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通讯:小笼竞争负载的定量傅里叶变换红外数据,用于全蒸气瞬间形成气体水合物气溶胶。

Communication: quantitative Fourier-transform infrared data for competitive loading of small cages during all-vapor instantaneous formation of gas-hydrate aerosols.

机构信息

Department of Chemistry, Suleyman Demirel University, Isparta 32260, Turkey.

出版信息

J Chem Phys. 2011 Oct 14;135(14):141103. doi: 10.1063/1.3652756.

Abstract

A simple method has been developed for the measurement of high quality FTIR spectra of aerosols of gas-hydrate nanoparticles. The application of this method enables quantitative observation of gas hydrates that form on subsecond timescales using our all-vapor approach that includes an ether catalyst rather than high pressures to promote hydrate formation. The sampling method is versatile allowing routine studies at temperatures ranging from 120 to 210 K of either a single gas or the competitive uptake of different gas molecules in small cages of the hydrates. The present study emphasizes hydrate aerosols formed by pulsing vapor mixtures into a cold chamber held at 160 or 180 K. We emphasize aerosol spectra from 6 scans recorded an average of 8 s after "instantaneous" hydrate formation as well as of the gas hydrates as they evolve with time. Quantitative aerosol data are reported and analyzed for single small-cage guests and for mixed hydrates of CO(2), CH(4), C(2)H(2), N(2)O, N(2), and air. The approach, combined with the instant formation of gas hydrates from vapors only, offers promise with respect to optimization of methods for the formation and control of gas hydrates.

摘要

一种简单的方法已经被开发出来,用于测量气体水合物纳米颗粒气溶胶的高质量傅里叶变换红外(FTIR)光谱。该方法的应用使得我们能够使用全蒸汽方法,包括醚催化剂而不是高压来促进水合物形成,对在亚秒时间尺度上形成的气体水合物进行定量观察。这种采样方法具有通用性,允许在 120 到 210 K 的温度范围内对单一气体或水合物小笼中不同气体分子的竞争吸收进行常规研究。本研究强调了通过将蒸汽混合物脉冲到保持在 160 或 180 K 的冷室中形成的水合物气溶胶。我们强调了在“瞬间”形成水合物后平均 8 秒记录 6 次扫描的气溶胶光谱,以及随着时间的推移水合物的演变。我们报告和分析了单一小笼客体和 CO(2)、CH(4)、C(2)H(2)、N(2)O、N(2)和空气的混合水合物的定量气溶胶数据。这种方法与仅从蒸汽瞬间形成气体水合物相结合,为优化气体水合物的形成和控制方法提供了希望。

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