Differential Ion Mobility Separations/Mass Spectrometry with High Resolution in Both Dimensions

Differential Ion Mobility Separations/Mass Spectrometry with High Resolution in Both Dimensions
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DOI:
10.1021/acs.analchem.8b04518
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发表时间:
2019-01-15
影响因子:
7.4
通讯作者:
Shvartsburg, Alexandre A.
Shvartsburg, Alexandre A.
中科院分区:
化学1区
文献类型:
--
作者:
Baird, Matthew A.;Anderson, Gordon A.;Shvartsburg, Alexandre A.

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与质谱的强正交性使微分离子迁移谱 (FAIMS) 成为异构体分离的强大工具。然而,只有使用富含 He 或 H-2 的缓冲液才能总体实现高 FAIMS 分辨率。这阻碍了与在超高真空下运行的傅里叶变换质谱仪的耦合,但 FTMS 卓越的 m/z 分辨率和精度对于一线生物和环境应用是必不可少的。通过将波形幅度提高到 6 kV,我们仅使用 N-2 就实现了高 FAIMS 分辨率,从而可以与任何 MS 平台直接集成:这里是带有电子转移解离 (ETD) 选项的 Orbitrap XL。对替代位点上具有多种翻译后修饰的完整组蛋白尾(50 个残基)的初步评估表明,具有分离和自信地识别中下范围内 PTM 定位变体的广泛能力。
Strong orthogonality to mass spectrometry makes differential ion mobility spectrometry (FAIMS) a powerful tool for isomer separations. However, high FAIMS resolution has been achieved overall only with buffers rich in He or H-2. That obstructed coupling to Fourier transform mass spectrometers operating under ultrahigh vacuum, but exceptional m/z resolution and accuracy of FTMS are indispensable for frontline biological and environmental applications. By raising the waveform amplitude to 6 kV, we enabled high FAIMS resolution using solely N-2 and thus straightforward integration with any MS platform: here Orbitrap XL with the electron transfer dissociation (ETD) option. The initial evaluation for complete histone tails (50 residues) with diverse post-translational modifications on alternative sites demonstrates a broad capability to separate and confidently identify the PTM localization variants in the middle-down range.