Title: Fluorographene as a Mass Spectrometry Probe for High-Throughput Identification and Screening of Emerging Chemical Contaminants in Complex Samples

Author: Xiu Huang, Qian Liu*, Xiaoyu Huang, Zhou Nie, Ting Ruan, Yuguo Du, and Guibin Jiang

Abstract: Mass spectrometry techniques for high-throughput analysis of complex samples are of profound importance in many areas such as food safety, omics studies, and environmental health science. Here we report the use of fluorographene (FG) as a new mass spectrometry probe for high-throughput identification and screening of emerging chemical contaminants in complex samples. FG was facilely synthesized by one-step exfoliation of fluorographite. With FG as a matrix or probe in matrix-assisted or surface-enhanced laser desorption/ionization time-of-flight mass spectrometry (MALDI- or SELDI-TOF MS), higher sensitivity (detection limits at ppt or subppt levels), and better reproducibility were achieved than with other graphene-based materials due to the unique chemical structure and self-assembly properties of FG. The method was validated with different types of real complex samples. By using FG as a SELDI probe, we could easily detect trace amount of bisphenol S in paper products and high-fat canned food samples. Furthermore, we have successfully identified and screened as many as 28 quaternary ammonium halides in sewage sludge samples collected from municipal wastewater treatment plants. These results demonstrate that FG probe is a powerful tool for high-throughput analysis of complex samples by MS.

Link: http://pubs.acs.org/doi/abs/10.1021/acs.analchem.6b04167

Comments:

这一工作描述了一种新的高通量质谱探针——氟化石墨烯（FG），既可以在MALDI-TOF MS中作为小分子分析的基质使用，又可以作为富集材料实现痕量目标分析物的高效富集。与传统的石墨烯相比，氟化可以赋予这种材料一些特殊的性质，使之可应用于更广范围的分析物。

我们除了测试了这种材料对一些常规的污染物的分析性能，还用它对一些纸制品和罐头食品中的双酚S进行了快速检测，并且可以对污泥中的季铵盐类新型污染物进行快速鉴定与筛查，表明这种材料可以直接应用于复杂样品的分析。这种材料是上海有机所黄晓宇老师课题组合成的，在此也对黄老师表示感谢！

这一工作投到Anal. Chem.后，很快就收到了审稿意见，两位审稿人均给出了“Publish either as is or subject to minor revisions as indicated”的意见。一个小插曲是ACS的投稿系统显示文章和我们之前发表的论文有18%的重复（实际上基本上都是一些惯用的实验条件描述和一些专有名词等），但是我们并未对自己之前的论文进行引用，因此编辑建议把我们之前的论文也引上就OK了。看来适当的自引也是有必要的~~

传统意义上一般认为MALDI-TOF MS只能用于大分子的定性分析，我们近期的工作表明作为一种简单、快速、高通量的质谱技术，MALDI-TOF MS的应用潜力还大有可挖掘的空间，特别是在痕量小分子化合物的分析方面，MALDI-TOF MS大有可为！

欢迎各位同行拍砖！

FG for LDI MS.pdf