Dynamic range and mass accuracy of wide-scan direct infusion nanoelectrospray Fourier transform ion cyclotron resonance mass spectrometry-based metabolomics increased by the spectral stitching method
Dynamic range and mass accuracy of wide-scan direct infusion nanoelectrospray Fourier transform ion cyclotron resonance mass spectrometry-based metabolomics increased by the spectral stitching method
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DOI：
10.1021/ac062446p
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发表时间：
2007-06-15
影响因子：
7.4
通讯作者：
Viant, Mark R.
中科院分区：
文献类型：
--
作者：
Southam, Andrew D.;Payne, Tristan G.;Viant, Mark R.
直接注入纳米电喷雾傅里叶变换离子回旋共振质谱（DI nESI FT-ICR MS）为分析复杂代谢物混合物提供了高质量准确度和分辨率。然而，在宽质量范围内的高动态范围只能以牺牲质量精度为代价来实现，因为进入ICR检测器的大量离子会引起不利的空间电荷效应。在这里，我们报告了宽扫描DI nESI FT-ICR MS的优化策略，该策略增加了动态范围，但保持了高质量准确度。它包括多个相邻的选择离子监测（SIM）窗口的集合，这些窗口使用新型算法缝合在一起。最终的SIM拼接方法来自于几个优化实验，包括21个相邻的SIM窗口，每个窗口的宽度m/z为30（从m/z 70到500;相邻窗口重叠m/z 10），自动增益控制（AGC）目标为1 × 10（5）个电荷。SIM拼接和宽扫描范围（WSR; Thermo Electron）使用定义的标准进行比较，以评估质量准确度，并使用肝脏提取物评估峰计数和动态范围。与WSR（AGC目标分别为1 x 10（5）和5 x 10（5））相比，SIM拼接将最大质量误差降低了1.3倍和4.3倍，并将峰值计数增加了5.3倍和1.8倍。SIM拼接实现了0.18 ppm的均方根质量误差，并在肝脏提取物中检测到超过3000个峰。这种新方法增加了代谢组覆盖率，具有非常高的质量准确性，并且在5.5分钟/样品下有利于高通量代谢组学。
Direct infusion nanoelectrospray Fourier transform ion cyclotron resonance mass spectrometry (DI nESI FT-ICR MS) offers high mass accuracy and resolution for analyzing complex metabolite mixtures. High dynamic range across a wide mass range, however, can only be achieved at the expense of mass accuracy, since the large numbers of ions entering the ICR detector induce adverse space-charge effects. Here we report an optimized strategy for wide-scan DI nESI FT-ICR MS that increases dynamic range but maintains high mass accuracy. It comprises the collection of multiple adjacent selected ion monitoring (SIM) windows that are stitched together using novel algorithms. The final SIM-stitching method, derived from several optimization experiments, comprises 21 adjoining SIM windows each of width m/z 30 (from m/z 70 to 500; adjacent windows overlap by m/z 10) with an automated gain control (AGC) target of 1 x 10(5) charges. SIM-stitching and wide-scan range (WSR; Thermo Electron) were compared using a defined standard to assess mass accuracy and a liver extract to assess peak count and dynamic range. SIM-stitching decreased the maximum mass error by 1.3- and 4.3-fold, and increased the peak count by 5.3- and 1.8-fold, versus WSR (AGC targets of 1 x 10(5) and 5 x 10(5), respectively). SIM-stitching achieved an rms mass error of 0.18 ppm and detected over 3000 peaks in liver extract. This novel approach increases metabolome coverage, has very high mass accuracy, and at 5.5 min/sample is conducive for high-throughput metabolomics.