质子提取反应质谱测定OH离子和酮类、酸类有机物间反应速率常数

Measuring the Rate Constants of Reactions Between OH and Ketone/Acids by Proton Extraction Reaction Mass Spectrometry

  • 摘要: 近年来,一种新的质子提取反应质谱(proton extraction reaction mass spectrometry,PER-MS)技术被提出,其使用OH作为母体离子检测VOCs,相对于传统质子转移反应质谱(proton transfer reaction mass spectrometry,PTR-MS)技术扩大了可检测范围,但由于缺乏OH和VOCs之间的反应速率常数数据,限制了其自定量测量的能力。本研究建立了一种可测量OH和VOCs之间反应速率常数的方法,在漂移管温度为308 K的环境中,对OH和7种VOCs(丙酮、2-丁酮、2-戊酮、2-己酮、2-庚酮、甲酸和乙酸)之间的反应速率常数进行测定,其中,丙酮、2-丁酮和甲酸的测量结果与文献理论计算/测量数据一致,证明了该方法的可靠性。本研究丰富了OH和VOCs之间的反应速率常数数据库,提高了PER-MS技术的自定量测量能力。

     

    Abstract: Due to its characteristics of short response time (1-10 s), low limit of detection (LOD) (10−12 (V/V)), and self-quantitative measurement, proton transfer reaction mass spectrometry (PTR-MS) has become a powerful technique for real-time trace detection of volatile organic compounds (VOCs). Different from traditional VOCs detection technology, PTR-MS is termed as self-quantitative detection, can provide empirical concentration of the analytes without calibration, which makes it more advantageous in the quantitative detection of multi-component VOCs. Self-quantitative measurement detects the concentration of VOCs by calculating the reaction rate constants of ion-molecule reactions, there is no need for prior calibration unless exceptionally high measurement accuracy is desired. In 2014, our research team developed a new method of proton-extraction-reaction mass spectrometry (PER-MS) with OH anion as the reagent ions, which can be applied for the detection of VOCs and even inorganic compounds. Due to the lack of reaction rate constant data of OH and VOCs, the ability for self-quantitative measurements is limited. Therefore, in order to expand the data on the reaction rate constants of OH and VOCs and promote the self-quantitative measurement ability of PER-MS technique, a new method of proton extraction reaction mass spectrometry (PER-MS) was developed for measuring reaction rate constants of OH and VOCs. The reaction rate constants were calculated based on the reaction kinetic equations after detecting the signal intensity of product ions and reactive ions by PER-MS and measuring the number density of VOCs and the reaction time. In this work, the pressure in the ion detection system was 7.4×10−5 Pa, the pressure in the drift tube was 200 Pa, and the temperature of drift tube was kept at 308 K. Acetonitrile was used as a reference to measure the reaction rate constants of acetone with OH. The measured results are agreement with the data reported in the literature. The reaction rate constants of seven VOCs (acetone, 2-butanone, 2-pentanone, 2-hexanone, 2-heptanone, formic acid and acetic acid) reacting with OH ion were measured by the proposed method. The results enrich the contents of the reaction rate constants between OH and VOCs, and improve the capability of self-quantitative detection for PER-MS, and also provide a useful reference for the research of ion-molecular reactions.

     

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