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多路复用化学动力学光电离质谱仪:一种解析异构体化学动力学的新方法。

The multiplexed chemical kinetic photoionization mass spectrometer: a new approach to isomer-resolved chemical kinetics.

作者信息

Osborn David L, Zou Peng, Johnsen Howard, Hayden Carl C, Taatjes Craig A, Knyazev Vadim D, North Simon W, Peterka Darcy S, Ahmed Musahid, Leone Stephen R

机构信息

Combustion Research Facility, Mail Stop 9055, Sandia National Laboratories, Livermore, California 94551-0969, USA.

出版信息

Rev Sci Instrum. 2008 Oct;79(10):104103. doi: 10.1063/1.3000004.

DOI:10.1063/1.3000004
PMID:19044733
Abstract

We have developed a multiplexed time- and photon-energy-resolved photoionization mass spectrometer for the study of the kinetics and isomeric product branching of gas phase, neutral chemical reactions. The instrument utilizes a side-sampled flow tube reactor, continuously tunable synchrotron radiation for photoionization, a multimass double-focusing mass spectrometer with 100% duty cycle, and a time- and position-sensitive detector for single ion counting. This approach enables multiplexed, universal detection of molecules with high sensitivity and selectivity. In addition to measurement of rate coefficients as a function of temperature and pressure, different structural isomers can be distinguished based on their photoionization efficiency curves, providing a more detailed probe of reaction mechanisms. The multiplexed three-dimensional data structure (intensity as a function of molecular mass, reaction time, and photoionization energy) provides insights that might not be available in serial acquisition, as well as additional constraints on data interpretation.

摘要

我们开发了一种用于研究气相中性化学反应动力学和异构产物分支的多路复用时间和光子能量分辨光电离质谱仪。该仪器采用侧面采样流动管反应器、用于光电离的连续可调同步辐射、占空比为100%的多质量双聚焦质谱仪以及用于单离子计数的时间和位置敏感探测器。这种方法能够以高灵敏度和选择性对分子进行多路复用通用检测。除了测量速率系数作为温度和压力的函数外,不同的结构异构体可以根据其光电离效率曲线进行区分,从而为反应机理提供更详细的探测。多路复用三维数据结构(强度作为分子量、反应时间和光电离能量的函数)提供了串行采集可能无法获得的见解,以及对数据解释的额外约束。

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