Three-Scale in Situ Investigation on the Film Morphology and Mass Transfer Channels during the Thickening Growth of Hydrates on Gas Bubble

Three-Scale in Situ Investigation on the Film Morphology and Mass Transfer Channels during the Thickening Growth of Hydrates on Gas Bubble
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气泡上水合物增稠生长过程中膜形貌和传质通道的三尺度原位研究

DOI:
10.1021/acs.cgd.8b01847
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发表时间:
2019
影响因子:
3.8
通讯作者:
Guang-Jin Chen
Guang-Jin Chen
中科院分区:
化学2区
文献类型:
--
作者:
Xin-Yang Zeng;Guozhong Wu;Jin-Rong Zhong;Dao-Yi Chen;Chang-Yu Sun;Guang-Jin Chen

文献摘要

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提出了一种结合光学显微镜、共焦显微镜和拉曼光谱的三尺度原位观测技术,以深入了解悬浮在水中的气泡上形成的水合物膜的增厚生长动力学。研究了由纯CH4或CH4和C2H6混合物形成的水合物膜在增稠生长过程中的形态和传质通道的演变。结果表明,水合物膜在增厚生长过程中的形态演化取决于横向生长过程中水合物膜的初始形态。SiCH4和SiCH4-C2H6水合物具有相同的最终形态(例如,大量定义良好的多面体颗粒水合物),而SiCH4-C2H6水合物看起来呈块状。结果表明,随着水合物膜的生长,水合物膜上的气孔逐渐消失,表明水合物膜上的主要传质通道由气孔向晶格转变。
A three-scale in situ observation technique combining the optical microscope, confocal microscope, and Raman spectroscopy was proposed to gain insights into the thickening growth kinetic of hydrate film formed on a gas bubble suspended in water. The evolution of the morphology and mass transfer channels of the hydrate films formed from pure CH4 or the mixture of CH4 and C2H6 during thickening growth was investigated. Results demonstrated that the morphological evolution of hydrate films during thickening growth depended on the initial morphology of the hydrate film formed in the lateral growth. The sI CH4 and sI CH4–C2H6 hydrates had the same ultimate morphology (e.g., a large number of well-defined polyhedral granular hydrates), while the sII CH4–C2H6 hydrates appeared massive. It was clearly observed that the gas pores on the hydrate film gradually vanished with the growth of hydrate film, which suggested that the predominant mass transfer channels on the film changed from the gas pores to the lattices....