中空纤维膜液相微萃取-毛细管电泳法测定环境水样中的4种磺胺类药物
|
摘要
水样以3 000r·min-1速率离心10min后取上清液,依次用0.45,0.22μm滤膜过滤。加入KH2PO4调节滤液酸度至pH 4.5后,采用中空纤维膜液相微萃取-毛细管电泳法测定其中的4种磺胺类药物。最佳萃取条件为:萃取剂为正辛醇,接受相为24μL的150mmol·L-1 NaOH溶液,给出相为18mL的样品溶液(pH 4.5),搅拌速率为300r·min-1,萃取时间为60min。毛细管电泳运行电压为20kV;在3.447kPa压力下进样5s;负极端检测,检测波长为254nm;温度为25℃;缓冲溶液为30 mmol·L-1四硼酸钠溶液(pH 7.60)。4种磺胺类药物的质量浓度均在5.0~1 000μg·L~(-1)内与对应的峰面积呈线性关系,磺胺二甲基嘧啶、磺胺甲基嘧啶、磺胺嘧啶和磺胺甲恶唑的检出限(3S/N)依次为1.17,0.84,0.73,1.27μg·L~(-1),富集倍数在105~393之间。方法用于环境水样中4种磺胺类药物的测定,水产养殖用水和生活污水中分别检出了2,1种磺胺。加标回收率在82.3%~99.4%,测定值的相对标准偏差(n=5)为0.39%~6.6%。
Water sample was centrifuged for 10 min at a rate of 3 000 r·min-1,and the supernatant was taken and filtered surcessively through filters of 0.45 and 0.22μm.Acidity of the filtrate was adjusted to pH 4.5 by addition of KH2 PO4.The 4 sulfonamides in the filtrate were separated by hollow fiber membrane liquid phase microextraction under the following conditions:(1) extractant:n-octanol;(2)acceptor phase:24μL of 150 mmol·L-1 NaOH solution;(3) donor phase:18 mL of pH 4.5 sample solution;(4)time of extraction:60 min;(5) stirring rate during extraction:300 r·min-1,and determined by capillary electrophoresis under the following conditions:(1) operating voltage:20 kV;(2)time and pressure of sample introduction:5 s,3.447 kPa;(3) detection on cathodic side at the wavelength of 254 nm and temperature of 25℃;(4) buffer solution:30 mmol·L-1 borax solution of pH7.60.Linear relationships between values of peak area and mass concentration of the 4 sulfonamides were found in the same range of 5.0 to 1 000μg·L~(-1),with detection limits(3 S/N)of 1.17(SM2),0.84(SM1),0.73(SD)and 1.27μg·L~(-1)(SMZ),and enrichment factors between 105 and 393.In analysis of substantial samples by the proposed method,2 sulfonamides were detected in aquaculture water and 1 sulfonamide was detected in domestic sewage.Values of recovery obtained by standard addition method were in the range of 82.3%to 99.4%,and RSDs(n=5)were in the range of 0.39%-6.6%.
Water sample was centrifuged for 10 min at a rate of 3 000 r·min-1,and the supernatant was taken and filtered surcessively through filters of 0.45 and 0.22μm.Acidity of the filtrate was adjusted to pH 4.5 by addition of KH2 PO4.The 4 sulfonamides in the filtrate were separated by hollow fiber membrane liquid phase microextraction under the following conditions:(1) extractant:n-octanol;(2)acceptor phase:24μL of 150 mmol·L-1 NaOH solution;(3) donor phase:18 mL of pH 4.5 sample solution;(4)time of extraction:60 min;(5) stirring rate during extraction:300 r·min-1,and determined by capillary electrophoresis under the following conditions:(1) operating voltage:20 kV;(2)time and pressure of sample introduction:5 s,3.447 kPa;(3) detection on cathodic side at the wavelength of 254 nm and temperature of 25℃;(4) buffer solution:30 mmol·L-1 borax solution of pH7.60.Linear relationships between values of peak area and mass concentration of the 4 sulfonamides were found in the same range of 5.0 to 1 000μg·L~(-1),with detection limits(3 S/N)of 1.17(SM2),0.84(SM1),0.73(SD)and 1.27μg·L~(-1)(SMZ),and enrichment factors between 105 and 393.In analysis of substantial samples by the proposed method,2 sulfonamides were detected in aquaculture water and 1 sulfonamide was detected in domestic sewage.Values of recovery obtained by standard addition method were in the range of 82.3%to 99.4%,and RSDs(n=5)were in the range of 0.39%-6.6%.
引文
[1]HIBA A,CARINE A,HAIFA A R,et al.Monitoring of twenty-two sulfonamides in edible tissues:Investigation of new metabolites and their potential toxicity[J].Food Chemistry,2016,192(1):212-227.
