Combining Ultraviolet Photodissociation and Two-Dimensional Mass Spectrometry: A Contemporary Approach for Characterizing Singly Charged Agrochemicals
Combining Ultraviolet Photodissociation and Two-Dimensional Mass Spectrometry: A Contemporary Approach for Characterizing Singly Charged Agrochemicals
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DOI：
10.1021/acs.analchem.1c01185
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发表时间：
2021-07-01
影响因子：
7.4
通讯作者：
O'Connor, Peter B.
中科院分区：
文献类型：
--
作者：
Marzullo, Bryan P.;Morgan, Tomos E.;O'Connor, Peter B.
紫外光解离（UVPD）已被证明可以为各种化学上不同的化合物产生广泛的结构信息数据。在这里，我们证明了193 nm UVPD片段化技术的性能上的结构/部分表征的14个单电荷的农用化学品。二维质谱（2DMS）使用红外多光子解离（IRMPD）和电子诱导解离（EID）先前已被应用到一个选择范围的单电荷农药。通过UVPD和2D-UVPD方法对大多数物质实现的>= 80%的部分覆盖率与先前研究中通过其他片段化技术获得的数据相当，并且在某些情况下上级，表明UVPD对这些类型的物质是可行的。采用三维（3D）峰拾取方法从2DMS光谱中提取数据，克服了以往研究中使用的线提取方法的局限性，成功地分离出了毫道尔顿精度的前体特异性片段。全光谱内部校准结合3D峰值拾取在整个2DMS光谱中获得了百万分之一（ppm）到十亿分之一（ppb）的质量精度。
Ultraviolet photodissociation (UVPD) has been shown to produce extensive structurally informative data for a variety of chemically diverse compounds. Herein, we demonstrate the performance of the 193 nm UVPD fragmentation technique on structural/moiety characterization of 14 singly charged agro-chemicals. Two-dimensional mass spectrometry (2DMS) using infrared multiphoton dissociation (IRMPD) and electron-induced dissociation (EID) have previously been applied to a select range of singly charged pesticides. The >= 80% moiety coverage achieved for the majority of the species by the UVPD and 2D-UVPD methods was on par with and, in some cases, superior to the data obtained by other fragmentation techniques in previous studies, demonstrating that UVPD is viable for these types of species. A three-dimensional (3D) peak picking method was implemented to extract the data from the 2DMS spectrum, overcoming the limitations of the line extraction method used in previous studies, successfully separating precursor specific fragments with milli-Dalton accuracy. Whole spectrum internal calibration combined with 3D peak picking obtained sub-part-per-million (ppm) to part-per-billion (ppb) mass accuracies across the entire 2DMS spectrum.