Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique
Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique
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DOI：
10.1021/acs.analchem.9b05718
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发表时间：
2020-07-21
影响因子：
7.4
通讯作者：
McLean, John A.
中科院分区：
文献类型：
--
作者：
May, Jody C.;Knochenmuss, Richard;McLean, John A.
描述了一种用于提高离子迁移率测量的灵敏度和分辨率的组合数据采集和数据处理策略。该策略在市售的漂移管离子迁移率质谱（IM-MS）仪器上实现，并利用现有的离子多路复用策略来实现高达8倍的离子信号增益和新的采集后数据重建技术，称为“高分辨率解复用”（HRdm），以提高离子迁移率维度的分辨率。一系列的异构体混合物进行了定性研究与HRdm，包括生物相关的脂质和碳水化合物，成功地解决了HRdm，包括两个单糖区域异构体的漂移时间仅为0.8%的差异。对于复杂的三糖异构体混合物，HRdm能够分离6种组分中的5种。对双峰分辨率（R-pp）和峰间分离（Δ P）的分析表明，HRdm在最高去卷积设置下的有效分辨率（R-p）在180至250之间。总体分析时间和漂移时间测量精度被认为是不受影响的标准和HRdm处理的数据集，这使得统计上相同的碰撞截面值直接从所有离子迁移率谱确定。
A combined data acquisition and data processing strategy for improving the sensitivity and resolution of ion mobility measurements is described. This strategy is implemented on a commercially available drift tube ion mobility-mass spectrometry (IM-MS) instrument and utilizes both an existing ion multiplexing strategy to achieve up to an 8-fold gain in ion signal and a new postacquisition data reconstruction technique, termed "high resolution demultiplexing" (HRdm), to improve resolution in the ion mobility dimension. A series of isomeric mixtures were qualitatively investigated with HRdm, including biologically relevant lipids and carbohydrates, which were successfully resolved by HRdm, including two monosaccharide regioisomers which differed in drift time by only 0.8%. For a complex trisaccharide isomer mixture, HRdm was able to resolve 5 out of 6 components. An analysis of two-peak resolution (R-pp) and peak-to-peak separation (Delta P) indicated that HRdm performs with an effective resolving power (R-p) of between 180 to 250 for the highest deconvolution settings. Overall analysis times and drift time measurement precision were found to be unaffected between standard and HRdm processed data sets, which allowed statistically identical collision cross section values to be directly determined from all ion mobility spectra.