[2]HE X,DENG M,WANG Q,et al.Residues and health risk assessment of quinolones and sulfonamides in cultured fish from Pearl River Delta,China[J].Aquaculture,2016,458(1):38-46.
[3]WISE R.Antimicrobial resistance:Priorities for action[J].Journal of Antimicrobial Chemotherapy,2002,49(4):585-586.
[4]洪蕾洁,石璐,张亚雷,等.固相萃取-高效液相色谱法同时测定水体中的10种磺胺类抗生素[J].环境科学,2012,33(2):652-657.
[5]HERRERA-HERRERA A V,HERNNDEZBORGES J,BORGESMIQUEL T M,et al.Dispersive liquidliquid microextraction combined with ultra-high performance liquid chromatography for the simultaneous determination of 25sulfonamide and quinolone antibiotics in water samples[J].Journal of Pharmaceutical and Biomedical Analysis,2013,75(5):130-137.
[6]WULF N R,MATUSZEWSKI K A.Sulfonamide cross-reactivity:Is there evidence to support broad cross-allergenicity?[J].American Journal of HealthSystem Pharmacy,2013,70(17):1483-1483.
[7]ASSASSI N,TAZEROUTI A,CANSELIER J P.Analysis of chlorinated,sulfochlorinated and sulfonamide derivatives of n-tetradecane by gas chromatography mass spectrometry[J].Journal of Chromatography A,2005,1071(1/2):71-80.
[8]隋丽丽,隋崴崴,江艳,等.固相萃取-高效液相色谱法测定水中磺胺类药物[J].理化检验-化学分册,2013,49(4):428-431.
[9]杜鹃,赵洪霞,陈景文.固相萃取-高效液相色谱-串联质谱法同时测定养殖海水中23种抗生素[J].色谱,2015,33(4):348-353.
[10]LIU J J,JIANG M,LI G,et al.Miniaturized salting-out liquid-liquid extraction of sulfonamides from different matrices[J].Analytica Chimica Acta,2010,679(1/2):74-74.
[11]BEN W,QIANG Z,ADAMS C,et al.Simultaneous determination of sulfonamides,tetracyclines and tiamulin in swine wastewater by solid-phase extraction and liquid chromatography-mass spectrometry[J].Journal of Chromatography A,2008,1202(2):173-180.
[12]周志洪,黄卓尔,吴清柱,等.在线固相萃取-液相色谱-串联质谱法测定环境水体中抗生素[J].分析试验室,2016,9(1):1092-1098.
[13]BALAKRISHNAN V K,TERRY K A,TOITO J.Determination of sulfonamide antibiotics in wastewater:A comparison of solid phase microextraction and solid phase extraction methods[J].Journal of Chromatography A,2006,1131(1/2):1-10.
[14]MCCLURE E L,WONG C S.Solid phase microextraction of macrolide,trimethoprim,and sulfonamide antibiotics in wastewaters[J].Journal of Chromatography A,2007,1169(1/2):53-62.
[15]XU X,SU R,ZHAO X,et al.Ionic liquid-based microwave-assisted dispersive liquid-liquid microextraction and derivatization of sulfonamides in river water,honey,milk,and animal plasma[J].Analytica Chimica Acta,2011,707(1):92-99.
[16]SANTANA F D,OLIVEIRA A D,BONATO P S.Chiral liquid chromatographic determination of mirtazapine in human plasma using two-phase liquidphase microextraction for sample preparation[J].Analytica Chimica Acta,2005,549(1):96-103.
[17]HUANG S P,HUANG S D.Determination of organochlorine pesticides in water using solvent cooling assisted dynamic hollow-fiber-supported headspace liquid-phase microextraction[J].Journal of Chromatography A,2007,1176(1):19-25.
[18]TAO Y,LIU J F,HU X L,et al.Hollow fiber supported ionic liquid membrane microextraction for determination of sulfonamides in environmental water samples by high-performance liquid chromatography[J].Journal of Chromatography A,2009,1216(35):6259-6266.
[19]吴翠琴,陈迪云,周爱菊,等.离子液体单滴微萃取-高效液相色谱法测定水体中磺胺类药物[J].分析化学,2011,39(1):17-21.
[20]GUO X,YIN D,PENG J,et al.Ionic liquid-based single-drop liquid-phase microextraction combined with high-performance liquid chromatography for the determination of sulfonamides in environmental water[J].Journal of Separation Science,2012,35(3):452-458.
[21]常安刚,周凯,江静,等.温度驱动的离子液体分散液-液微萃取法同时检测环境水体中磺胺类药物[J].环境化学,2013,32(2):295-301.
[22]WEN Y,LI J,ZHANG W,et al.Dispersive liquidliquid microextraction coupled with capillary electrophoresis for simultaneous determination of sulfonamides with the aid of experimental design[J].Electrophoresis,2011,32(16):2131-2138.
