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水凝胶涂覆纸喷雾离子化用于生物流体样品直接质谱分析
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作者单位
何元毅,詹柳娟,黄光明 中国科学技术大学化学与材料科学学院 
基金项目:国家自然基金面上项目(21775143,21475121);合肥物质科学技术中心创新项目培育基金(2017FXCX003);中国科学院合肥大科学中心高端用户培育基金资助(2018HSC-UE001,2018HSC-UE016);中央高校基本科研业务费专项资金
中文摘要:基于琼脂糖水凝胶涂覆的纸基质,实现了纸喷雾离子化,建立了一种新的纸喷雾离子化质谱技术,直接分析生物流体样品。利用纸表面涂覆的水凝胶材料限制液滴的扩散,使互不相溶的喷雾溶剂液滴与生物样品液滴之间形成液液萃取,提高了检测灵敏度。同时通过限制液滴扩散,减少了喷雾溶剂挥发面积,降低了挥发速度,获得了时间更长的稳定质谱信号,可对生物流体样品中的低丰度药物快速、准确定量。相较于常规纸喷雾离子化,该方法喷雾时间延长近10倍,分析物信号提高近100倍,定量分析全血和尿液中的药物,检出限可降低7~33倍。方法材料制备简单,方便快捷,灵敏度高,在现场临床诊断上具有很大的应用潜力。
中文关键词:质谱分析  纸喷雾  液液萃取  琼脂糖水凝胶
 
Direct Mass Spectrometry Detection of Biofluid Using Hydrogel-coated Paper Spray Ionization
Abstract:A novel paper spray ionization mass spectrometric(PSI-MS) method was developed for the direct detection of biofluid.The agarose hydrogel coated paper substrate was used to alleviate the lateral diffusion of polar extraction solvent to achieve both high extraction efficiency and ambient ionization,whereupon liquid-liquid extraction occurred between the biofluid sample droplet and the polar extract/spray solvent.Hence,the overall sensitivity of hydrogel coated PSI-MS could be improved greatly due to better extraction efficiency.Meanwhile,the evaporation rate for the extract/spray solvent was reduced due to its less diffusion,and a longer and more stable continuous mass spectrometry signal was obtained.In addition,ethyl acetate was used here as spray and extract solvents to form liquid-liquid extraction,high voltage DC was applied on the hydrogel coated paper substrate where sample was placed to achieve fast and accurate quantification of low abundance therapeutic drugs in biofluid samples.Compared with PSI-MS,the hydrogel coated PSI-MS extended the spray time by nearly 10 times and the signal for analyte by about 100 times.The method was applied in the quantitative detection of drugs in whole blood and urine samples with the limits of detection(LODs) decreased by 7-33 times.The hydrogel coated PSI-MS showed its great potential in the area of on site clinical diagnosis,owing to its simple preparation,high sensitivity and convenient operation.
Key Words:mass spectrometry  paper spray  liquid-liquid extraction  agarose hydrogel
引用本文:何元毅,詹柳娟,黄光明.水凝胶涂覆纸喷雾离子化用于生物流体样品直接质谱分析[J].分析测试学报,2020,39(1):141-145.
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