):22-24.
[36]郑屏,盛旋,余晓峰,等.基质固相分散液相色谱法检测辣椒产品中的黄曲霉毒素[J].色谱,2006,24(1):62-64.
[37]Burgos-Sol6rzano,G.I.Brennecke,J.F.Stadtherr,M.A,et al.Solubility measurements and modeling of molecules of biological and pharmaceutical interest with supercritical CO_2[J].Fluid Phase Equilibria,2004,220(1):55-67.
[38]Ganzler K,Salgo A,Valko K.J,et al.Microwave extraction:A novel sample preparation method for chromatography[J].Journal of Chromatography A,1986,371:299-306.
[39]刘靖靖,林黎明,江志刚,等.高效液相色谱法同时检测8种喹诺酮类兽药残留量[J]1分析试验室,2007,26(8):5-9.
[40]Ridgway K,Thorpe EE.Handbook of solvent extraction.[M].New York:Wiley-Interscience,1983:583.
[41]VErrail MS.Science and practice of liquid-liquid extraction.Vol.2.[M].Oxford:Science Rublications,1992:194.
[42]平言,冯闻铮,苗勇,等.螺旋霉素发酵滤液提取过程工艺研究[J].清华大学学报(自然科学版),1997,37(12):64.
[43]刘宏程,黎其万,佴注,等.HPLC测定动物组织中己烯雌酚、呋喃唑酮、磺胺类药物残留[J].化学通报,2006,1:66-69.
[44]方国凯.动物源性食品中痕量磺胺兽药残留的分析[J].食品研究与开发,2007,28(5):101-104.
[45]李孟玻,张德云,彭之见,等.高效液相色谱法测定鱼肉中残留磺胺类药物[J].理化检验-化学分册,2006,42(8):611-61.
[46]汤瑶,何华,吴斌,等.固相萃取-HPLC法测定蜂蜜中残留的10种磺胺类药物[J].分析测试学报,2005,24(1):96-99.
[47]王绍云,周光明,王莉,等.反相高效液相色谱法测定肝组织中土霉素、四环素残留量[J].西安师范大学学报(自然科学版),2005,30(6):1079-1081.
[48]蔡颖,韩奕奕,何志军,等.反相高效液相色谱法测定乳制品中土霉素、四环素和金霉素残留量[J].化学世界,2006,(7):398-400.
[49]秦燕,陈毓芳,林峰等.固相萃取-高效液相色谱法同时测定牛奶中多种四环素残留[J].食品科学,2005,26(3):202-204.
[50]Pilaf Vinas,Nuria Balsalobre,Carmen Lopez-Erroz,et al.Liquid chromatography with ultraviolet absorbance detection for the analysis of tetracycline residues in honey[J].J.Chromatogr.A,2004,1022:125-129.
[51]刘艳华,张纯萍,门立强,等.液相色谱-串联质谱法测定鸡肌肉组织中的四环素类约物残留[J].色谱,2006,24(2):171-173.
[52]岳振峰,邱月明,林秀云,等.高效液相色谱串联质谱法测定牛奶中四环素类抗生素及其代谢产物[J].分析化学研究报告,2006,34(9):1255-1259.
[53]Marc Cherlet,Siska Croubels,Patrick De Backer,et al.Quantitative determination of chlortetracycline content in animal plasma atcontrolled keto-enol tautomerism by liquid chromatography-electrospray Ionization-tandem mass spectrometry[J].Journal of Chromatography A,2006,l l02:116-124.
[54]Marc Cherlet,Mario Schelkens,Siska Croubels,et al.Quantitative multi-residue analysis of tetracyclines and their4-epimers in pig tissues by high-performance liquid chromatography combined with positive-ion electrospray ionization mass spectrometry[J].Analytica Chimica Acta,2003,492:199-213.
[55]秦燕,张美金,林海丹,等.高效液相色谱-电喷雾串联质谱法测定动物饲料中的10种磺胺[J].色谱,2005,23(4):397-400.
[56]庞国芳,曹彦忠,张进杰,等.液相色谱.串联质谱同时测定家禽组织中16种磺胺残留[J].分析化学研究报告,2005,33(9):1252-1256.
[57]Thomas S.Thompson,Donald K.Noot,et al.Determination of sulfonamides in honey by liquid chromatography-tandem mass spectrometry[J].Analytica Chimica Acta,2005,551:168-176.