[2]HE X,DENG M,WANG Q,et al.Residues and health risk assessment of quinolones and sulfonamides in cultured fish from Pearl River Delta,China[J].Aquaculture,2016,458(1):38-46.
[3]WISE R.Antimicrobial resistance:Priorities for action[J].Journal of Antimicrobial Chemotherapy,2002,49(4):585-586.
[4]洪蕾洁,石璐,张亚雷,等.固相萃取-高效液相色谱法同时测定水体中的10种磺胺类抗生素[J].环境科学,2012,33(2):652-657.
[5]HERRERA-HERRERA A V,HERNNDEZBORGES J,BORGESMIQUEL T M,et al.Dispersive liquidliquid microextraction combined with ultra-high performance liquid chromatography for the simultaneous determination of 25sulfonamide and quinolone antibiotics in water samples[J].Journal of Pharmaceutical and Biomedical Analysis,2013,75(5):130-137.
[6]WULF N R,MATUSZEWSKI K A.Sulfonamide cross-reactivity:Is there evidence to support broad cross-allergenicity?[J].American Journal of HealthSystem Pharmacy,2013,70(17):1483-1483.
[7]ASSASSI N,TAZEROUTI A,CANSELIER J P.Analysis of chlorinated,sulfochlorinated and sulfonamide derivatives of n-tetradecane by gas chromatography mass spectrometry[J].Journal of Chromatography A,2005,1071(1/2):71-80.
[8]隋丽丽,隋崴崴,江艳,等.固相萃取-高效液相色谱法测定水中磺胺类药物[J].理化检验-化学分册,2013,49(4):428-431.
[9]杜鹃,赵洪霞,陈景文.固相萃取-高效液相色谱-串联质谱法同时测定养殖海水中23种抗生素[J].色谱,2015,33(4):348-353.
[10]LIU J J,JIANG M,LI G,et al.Miniaturized salting-out liquid-liquid extraction of sulfonamides from different matrices[J].Analytica Chimica Acta,2010,679(1/2):74-74.
[11]BEN W,QIANG Z,ADAMS C,et al.Simultaneous determination of sulfonamides,tetracyclines and tiamulin in swine wastewater by solid-phase extraction and liquid chromatography-mass spectrometry[J].Journal of Chromatography A,2008,1202(2):173-180.
[12]周志洪,黄卓尔,吴清柱,等.在线固相萃取-液相色谱-串联质谱法测定环境水体中抗生素[J].分析试验室,2016,9(1):1092-1098.
[13]BALAKRISHNAN V K,TERRY K A,TOITO J.Determination of sulfonamide antibiotics in wastewater:A comparison of solid phase microextraction and solid phase extraction methods[J].Journal of Chromatography A,2006,1131(1/2):1-10.
[14]MCCLURE E L,WONG C S.Solid phase microextraction of macrolide,trimethoprim,and sulfonamide antibiotics in wastewaters[J].Journal of Chromatography A,2007,1169(1/2):53-62.
[15]XU X,SU R,ZHAO X,et al.Ionic liquid-based microwave-assisted dispersive liquid-liquid microextraction and derivatization of sulfonamides in river water,honey,milk,and animal plasma[J].Analytica Chimica Acta,2011,707(1):92-99.
[16]SANTANA F D,OLIVEIRA A D,BONATO P S.Chiral liquid chromatographic determination of mirtazapine in human plasma using two-phase liquidphase microextraction for sample preparation[J].Analytica Chimica Acta,2005,549(1):96-103.
[17]HUANG S P,HUANG S D.Determination of organochlorine pesticides in water using solvent cooling assisted dynamic hollow-fiber-supported headspace liquid-phase microextraction[J].Journal of Chromatography A,2007,1176(1):19-25.
[18]TAO Y,LIU J F,HU X L,et al.Hollow fiber supported ionic liquid membrane microextraction for determination of sulfonamides in environmental water samples by high-performance liquid chromatography[J].Journal of Chromatography A,2009,1216(35):6259-6266.
[19]吴翠琴,陈迪云,周爱菊,等.离子液体单滴微萃取-高效液相色谱法测定水体中磺胺类药物[J].分析化学,2011,39(1):17-21.
[20]GUO X,YIN D,PENG J,et al.Ionic liquid-based single-drop liquid-phase microextraction combined with high-performance liquid chromatography for the determination of sulfonamides in environmental water[J].Journal of Separation Science,2012,35(3):452-458.
[21]常安刚,周凯,江静,等.温度驱动的离子液体分散液-液微萃取法同时检测环境水体中磺胺类药物[J].环境化学,2013,32(2):295-301.
[22]WEN Y,LI J,ZHANG W,et al.Dispersive liquidliquid microextraction coupled with capillary electrophoresis for simultaneous determination of sulfonamides with the aid of experimental design[J].Electrophoresis,2011,32(16):2131-2138.