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TBAB hydrate formation and growth in a microdevice under static and dynamic conditions

Petroleum Science 2024年第2期21卷 1396-1404页

作者： Xingxun Li Ming Liu Qingping Li Weixin Pang Guangjin Chen Changyu Sun State Key Laboratory of Heavy Oil Processing China University of Petroleum BeijingBeijing102249China State Key Laboratory of Natural Gas hydrate CNOOC Research Institute Co.Ltd.Beijing100027China

The natural gas hydrate has become one of the most promising future green energy sources on the earth.The natural gas hydrates mostly exist in the sediments with porous structure, so a solid understanding of the hydrate formation and growth processes in the porous medium is of significance for the exploitation of natural gas hydrate. The micro-packed bed device is one of the efficient microfluidic devices in the engineering field, but it has been rarely used for the hydrate-based research. In this study, a transparent micro-packed bed device filled with glass beads was developed to mimic the porous condition of sediments, and used to in-situ visualize the hydrate formation and growth habits in the pore spaces under both static and dynamic conditions. For the static experiment, two types of hydrate growth patterns in porous medium were observed and identified in the micro-packed bed device, which were the graincoating growth and pore-filling growth. For the dynamic condition, the hydrate formation, growth,distribution habits and hydrate blockage phenomena in the pore spaces were in-situ visually captured.The impacts of flowrate and subcooling on the pressure variation of the micro-packed bed and the duration of the hydrate growth under dynamic flow condition in pores were in-situ monitored and analyzed. The higher flowrate could result in the faster hydrate growth and more severe blockage in pores, but the effect of subcooling condition might be less significant at the high flowrate.

关键词： hydrate formation hydrate growth Microdevice In-situ measurement

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hydrate formation from liquid CO_(2) in a glass beads bed

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Chinese Journal of Chemical Engineering 2022年第3期35卷 185-191页

作者： Nan Li Jing-Yu Kan Chang-Yu Sun Guang-Jin Chen State Key Laboratory of Heavy Oil Processing China University of Petroleum-Beijing at KaramayKaramay 834000China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China

CO_(2)sequestration in marine sediments as solid hydrates is a potential way to capture and store anthropogenic CO_(2).In this study,hydrate formation from liquid CO_(2)in marine sediments was simulated in a glass beads bed,and the factors affecting the kinetics of hydrate formation were investigated.The results indicated that the rapid initial hydrate formation with a high driving force always increases the mass transfer resistance,which slows down hydrate growth.The final ratio of water conversion is higher under conditions of low temperature and higher pressure.A smaller particle size is conductive to initial CO_(2)hydrate growth,but the water conversion ratio in a bed with larger particles is slightly higher.Compared with other factors,the change in water saturation has an obvious effect on the final water conversion.To inhibit the initial hydrate formation during the injection process,in this paper,a kinetic inhibitor is proposed for pre-injection into marine sediments.This work shows that at a low pressure,a lowconcentration inhibitor has an obvious inhibition effect on hydrate growth.However,at a high pressure,it is necessary to increase the concentration of inhibitor to produce an obvious inhibition effect.

关键词： Liquid CO_(2) hydrate formation Sequestration Kinetic Water conversion

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Investigations on methane hydrate formation,dissociation,and viscosity in gas-water-sand system

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Petroleum Science 2022年第5期19卷 2420-2430页

作者： Shang-Fei Song Shun-Kang Fu Qing-Yun Liao Bo-Hui Shi Hong-Ju Chen Jing Gong State Key Laboratory of Natural Gas hydrates/National Engineering Laboratory for Pipeline Safety China University of PetroleumBeijing102249China PipeChina West East Pipeline Company Shanghai200122China Key Lab of Deepwater Engineering CNOOC Research InstituteBeijing100028China

