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固体表面上气体水合物向上生长及水迁移的动力学过程。

Kinetic process of upward gas hydrate growth and water migration on the solid surface.

作者信息

Liang Huiyong, Guan Dawei, Liu Yuda, Zhang Lunxiang, Zhao Jiafei, Yang Lei, Song Yongchen

机构信息

Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education, Dalian University of Technology, Dalian 116024, China; Ningbo Institute of Dalian University of Technology, Ningbo 315016, China.

Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education, Dalian University of Technology, Dalian 116024, China.

出版信息

J Colloid Interface Sci. 2022 Nov 15;626:1003-1014. doi: 10.1016/j.jcis.2022.07.024. Epub 2022 Jul 5.

Abstract

Gas hydrates have gained great interest in the energy and environmental field as a medium for gas storage and transport, gas separation, and carbon dioxide sequestration. The presence of small doses of surfactants in the aqueous phase has been reported to enhance hydrate formation; however, the underlying mechanisms remain poorly understood. Thus, in situ high-resolution X-ray computed tomography measurements were performed to monitor the upward water migration and the resulting hydrate nucleation and growth. It was found that the presence of hydrate crystals at the gas-liquid-solid contact line triggered the enhanced growth of hydrates on the reactor wall. A time delay was observed between the disappearance of the bulk water reservoir and its transformation into hydrate. The lower interfacial tension between the hydrate surface and the solution facilitated its adsorption onto the reactor wall once a thin film of hydrate nucleated on the solid wall surface. These hydrate layers present on the reactor wall were found to be porous, wherein the porosity decreased with increased subcooling. These fundamental results will be of value in understanding the mechanism of hydrate growth in the presence of surfactants and its potential application in hydrate-based technologies.

摘要

气体水合物作为气体储存与运输、气体分离及二氧化碳封存的介质,在能源和环境领域引起了极大关注。据报道,水相中存在少量表面活性剂可促进水合物形成;然而,其潜在机制仍知之甚少。因此,进行了原位高分辨率X射线计算机断层扫描测量,以监测向上的水迁移以及由此产生的水合物成核和生长。研究发现,气液固接触线处水合物晶体的存在引发了反应器壁上水合物的加速生长。在大量水库消失及其转化为水合物之间观察到了时间延迟。一旦在固体壁表面形成水合物薄膜,水合物表面与溶液之间较低的界面张力促进了其在反应器壁上的吸附。发现存在于反应器壁上的这些水合物层是多孔的,其中孔隙率随过冷度增加而降低。这些基础结果对于理解表面活性剂存在下水合物生长的机制及其在基于水合物的技术中的潜在应用具有重要价值。

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