Ultrahigh-Resolution Differential Ion Mobility Spectrometry Using Extended Separation Times

Ultrahigh-Resolution Differential Ion Mobility Spectrometry Using Extended Separation Times
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DOI:
10.1021/ac102689p
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发表时间:
2011-01-01
影响因子:
7.4
通讯作者:
Smith, Richard D.
Smith, Richard D.
中科院分区:
化学1区
文献类型:
--
作者:
Shvartsburg, Alexandre A.;Smith, Richard D.

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离子迁移率谱(IMS),特别是微分IMS或场不对称波形IMS(FAIMS),正在成为分离和识别气体的一种通用工具。相离子,特别是与质谱学相结合。自FAIMS问世以来的二十多年里,分辨率(R)一直受到低于20的限制。更强的电场和优化的混合气体最近将可实现的R提高到接近200,但这种方法的进一步进展受到电击穿的阻碍。然而,使用任意气体和场强的平面FAIMS器件的分辨率作为分离时间(T)的平方根。在这里,我们通过减少载气流量,将t从先前的最大值S扩展到4倍,并如预测的那样将分辨率提高了2倍,对于多电荷多肽,分辨率提高到>300。由此产生的拆分增益使以前的“共洗脱”多肽异构体得以分离,包括折叠异构体和修饰多肽的定位变体。更广泛地说,在胰酶消化分离中已经达到了类似200的峰值容量。
Ion mobility spectrometry (IMS), and particularly differential IMS or field asymmetric waveform IMS (FAIMS), is emerging as a versatile tool for separation and identification of gas. phase ions, especially in conjunction with mass spectrometry. For over two decades since its inception, the utility of FAIMS was constrained by resolving power (R) of less than similar to 20. Stronger electric fields and optimized gas mixtures have recently raised achievable R to similar to 200, but further progress with such approaches is impeded by electrical breakdown. However, the resolving power of planar FAIMS devices using any gas and field intensity scales as the square root of separation time (t). Here, we extended t from the previous maximum of 0.2 s up to 4-fold by reducing the carrier gas flow and increased the resolving power by up to 2-fold as predicted, to >300 for multiply charged peptides. The resulting resolution gain has enabled separation of previously "co-eluting" peptide isomers, including folding conformers and localization variants of modified peptides. More broadly, a peak capacity of similar to 200 has been reached in tryptic digest separations.