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Investigation of kinetics of tetrabutylammonium chloride (TBAC) + CH4 semiclathrate hydrate formation

机译:四丁基氯化铵(TBAC)+ CH 4 半包合物水合物形成动力学的研究

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For potential application in advanced gas storage at moderate temperatures, a systematic study on tetrabutylammonium chloride (TBAC) + CH4 semiclathrate hydrate formation kinetics was conducted using isobaric kinetics measurements to evaluate the effects of pressure (6.0, 3.0 MPa), temperature (278 K, subcooling degree of 6 K), and salt concentration (0.10, 0.20, 0.30, 0.34, 0.45 mass fraction). The results revealed that the systems showed shorter induction time, higher normalized gas consumption and higher rapid growth rate under a higher supersaturation environment, represented by higher pressure or lower temperature. Besides, the effect of salt concentration was complicated. With the increase of salt concentration, the total gas consumption was almost the same while the normalized gas consumption decreased greatly, indicating that the amount of CH4 trapped in the hydrate unit greatly decreased and the system with low salt concentration was a good choice for advanced gas storage. In addition, a Raman device was employed to reveal the structural properties. The spectra showed that the (TBAC + CH4) semiclathrate hydrates were formed with hexagonal structure or tetragonal structure under different salt concentrations, which were different from the structures of pure TBAC hydrate. It was assumed that at low salt concentrations the addition of CH4 induced the formation of hexagonal structure since it had three 512 cages per TBAC which was higher than that of the tetragonal structure.
机译:为了在中等温度下高级气体存储中潜在应用,使用等压动力学测量法对四丁基氯化铵(TBAC)+ CH 4 半包合物水合物形成动力学进行了系统研究,以评价压力(6.0,3.0 MPa),温度(278 K,过冷度6 K)和盐浓度(0.10、0.20、0.30、0.34、0.45质量分数)的影响。结果表明,在较高的过饱和度环境下,以较高的压力或较低的温度表示,该系统显示出较短的诱导时间,较高的归一化气体消耗量和较高的快速生长速率。此外,盐浓度的影响复杂。随着盐浓度的增加,总气体消耗量几乎相同,而标准化气体消耗量却大大减少,这表明水合物单元中捕获的CH 4 量大大增加了。降低了盐浓度,低盐浓度的系统是高级气体存储的理想选择。另外,采用拉曼装置来揭示结构特性。光谱表明,在不同的盐浓度下,(TBAC + CH 4 )半包合物水合物形成为六边形或四方结构,这与纯TBAC水合物的结构不同。 。假定在低盐浓度下添加CH 4 会诱导六边形结构的形成,因为它具有三个5 12 < / TBAC的笼子比四方结构的笼子高。

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