Dramatic Improvement in Sensitivity with Pulsed Mode Charge Detection Mass Spectrometry.

Dramatic Improvement in Sensitivity with Pulsed Mode Charge Detection Mass Spectrometry.
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脉冲模式电荷检测质谱法的灵敏度显着提高。

DOI:
10.1021/acs.analchem.9b03586
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发表时间:
2019
影响因子:
7.4
通讯作者:
Jarrold,MartinF
Jarrold,MartinF
中科院分区:
化学1区
文献类型:
--
作者:
Todd,AaronR;Jarrold,MartinF

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电荷检测质谱(CDMS)是一种新兴的有价值的工具,以确定质量分布的异质性和高质量的样品。它是一种单粒子技术,其中通过同时测量其质荷比(m/z)和电荷来确定单个离子的质量。离子被捕获在静电线性离子阱(ELIT)中,并通过检测圆柱来回振荡。阱是打开的,并且能够捕获离子持续总测量时间的一小部分,因此连续离子束中的大部分离子(>99.8%)丢失。在这里,我们实现了一个离子存储方案,其中离子被积累和存储在一个六极,然后在正确的时间注入ELIT,使它们被捕获。这种脉冲操作模式将CDMS的灵敏度提高了2个数量级以上,这允许分析低得多的滴度样品。用1.3 μL样品检测T = 4个衣壳的B型肝炎病毒的最低检测限为3.3 × 108个/mL。离子聚集和存储的六极离离子阱有相当大的距离,因此当离子在六极和ELIT之间移动时,离子会通过它们的m/z值及时分散。通过改变离子释放和捕获之间的延迟时间,可以捕获不同的m/z值窗口。
Charge detection mass spectrometry (CDMS) is emerging as a valuable tool to determine mass distributions for heterogeneous and high-mass samples. It is a single-particle technique where masses are determined for individual ions from simultaneous measurements of their mass-to-charge ratio (m/z) and charge. Ions are trapped in an electrostatic linear ion trap (ELIT) and oscillate back and forth through a detection cylinder. The trap is open and able to trap ions for a small fraction of the total measurement time so most of the ions (>99.8%) in a continuous ion beam are lost. Here, we implement an ion storage scheme where ions are accumulated and stored in a hexapole and then injected into the ELIT at the right time for them to be trapped. This pulsed mode of operation increases the sensitivity of CDMS by more than 2 orders of magnitude, which allows much lower titer samples to be analyzed. A limit of detection of 3.3 × 108particles/mL was obtained for hepatitis B virusT= 4 capsids with a 1.3 μL sample. The hexapole where the ions are accumulated and stored is a significant distance from the ion trap so ions are dispersed in time by theirm/zvalues as they travel between the hexapole and the ELIT. By varying the delay time between ion release and trapping, different windows ofm/zvalues can be trapped.
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