[58]L.Verzegnassi,M.-C.Savoy-Perroud,R.H.Stadler,et al.Application of liquid chromatography-electrospray ionization tandem mass spectrometry to the detection of 10sulfonamides in honey[J].Journal of Chromatography A,2002,977:77-87.
[59]陈丽霞,马占峰,孙燕,等.水产品的药物残留及其检测[J].食品质量安全与检测,2007.9:20-21.
[60]邢晓平,等.毛细管电泳-电化学检测法测定鸡蛋中残留四环素类抗生素[J].食品科 学,2007,28(10):470-473.
[61]何金环,王一凡,等.TTC和ELISA法检测纯牛奶中抗菌药物残留比较[J].安徽农业科学,2007,35(9):2576-2577.
[62]韩道丽,赵元黎,朱双美,等.浓硝酸处理碳纳米管对4-硝基苯酚的吸附性能研究[J].光散射学报,2006,18(4):319-322.
[63]李孟玻,张德云,彭之见,等.高效液相色谱法测定鱼肉中残留磺胺类药物[J].理化检验-化学分册,2006,42(8):611-613.
[64]程雪梅.色谱分析样品前处理技术--固相萃取法[J].热带农业工程,2002,(1):14-16.
[65]孙文秀,黄智鹏,张鹭,等.浓硝酸处理前后多壁碳纳米管的荧光特性研究[J].光谱学与光谱分析,2005,25(1):10-12.
[2]Yi Wen,Ying Wang,Yu-Qi Feng,et al.Simultaneous residue monitoring of four tetracycline antibiotics in fish muscle by in-tube solid-phase microextraction coupled with high-performance liquid chromatography[J].Talanta,2006,70:153-159.
[3]Commission Regulation no.2377/90,Off.J.Eur.Commun.,18 August 1990,no.L224.
[4]The maximum residue limit of veterinary drugs in edible animal food established by Ministry of Agriculture of People's Republic of China,Chin.J.Vet.Drug 37(2003)15.
[5]Guo-Zhen Fang,Jin-Xing He,Shuo Wang,et al.Multiwalled carbon nanotubes as sorbent for on-line coupling of solid-phase extraction to high-performance liquid chromatography for simultaneous determination of 10 sulfonamides in eggs and pork[J],Journal of Chromatography A,2006,1127:12-17.
[6]B.Shao,D.Dan,Y.N.Wu,J.Y.Hu,et al.Simultaneous determination of 17 sulfonamide residues in porcine meat,kidney and liver by solid-phase extraction and liquid chromatography-tandem mass spectrometry[J].Anal.Chim.Acta,2005,546:174.
[7]鲁晓翠,候玉泽,邓瑞广,等.磺胺类药物在动物性食品中的残留与检测[J].动物医学进展,2007,28(2):70-74.
[8]董丹.液相色谱-质谱/质谱测定动物源性食品和水中17种磺胺[D].东北大学理学院,2005:5-10.
[9]L.Verzegnassi,M.-C.Savoy-Perroud,R.H.Stadler,et al.Application of liquid chromatography-electrospray ionization tandem mass spectrometry to the detection of 10sulfonamidesin honey.[J]Journal of Chromatography A,2002,977:77-87.
[10]Nancy T.Malintan,Mustafa Ali Mohd.Determination of sulfonamides in selected Malaysian swine wastewater by high-performance liquid chromatography[J].Journal of Chromatography A,2006,1127:154-160.
[11]沈永聪,李守军,杨林,等.牛奶中抗生素残留检测技术进展[J].食品科学,2006:87-88.
[12]陆勤,林蜂,朱柳明,等.牛奶中磺胺类抗生素的快速检测分析[J].乳品加工报,2006,8(11):51-53.
[13]汤丽芬,张选红.反向液相色谱法同时测定广州部分地区肉类4种抗生素的残留[J].中国卫生检验杂志,2003,14(3):270-271.
[14]刘清,刘军.鲜牛奶中磺胺类兽药残留检测调查[J].职业与卫生,2003,19(9):41-42.
[15]侯为道,傅小鲁.动物性食品中兽药残留水平及膳食安全性评价[J].现代预防医学,2004,31(1):47-49.
[16]李翠枝,刘艳辉,郭军,等.抗生素和其他兽药残留的危害[J].中国乳品工业,2004,32(10):17-22.
[17]徐士新.食品法典工作法规[M].北京:中国农业科学技术出版社,2004,169.
[18]丁志刚,王静,高红梅,等.抗生素残留检测技术的研究进展[J].食品与发酵工业,2005,31(6):112-115.
