Title: Screening of Toxic Chemicals in a Single Drop of Human Whole Blood Using Ordered Mesoporous Carbon as a Mass Spectrometry Probe

Authors: Xiu Huang, Qian Liu*, Jianjie Fu, Zhou Nie, Ke Gao, and Guibin Jiang

Abstract: Surface-enhanced laser desorption/ionization (SELDI) is a versatile and high-throughput mass spectrometry (MS) technique that uses a probe for extraction, enrichment, desorption, and ionization of target analytes. Here we report ordered mesoporous carbon as a new SELDI probe for rapid screening and identification of trace amount of toxic chemicals in a single drop of human whole blood without complicated sample preparation procedures. We demonstrate that ordered mesoporous carbon not only can selectively enrich a wide variety of low-mass toxic compounds from whole blood samples but also can be used as an excellent matrix to assist the laser desorption/ionization process of small molecules with low background noise, high repeatability, and good salt tolerance. High sensitivity (detection limits at ppt levels) and good reproducibility for typical toxic compounds were obtained. With CMK-8 as a SELDI probe, we successfully identified and screened six perfluorinated compounds in a single drop of whole blood collected from workers in a perfluorochemical plant. The method was also validated with complex samples such as human urine and environmental water samples. With distinct advantages such as simplicity, rapidness, minimal sample requirement, and high reliability, this method keeps great promise for various aspects of application.

Link: http://pubs.acs.org/doi/abs/10.1021/acs.analchem.6b00444 

Comments:

这个工作是上一个工作的延续。在上一个工作中，我们开发了一种有序介孔碳萃取+石墨烯MALDI基质的质谱筛查方法，可以高通量、快速地对复杂样品中的痕量污染物进行筛查。文章发表后，我们就思考，是否可以直接将有序介孔碳作为MALDI基质呢，这样就无需使用石墨烯，可以直接在介孔碳上进行质谱分析，也省略了洗脱的步骤，方法不就更加快速简便吗？于是立刻就进行了尝试，发现介孔碳果然是可以直接作为MALDI基质使用的，而且效果还不错！经过查阅文献，发现目前还没有使用介孔碳作为MALDI基质的文献，这样就保证在方法上具有创新性。但是仅仅开发一种新基质，工作的档次还是不够。于是我们就尝试用这种方法进行更复杂的样品（全血）、更小的样品量（单滴）的分析，这样这种新方法的可应用性就得到了进一步的增强，也更贴近实际分析的需求。

思路确定后，实验进行得就比较顺利了。令人兴奋的是，在单滴人全血的分析中，我们得到了比上一个工作更好的结果：我们可以筛查出工人体内更多种的痕量有毒污染物，而且分析结果比之前的方法更准确、分析速度更快！这些结果给予了我们更大的信心。

论文撰写好后，直接投给了Anal. Chem.。一个月后，审稿意见回来，两位审稿人均建议小修后接受，于是改好后很快就接受了。

这种新方法充分地发挥了有序介孔碳这种新材料的多方位的能力，纳米孔道、光能量吸收、传递等。借助这些性能，我们仅仅需要一滴血样，就可以对其中的多种痕量有毒有害物质进行高通量筛查。该方法在不同的领域如环境健康、法医学、组学等都应该有着不错的应用前景。  

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