Wang He-Xing, Wang Bin, Zhou Ying, Jiang Qing-Wu
Key Laboratory of Public Health Safety of Ministry of Education, School of Public Health, Fudan University, Shanghai, 200032, China.
Anal Bioanal Chem. 2014 Dec;406(30):8049-58. doi: 10.1007/s00216-014-8197-6. Epub 2014 Oct 30.
A rapid and sensitive method for the screening and selective quantification of antibiotics in urine by two-dimensional ultraperformance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was developed. This method allowed the injection of 200 μL urine extract. The 200-μL injection volume used in this method increased the absolute sensitivity for target antibiotics in solvent by an average 13.3 times, with a range from 8.4 to 28.5 times, compared with the 10-μL conventional injection volume. A 96-well solid phase extraction procedure was established to eliminate the contamination on the chromatographic column resulting from the large-volume injection and increase the throughput of sample preparation. Fourteen target antibiotics from six common categories (β-lactams, quinolones, tetracyclines, macrolides, sulfonamides, and chloramphenicols) were selected as model compounds, and a database containing an additional 74 antibiotics was compiled for posttarget screening. The limit of detection of the target antibiotics, defined as a signal-to-noise ratio of 3, ranged from 0.04 to 1.99 ng/mL. The mean interday recoveries ranged between 79.6 and 121.3 %, with a relative standard deviation from 2.9 to 18.3 % at three spiking levels of 20 ng/mL, 50 ng/mL, and 100 ng/mL. This method was successfully applied in 60 real urine samples from schoolchildren aged 8-11 years, and four target antibiotics (azithromycin, sulfadiazine, trimethoprim, and oxytetracycline) and two posttarget antibiotics (sulfadimidine and cefaclor) were found in the urine samples. This method can be used as a large-scale biomonitoring tool for exposure of the human population to antibiotics.
建立了一种二维超高效液相色谱-四极杆飞行时间质谱联用快速灵敏的尿液中抗生素筛选及选择性定量分析方法。该方法允许进样200 μL尿液提取物。与10 μL传统进样体积相比,此方法采用的200 μL进样体积使目标抗生素在溶剂中的绝对灵敏度平均提高了13.3倍,范围为8.4至28.5倍。建立了96孔固相萃取程序,以消除大体积进样对色谱柱造成的污染并提高样品制备通量。选择了来自6个常见类别的14种目标抗生素(β-内酰胺类、喹诺酮类、四环素类、大环内酯类、磺胺类和氯霉素类)作为模型化合物,并编制了一个包含另外74种抗生素的数据库用于目标后筛选。目标抗生素的检测限定义为信噪比为3时,范围为0.04至1.99 ng/mL。在20 ng/mL、50 ng/mL和100 ng/mL三个加标水平下,日间平均回收率在79.6%至121.3%之间,相对标准偏差为2.9%至18.3%。该方法成功应用于60份8至11岁学龄儿童的实际尿液样本,在尿液样本中发现了4种目标抗生素(阿奇霉素、磺胺嘧啶、甲氧苄啶和土霉素)和2种目标后抗生素(磺胺二甲嘧啶和头孢克洛)。该方法可作为人群抗生素暴露的大规模生物监测工具。