[19]Kroner K.H,Hustedt H.New techniques for Solid-Liquid Separation in enzyme recovery-aqueous two-Phase extraction and cross-floe filtration[J].Royal Flemish Soc of Engineers,1986,2:1021-1033.
[20]苏仲毅,陈猛,袁东星,等.固相萃取-超高压液相色谱-串联质谱法分析海水中9种磺胺类抗生素[J].厦门大学学报(自然科学版),2007,46(增刊1):72-76.
[21]谭建华,唐才明,余以义,等.高效液相色谱法同时分析城市河水中的多种抗生素[J].色谱,2007,25(4):546-549.
[22]刘虹,张国平,刘丛强,等.固相萃取-色谱测定水、沉积物及士壤中氯霉素和3种四环素类抗生素[J].分析化学,2007,35(3):315-319.
[23]徐锦忠,吴斌,丁涛,等.高效液相色谱-电喷雾串联质谱法测定蜂蜜中的林可胺类抗生素残留[J].色谱,2006,24(4):436-439.
[24]刘玉春,徐维海,余莉莉,等.固相萃取液相色谱-兽约质谱/质谱联用测定河水中大环内酯类抗生素[J].分析测试学报,2006,25(2):1-5.
[25]贾秀红.碳纳米管吸附性能的研究进展[J].炭素技术,2004,23(3):25-30.
[26]韩宝武,范必威.固相萃取-高效液相色谱法同时检测牛奶中四环素类抗生素残留[J].广州化工,2007,5:39-40.
[27]Cai Y Q,Jiang G B,Liu J F,et al.Multi-walled carbon nanotubes packed cartridge for the solid-phase extraction of several phthalate esters from water samples and their determination by high performance liquid chromatography[J].Anal.Chim.Acta,2003,494:149-156.
[28]Cai Y Q,Cai Y E,Mou S F,et al.Multi-walled carbon nanotubes as a solid-phase extraction adsorbent for the determination of chlorophenols in environmental water samples [J].J.Chromatogr.A,2005,1081:245-247.
[29]Arthur C,Pawliszyn J.Solid phase microextraction with thermal desorption using fused silica optical fibers[J].Anal Chem,1990,62:2145-2148.
[30]McClure,Evelyn L.Wong,Charles S,et al.Solid phase microextraction of macrolide,trimethoprim,and sulfonamide antibiotics in wastewaters[J].Journal of Chromatography A, 2007,1169(1/2):53-62.
[31]Barker S.A.Long A.R.Short C.R.Isolation of drug residues from tissues by solid phase dispersion[J].Journal of Chromatography A,1989,475(1):353-361.
[32]Barker,S.A.Matrix solid-phase dispersion[J].Journal of Chromatography A,2000,885(1):115-127.
[33]Barker S.A.Applications of matrix solid-phase dispersion in food analysis[J].Journal of Chromatography A,2000,880:63-68.
[34]耿志明,李鹏,陈明,等.基质固相分散-高效液相色谱法测定鱼肉中磺胺类药物残留[J].江苏农业学报,2006,22(3):310-312.
[35]罗瑞峰,马小宁.柱后衍生高效液相色谱法测定猪肉中的链霉素残留[J].化学分析计量,2006,15(3):22-24.
[36]郑屏,盛旋,余晓峰,等.基质固相分散液相色谱法检测辣椒产品中的黄曲霉毒素[J].色谱,2006,24(1):62-64.
[37]Burgos-Sol6rzano,G.I.Brennecke,J.F.Stadtherr,M.A,et al.Solubility measurements and modeling of molecules of biological and pharmaceutical interest with supercritical CO_2[J].Fluid Phase Equilibria,2004,220(1):55-67.
[38]Ganzler K,Salgo A,Valko K.J,et al.Microwave extraction:A novel sample preparation method for chromatography[J].Journal of Chromatography A,1986,371:299-306.
[39]刘靖靖,林黎明,江志刚,等.高效液相色谱法同时检测8种喹诺酮类兽药残留量[J]1分析试验室,2007,26(8):5-9.
[40]Ridgway K,Thorpe EE.Handbook of solvent extraction.[M].New York:Wiley-Interscience,1983:583.
[41]VErrail MS.Science and practice of liquid-liquid extraction.Vol.2.[M].Oxford:Science Rublications,1992:194.
[42]平言,冯闻铮,苗勇,等.螺旋霉素发酵滤液提取过程工艺研究[J].清华大学学报(自然科学版),1997,37(12):64.
