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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >New Insights on Gas Hydroquinone Clathrates Using in Situ Raman Spectroscopy: Formation/Dissociation Mechanisms, Kinetics, and Capture Selectivity
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New Insights on Gas Hydroquinone Clathrates Using in Situ Raman Spectroscopy: Formation/Dissociation Mechanisms, Kinetics, and Capture Selectivity

机译:使用原位拉曼光谱法的气体氢醌包装的新见解:形成/解离机制,动力学和捕获选择性

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Hydroquinone (HQ) is known to form organic clathrates with different gaseous species over a wide range of pressures and temperatures. However, the enclathration reaction involving HQ is not fully understood. This work offers new elements of understanding HQ clathrate formation and dissociation mechanisms. The kinetics and selectivity of the enclathration reaction were also investigated. The focus was placed on HQ clathrates formed with CO2 and CH4 as guest molecules for potential use in practical applications for the separation of a CO2/CH4 gas mixture. The structural transition from the native form (alpha-HQ) to the clathrate form (beta-HQ), as well as the reverse process, were tracked using in situ Raman spectroscopy. The clathrate formation was conducted at 323 K and 3.0 MPa, and the dissociation was conducted at 343 K and 1.0 kPa. The experiments with CH4 confirmed that a small amount of gas can fill the alpha-HQbefore the phase transition from alpha- to beta-HQ begins. The dissociation of the CO2-HQ clathrates highlighted the presence of a clathrate structure with no guest molecules. We can therefore conclude that HQ clathrate formation and dissociation are two-step reactions that pass through two distinct reaction intermediates: guest loaded alpha-HQ and guest-free beta-HQ When an equimolar CO2/CH4 gas mixture is put in contact with either the alpha-HQ or the guest-free beta-HQ the CO2 is preferentially captured. Moreover, the guest-free beta-HQ can retain the CO2 quicker and more selectively.
机译:已知氢醌(HQ)以在各种压力和温度范围内形成具有不同气态物质的有机克拉氏物。然而,涉及总HQ的外壳反应尚未完全理解。这项工作提供了了解HQ Clathrate地层和解离机制的新内容。还研究了壳体反应的动力学和选择性。将重点放在用CO 2和CH 4形成的HQ Clathrates上,作为用于分离CO 2 / CH4气体混合物的实际应用中的潜在应用。使用原位拉曼光谱跟踪从天然形式(α-HQ)到包裹形式(β-HQ)以及反向过程的结构过渡。在323 k和3.0MPa下进行包合物形成,并在343k和1.0kPa下进行解离。 CH4的实验证实,少量气体可以填充α-hqefore从α-至β-hQ开始的相变。 CO2-HQ Clathrates的解离强调了没有客销分子的裂纹结构的存在。因此,我们可以得出结论,HQ Clathrate的形成和解离是通过两个不同反应中间体的两步反应:客人装载了α-HQ和无众不宾β-HQ,当等摩尔CO2 / CH4气体混合物与任何一种优先捕获Alpha-HQ或Fiable-Free Beta-HQ。此外,无家客人的Beta-HQ可以更快地保留CO2和更有用的。

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