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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Product screening of fast reactions in IR-laser-heated liquid water filaments in a vacuum by mass spectrometry
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Product screening of fast reactions in IR-laser-heated liquid water filaments in a vacuum by mass spectrometry

机译：质谱法在真空中红外激光加热的液态水细丝中快速反应的产物筛选

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摘要

In the present article a novel approach for rapid product screening of fast reactions in IR-laser-heated liquid microbeams in a vacuum is highlighted. From absorbed energies, a shock wave analysis, high-speed laser stroboscopy, and thermodynamic data of high-temperature water the enthalpy, temperature, density, pressure, and the reaction time window for the hot water filament could be characterized. The experimental conditions (30 kbar, 1750 K, density similar to 1 g/cm(3)) present during the lifetime of the filament (20-30 ns) were extreme and provided a unique environment for high-temperature water chemistry. For the probe of the reaction products liquid beam desorption mass spectrometry was employed. A decisive feature of the technique is that ionic species, as well as neutral products and intermediates may be detected (neutrals as protonated aggregates) via time-of-flight mass spectrometry without any additional ionization laser. After the explosive disintegration of the superheated beam, high-temperature water reactions are efficiently quenched via expansion and evaporative cooling. For first exploratory experiments for chemistry in ultrahigh-temperature, -pressure and -density water, we have chosen resorcinol as a benchmark system, simple enough and well studied in high-temperature water environments much below 1000 K. Contrary to oxidation reactions usually present under less extreme and dense supercritical conditions, we have observed hydration and little H-atom abstraction during the narrow time window of the experiment. Small amounts of radicals but no ionic intermediates other than simple proton adducts were detected. The experimental findings are discussed in terms of the energetic and dense environment and the small time window for reaction, and they provide firm evidence for additional thermal reaction channels in extreme molecular environments.
机译：在本文中，提出了一种在真空中红外激光加热的液体微束中快速反应的快速产物筛选的新方法。从吸收的能量，冲击波分析，高速激光频闪法和高温水的热力学数据，可以表征热水丝的焓，温度，密度，压力和反应时间窗口。在灯丝寿命（20-30 ns）内存在的实验条件（30 kbar，1750 K，密度类似于1 g / cm（3））非常苛刻，为高温水化学提供了独特的环境。对于反应产物的探针，使用液束解吸质谱法。该技术的决定性特征是无需任何额外的电离激光，即可通过飞行时间质谱检测离子种类以及中性产物和中间体（中性为质子化的聚集体）。过热束爆炸性分解后，高温水反应通过膨胀和蒸发冷却被有效地淬灭。在超高温，高压和高密度水中进行化学实验的第一个探索性实验中，我们选择间苯二酚作为基准系统，该方法足够简单，并且在远低于1000 K的高温水环境中进行了深入研究。与氧化反应相反，通常在在极端和密集的超临界条件下，我们在狭窄的时间窗口内观察到水合和少量H原子抽象。除了简单的质子加合物，检测到少量的自由基，但没有离子中间体。从高能和稠密的环境以及较小的反应时间窗口讨论了实验发现，它们为极端分子环境中其他热反应通道提供了有力的证据。

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