Understanding the kinetics and viscosity of hydrate slurry in gas-water-sand system is of great significance for the high-efficiency and high-safety development of natural gas hydrates.The effect of micronsized sands with various concentrations and particle sizes on the hydrate formation,dissociation,and viscosity in gas-water-sand system are investigated in this work.The experimental results show that the hydrate induction time in the sandy system is slightly prolonged compared to the pure gas-water system,and the inhibition effect first strengthens and then weakens as the sand concentration increases from0 wt%to 5 wt%.Besides,the difference of hydrate formation amount in various cases is not obvious.The concentration and particle size of sand have little effect on the kinetics of hydrate formation.Both promoting and inhibiting effects on hydrate formation have been found in the sandy multiphase fluid.For the viscosity characteristics,there are three variations of hydrate slurry viscosity during the formation process:Steep drop type,S-type and Fluctuation type.Moreover,appropriate sand size is helpful to reduce the randomness of slurry viscosity change.Meanwhile,even at the same hydrate volume fraction,the slurry viscosity in the formation process is significantly higher than that in dissociation process,which needs further research.This work provides further insights of hydrate formation,dissociation,and viscosity in gas-water-sand system,which is of great significance for safe and economic development of natural gas hydrates.

关键词： hydrate slurry Micron-sized sands hydrate formation hydrate dissociation Viscosity characteristics

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Relation between soil matrix potential changes and water conversion ratios during methane hydrate formation processes in loess

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Journal of Natural Gas Chemistry 2011年第2期20卷 140-144页

作者： Peng Zhang Qingbai Wu Guanli Jiang Yibin Pu State Key Laboratory of Frozen Soil Engineering Cold and Arid Regions Environmental and Engineering Research Institute Chinese Academy of Sciences Lanzhou 730000 Gansu China

Abstract With a new apparatus designed and assembled by ourselves, the matrix potential of non-saturated loess was firstly measured and studied during methane hydrate formation processes. The experimental results showed that during two formation processes, the matrix potential changes of the loess all presented a good linear relationship with water conversion ratios. In addition, although it was well known that the secondary gas hydrate formation was easier than the initial, our experimental results showed that the initial hydrate formation efficiency in non-saturated loess was higher than that of the secondary.

关键词： hydrate formation non-saturated loess matrix potential water conversion ratio

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Experimental study on characteristics of pore water conversion during methane hydrates formation in unsaturated sand

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China Geology 2022年第2期5卷 276-284页

作者： Yun-kai Ji Chang-ling Liu Zhun Zhang Qing-guo Meng Le-le Liu Yong-chao Zhang Neng-you Wu Key Laboratory of Gas hydrate Ministry of Natural ResourcesQingdao Institute of Marine GeologyQingdao 266237China Laboratory for Marine Mineral Resources Pilot National Laboratory for Marine Science and TechnologyQingdao 266237China Faculty of Engineering China University of GeosciencesWuhan 430074China

Understanding the pore water conversion characteristics during hydrate formation in porous media is important to study the accumulation mechanism of marine gas hydrate.In this study,low-field NMR was used to study the pore water conversion characteristics during methane hydrate formation in unsaturated sand samples.Results show that the signal intensity of T_(2) distribution isn’t affected by sediment type and pore pressure,but is affected by temperature.The increase in the pressure of hydrogen-containing gas can cause the increase in the signal intensity of T_(2) distribution.The heterogeneity of pore structure is aggravated due to the hydrate formation in porous media.The water conversion rate fluctuates during the hydrate formation.The sand size affects the water conversion ratio and rate by affecting the specific surface of sand in unsaturated porous media.For the fine sand sample,the large specific surface causes a large gas-water contact area resulting in a higher water conversion rate,but causes a large water-sand contact area resulting in a low water conversion ratio(C_(w)=96.2%).The clay can reduce the water conversion rate and ratio,especially montmorillonite(C_(w)=95.8%).The crystal layer of montmorillonite affects the pore water conversion characteristics by hindering the conversion of interlayer water.

关键词： Porous media Unsaturated sand Methane hydrates Low-field NMR Pore water conversion hydrate formation NGHs exploration trial engineering Oil and gas exploration engineering Shenhu area South China Sea

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Molecular simulation studies on natural gas hydrates nucleation and growth:A review

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China Geology 2022年第2期5卷 330-344页

作者： Zheng-cai Zhang Neng-you Wu Chang-ling Liu Xi-luo Hao Yong-chao Zhang Kai Gao Bo Peng Chao Zheng Wei Tang Guang-jun Guo Laboratory for Marine Mineral Resources Pilot National Laboratory for Marine Science and TechnologyQingdao 266071China The Key Laboratory of Gas hydrate Ministry of Natural ResourcesQingdao Institute of Marine GeologyQingdao 266071China Key Laboratory of Petroleum Resource Research Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China

