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

机译:四丁基氯化铵(TBAC)+ CH4半浆液水合物形成的动力学研究

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摘要

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:对于在中等温度下在先进的气体存储潜在的应用,在氯化四丁基铵进行系统研究(TBAC)+ CH4 semiclathrate水合物形成动力学,使用同量异序动力学测量来评价的压力的效果而进行(6.0,3.0兆帕),温度(278 K,过冷-6 K的程度),和盐浓度(0.10,0.20,0.30,0.34,0.45质量分数)。结果表明,该系统表现出更短的诱导时间,较高的归一化的气体消耗和更高的快速增长速率更高的过饱和的环境中,由较高的压力或较低的温度下表示。此外,盐浓度的影响是复杂的。随着盐浓度的增加,总的气体消耗量几乎相同,而归一化的气体消耗大大降低,表明CH4的截留在水合物单元中的量显着降低,并用低盐浓度的系统是为先进的气体的好选择贮存。另外,采用了这样的拉曼装置以显示结构特性。该光谱表明,(TBAC + CH4)semiclathrate水合物用不同盐浓度下六方结构或四方结构,这是由纯TBAC水合物的结构的不同而形成。据推断,在低盐浓度加入CH4的诱导六边形结构的形成,因为它具有每TBAC 3个512笼这比四方结构的更高。

著录项

  • 来源
    《RSC Advances》 |2017年第84期|共7页
  • 作者

    Shi Lingli; Liang Deqing;

  • 作者单位

    Chinese Acad Sci Guangzhou Inst Energy Convers CAS Key Lab Gas Hydrate Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci Guangzhou Inst Energy Convers CAS Key Lab Gas Hydrate Guangzhou 510640 Guangdong Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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