Visualization investigation of TBAB hydrate formation in droplets on supercooled wall surfaces

doi:10.11949/0438-1157.20200982

Abstract

Abstract:

Hydrate is widely used in gas separation, transportation and storage, sewage treatment, seawater desalination and cold storage. However, natural hydrate formation is extremely slow, requiring higher pressure and lower temperature to maintain stability. In this paper, the nucleation and growth of tetrabutylammonium bromide (TBAB) hydrate crystals in a 2 μl droplet is experimentally studied by a high-speed camera under different subcooling degrees and concentrations. The growth characteristics of TBAB hydrate crystals in droplet are analyzed and the corresponding mathematical model is established. The results show that the induction time of hydrate nucleation can be effectively shortened by dropping droplets on the supercooled solid surface, and the rapid formation of hydrate can be promoted. The research provides a new method for solving the problem of large-scale industrial application of hydrates.

Key words: TBAB hydrate, droplet, rapid formation, visualization, dynamic model

摘要：

使用高速摄影技术对2 μl液滴中四丁基溴化铵（TBAB）水合物晶体的成核与生长进行了实验研究。对不同过冷度与不同浓度（10%，20%，30%，质量分数）的液滴中TBAB水合物晶体的生长特性进行了分析并建立了相应的数学模型，推导出TBAB水合物形成活化能E_a为-14.99 kJ/mol。研究结果表明，通过以液滴滴落过冷固体表面的方式可以有效缩短水合物成核的诱导时间，促进水合物的快速生成。为解决水合物在工业中大规模应用的难题提供了新方法。

关键词: TBAB水合物, 液滴, 快速生成, 可视化, 动力学模型

CLC Number:

TQ 028.8

LI Mengyang, GAO Ming, ZUO Qirong, ZHANG Lixin, ZHAO Yugang. Visualization investigation of TBAB hydrate formation in droplets on supercooled wall surfaces[J]. CIESC Journal, 2021, 72(4): 2094-2101.

李梦钖, 高明, 左启蓉, 章立新, 赵玉刚. 过冷壁面液滴中四丁基溴化铵水合物生成的可视化研究[J]. 化工学报, 2021, 72(4): 2094-2101.

Figures/Tables 7

Fig.1 Schematic diagram of experimental system

Fig.2 Morphology of hydrate growth in a 10% TBAB sessile droplet

Fig.3 Morphology of hydrate growth in a 20%TBAB sessile droplet

Fig.4 Morphology of hydrate growth in a 30%TBAB sessile droplet

Table 1 Average growth rate of hydrate crystals in different concentrations of TBAB droplets

过冷度/℃	10%TBAB晶体平均生长速率/(μm/s)	20%TBAB晶体平均生长速率/(μm/s)	30%TBAB晶体平均生长速率/(μm/s)
7	—	29.21	—
8	22.04	31.00	—
9	24.87	34.28	35.52
10	27.22	34.91	38.54
11	29.59	37.49	41.71
12	34.15	40.18	44.47

Fig.5 Variation of lnka with 1/Texp

Fig.6 Comparison of calculated and experimental results on crystal growth rate TBAB hydrate droplets

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