[43]刘宏程,黎其万,佴注,等.HPLC测定动物组织中己烯雌酚、呋喃唑酮、磺胺类药物残留[J].化学通报,2006,1:66-69.
[44]方国凯.动物源性食品中痕量磺胺兽药残留的分析[J].食品研究与开发,2007,28(5):101-104.
[45]李孟玻,张德云,彭之见,等.高效液相色谱法测定鱼肉中残留磺胺类药物[J].理化检验-化学分册,2006,42(8):611-61.
[46]汤瑶,何华,吴斌,等.固相萃取-HPLC法测定蜂蜜中残留的10种磺胺类药物[J].分析测试学报,2005,24(1):96-99.
[47]王绍云,周光明,王莉,等.反相高效液相色谱法测定肝组织中土霉素、四环素残留量[J].西安师范大学学报(自然科学版),2005,30(6):1079-1081.
[48]蔡颖,韩奕奕,何志军,等.反相高效液相色谱法测定乳制品中土霉素、四环素和金霉素残留量[J].化学世界,2006,(7):398-400.
[49]秦燕,陈毓芳,林峰等.固相萃取-高效液相色谱法同时测定牛奶中多种四环素残留[J].食品科学,2005,26(3):202-204.
[50]Pilaf Vinas,Nuria Balsalobre,Carmen Lopez-Erroz,et al.Liquid chromatography with ultraviolet absorbance detection for the analysis of tetracycline residues in honey[J].J.Chromatogr.A,2004,1022:125-129.
[51]刘艳华,张纯萍,门立强,等.液相色谱-串联质谱法测定鸡肌肉组织中的四环素类约物残留[J].色谱,2006,24(2):171-173.
[52]岳振峰,邱月明,林秀云,等.高效液相色谱串联质谱法测定牛奶中四环素类抗生素及其代谢产物[J].分析化学研究报告,2006,34(9):1255-1259.
[53]Marc Cherlet,Siska Croubels,Patrick De Backer,et al.Quantitative determination of chlortetracycline content in animal plasma atcontrolled keto-enol tautomerism by liquid chromatography-electrospray Ionization-tandem mass spectrometry[J].Journal of Chromatography A,2006,l l02:116-124.
[54]Marc Cherlet,Mario Schelkens,Siska Croubels,et al.Quantitative multi-residue analysis of tetracyclines and their4-epimers in pig tissues by high-performance liquid chromatography combined with positive-ion electrospray ionization mass spectrometry[J].Analytica Chimica Acta,2003,492:199-213.
[55]秦燕,张美金,林海丹,等.高效液相色谱-电喷雾串联质谱法测定动物饲料中的10种磺胺[J].色谱,2005,23(4):397-400.
[56]庞国芳,曹彦忠,张进杰,等.液相色谱.串联质谱同时测定家禽组织中16种磺胺残留[J].分析化学研究报告,2005,33(9):1252-1256.
[57]Thomas S.Thompson,Donald K.Noot,et al.Determination of sulfonamides in honey by liquid chromatography-tandem mass spectrometry[J].Analytica Chimica Acta,2005,551:168-176.
[58]L.Verzegnassi,M.-C.Savoy-Perroud,R.H.Stadler,et al.Application of liquid chromatography-electrospray ionization tandem mass spectrometry to the detection of 10sulfonamides in honey[J].Journal of Chromatography A,2002,977:77-87.
[59]陈丽霞,马占峰,孙燕,等.水产品的药物残留及其检测[J].食品质量安全与检测,2007.9:20-21.
[60]邢晓平,等.毛细管电泳-电化学检测法测定鸡蛋中残留四环素类抗生素[J].食品科 学,2007,28(10):470-473.
[61]何金环,王一凡,等.TTC和ELISA法检测纯牛奶中抗菌药物残留比较[J].安徽农业科学,2007,35(9):2576-2577.
[62]韩道丽,赵元黎,朱双美,等.浓硝酸处理碳纳米管对4-硝基苯酚的吸附性能研究[J].光散射学报,2006,18(4):319-322.
[63]李孟玻,张德云,彭之见,等.高效液相色谱法测定鱼肉中残留磺胺类药物[J].理化检验-化学分册,2006,42(8):611-613.
[64]程雪梅.色谱分析样品前处理技术--固相萃取法[J].热带农业工程,2002,(1):14-16.
[65]孙文秀,黄智鹏,张鹭,等.浓硝酸处理前后多壁碳纳米管的荧光特性研究[J].光谱学与光谱分析,2005,25(1):10-12.