How natural gas hydrates nucleate and grow is a crucial scientific question.The research on it will help solve practical problems encountered in hydrate accumulation,development,and utilization of hydrate related technology.Due to its limitations on both spatial and temporal dimensions,experiment cannot fully explain this issue on a micro-scale.With the development of computer technology,molecular simulation has been widely used in the study of hydrate formation because it can observe the nucleation and growth process of hydrates at the molecular level.This review will assess the recent progresses in molecular dynamics simulation of hydrate nucleation and growth,as well as the enlightening significance of these developments in hydrate applications.At the same time,combined with the problems encountered in recent hydrate trial mining and applications,some potential directions for molecular simulation in the research of hydrate nucleation and growth are proposed,and the future of molecular simulation research on hydrate nucleation and growth is prospected.

关键词： Natural gas hydrates Methane hydrate Molecular simulations hydrate nucleation hydrate growth hydrate formation Nucleation theory NGHs exploration trial engineering Oil and gas exploration engineering

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Synergistic effect of combination of surfactant and oxide powder on enhancement of gas hydrates nucleation

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Journal of Energy Chemistry 2017年第4期26卷 808-814页

作者： Anatoliy N.Nesterov Aleksey M.Reshetnikov Andrey Yu.Manakov Tatyana P.Adamova Institute of Earth’s Cryosphere SB RAS Malygina str.86Tyumen 625026Russian Federation Tyumen State University Volodarskogo Str.6Tyumen 625003Russian Federation Tyumen Industrial University Volodarskogo Str.38Tyumen 625000Russian Federation Nikolaev Institute of Inorganic Chemistry SB RAS Lavrentieva ave.3Novosibirsk 630090Russian Federation Novosibirsk State University Pirogova Str.2Novosibirsk 630090Russian Federation

In the present work we studied the induction periods of hydrate formation of natural gas in pure water, aqueous solutions of surfactants, and in the presence of surfactant together with aluminum oxide nanopowder, the activity of which as hydrate formation inducer was studied previously. Sodium dodecyl sulfate（SDS） or neonol AF-9-12 were used as the surfactants. It was demonstrated that the addition of either surfactants or aluminum oxide powder under our experimental conditions causes a decrease in the induction period of hydrate formation from;05 min for pure water to 30–35 min for water with additives. In the case of the simultaneous presence of surfactants and aluminum oxide powder in the system, induction period decreased to;0 min. So, the synergistic effect of the combination of surfactant and oxide powder on gas hydrate nucleation was demonstrated. Possible reasons of this effect have been discussed.

关键词： Gas hydrate hydrate formation Nucleation Induction period Surfactant Nanopowder

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Experimental study on geochemical characteristic of methane hydrate formed in porous media

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Journal of Natural Gas Chemistry 2009年第2期18卷 217-221页

作者： Qiang Chen Changling Liu Yuguang Ye Qingdao Institute of Marine Geology the Ministry of Land and Resources Qingdao 266071 Shandong China The key Laboratory of Marine Hydrocarbon Resources and Environment Resources the Ministry of Land and Resources Qingdao 266071 Shangdong China

The natural occurrence of methane hydrates in marine sediments has been intensively studied over the past decades, and geochemical charac-teristic of hydrate is one of the most attractive research fields. In this paper, we discussed the geochemical anomaly during hydrate formation in porous media. By doing so, we also investigated the temperature influence on hydrate formation under isobaric condition. It turns out that sub-cooling is an important factor to dominate hydrate formation. Larger subcooling provides more powerful driving force for hydrate formation. During the geochemical anomaly research, six kinds of ions and the total dissolved salt （TDS） were measured before and after the experiment in different porous media. The result is that all kinds of ionic concentration increased after hydrate formation which can be defined as salting out effect mainly affected by gas consumption. But the variation ratio of different ions is not equal. Ca^2＋ seems to be the most significantly influenced one, and its variation ratio is up to 80%. Finally, we theoretically made a model to calculate the TDS variation, the result is in good accordance with measured one, especially when gas consumption is large.

关键词： hydrate formation porous media subcooling salting out effect geochemical anomaly

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