DRILL: An Electrospray Ionization-Mass Spectrometry Interface for Improved Sensitivity via Inertial Droplet Sorting and Electrohydrodynamic Focusing in a Swirling Flow.

DRILL: An Electrospray Ionization-Mass Spectrometry Interface for Improved Sensitivity via Inertial Droplet Sorting and Electrohydrodynamic Focusing in a Swirling Flow.
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DOI:
10.1021/acs.analchem.7b01555
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发表时间:
2017-09-05
影响因子:
7.4
通讯作者:
Fedorov AG
Fedorov AG
中科院分区:
化学1区
文献类型:
--
作者:
Kottke PA;Lee JY;Jonke AP;Seneviratne CA;Hecht ES;Muddiman DC;Torres MP;Fedorov AG

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我们描述了 DRILL(干离子定位和运动)设备,它是电喷雾电离 (ESI)-质谱 (MS) 的接口,它利用旋流来实现惯性分离,根据电喷雾液滴的大小规定其不同的命运。该源增加了一种带电液滴轨迹操纵的新方法,当与流体动力阻力和电场力相结合时,提供了丰富的可能的钻操作模式。在这里,我们通过实验证明了通过电喷雾液滴/离子的涡流诱导惯性分选获得的灵敏度提高:一种可能的钻操作模式。在此模式下,DRILL 会去除较大的液滴,同时加速 ESI 羽流的剩余部分,产生含有高电荷小液滴和离子的高速富气体喷雾流,并将其引导至 MS 入口。使用与 ESI-MS 耦合的 DRILL 接口证明了血管紧张素 I 检测中信噪比的改善(10 倍增强)以及血管紧张素 II 检测中检测限的改善(10 倍增强,100 皮摩尔)。液相色谱 (LC)-MS 也证明了 DRILL 的实用性:将稳定同位素标记的肽混合物掺入复杂的天然组织提取物中,并通过 TSQ Vantage 上的计划外多重反应监测进行定量。 DRILL 证明 9 种肽中有 8 种的信号强度得到改善(高达 700 倍),并且对离子对的峰形没有影响。
We describe the DRILL (dry ion localization and locomotion) device, which is an interface for electrospray ionization (ESI)-mass spectrometry (MS) that exploits a swirling flow to enable the use of inertial separation to prescribe different fates for electrosprayed droplets based on their size. This source adds a new approach to charged droplet trajectory manipulation which, when combined with hydrodynamic drag forces and electric field forces, provides a rich range of possible DRILL operational modes. Here, we experimentally demonstrate sensitivity improvement obtained via vortex-induced inertial sorting of electrosprayed droplets/ions: one possible mode of DRILL operation. In this mode, DRILL removes larger droplets while accelerating the remainder of the ESI plume, producing a high velocity stream of gas-enriched spray with small, highly charged droplets and ions and directing it toward the MS inlet. The improved signal-to-noise ratio (10-fold enhancement) in the detection of angiotensin I is demonstrated using the DRILL interface coupled to ESI-MS along with an improved limit of detection (10-fold enhancement, 100 picomole) in the detection of angiotensin II. The utility of DRILL has also been demonstrated by liquid chromatography (LC)–MS: a stable isotope labeled peptide cocktail was spiked into a complex native tissue extract and quantified by unscheduled multiple reaction monitoring on a TSQ Vantage. DRILL demonstrated improved signal strength (up to a 700-fold) for 8 out of 9 peptides and had no effects on the peak shape of the transitions.
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