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Geochemical modeling to aid experimental design for multiple isotope tracer studies of coupled dissolution and precipitation reaction kinetics

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Acta Geochimica 2024年第1期43卷 1-15页

作者： Mingkun Chen Peng Lu yongchen song Chen Zhu Department of Earth and Atmospheric Sciences Indiana UniversityBloomingtonIN 47405USA School of Energy and Power Engineering Dalian University of TechnologyDalian 116024China EXPEC Advanced Research Center Saudi Aramco31311 DhahranSaudi Arabia

It is a challenge to make thorough but efficient experimental designs for the coupled mineral dissolution and precipitation studies in a multi-mineral system, because it is difficult to speculate the best experimental duration, optimal sampling schedule, effects of different experimental conditions, and how to maximize the experimental outputs prior to the actual experiments. Geochemical modeling is an efficient and effective tool to assist the experimental design by virtually running all scenarios of interest for the studied system and predicting the experimental outcomes. Here we demonstrated an example of geochemical modeling assisted experimental design of coupled labradorite dissolution and calcite and clayey mineral precipitation using multiple isotope tracers. In this study, labradorite(plagioclase) was chosen as the reactant because it is both a major component and one of the most reactive minerals in basalt. Following our isotope doping studies of single minerals in the last ten years, initial solutions in the simulations were doped withmultiple isotopes(e.g., Ca and Si). Geochemical modeling results show that the use of isotope tracers gives us orders of magnitude more sensitivity than the conventional method based on concentrations and allows us to decouple dissolution and precipitation reactions at near-equilibrium condition. The simulations suggest that the precise unidirectional dissolution rates can inform us which rate laws plagioclase dissolution has followed. Calcite precipitation occurred at near-equilibrium and the multiple isotope tracer experiments would provide near-equilibrium precipitation rates, which was a challenge for the conventional concentration-based experiments. In addition, whether the precipitation of clayey phases is the rate-limiting step in some multi-mineral systems will be revealed. Overall, the modeling results of multimineral reaction kinetics will improve the understanding of the coupled dissolution–precipitation in the multi-mineral systems and the quality of geochemic

关键词： Kinetics Feldspar Isotope doping Near-equilibrium CO_(2)sequestration Basalt

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Numerical study on gas production via a horizontal well from hydrate reservoirs with different slope angles in the South China Sea

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Deep Underground Science and Engineering 2024年第2期3卷 171-181页

作者： Tingting Luo Jianlin song Xiang Sun Fanbao Cheng Madhusudhan Bangalore Narasimha Murthy Yulu Chen Yi Zhao yongchen song School of Mechanics and Civil Engineering China University of Mining and TechnologyXuzhouChina Institute of Rock and Soil Mechanics Chinese Academy of SciencesWuhanChina Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of TechnologyDalianChina Faculty of Engineering and the Environment University of SouthamptonSouthamptonUK

It is important to study the effect of hydrate production on the physical and mechanical properties of low-permeability clayey–silty reservoirs for the largescale exploitation of hydrate reservoirs in the South China Sea.In this study,a multiphysical-field coupling model,combined with actual exploration drilling data and the mechanical experimental data of hydrate cores in the laboratory,was established to investigate the physical and mechanical properties of low-permeability reservoirs with different slope angles during 5-year hydrate production by the depressurization method via a horizontal well.The result shows that the permeability of reservoirs severely affects gas production rate,and the maximum gas production amount of a 20-m-long horizontal well can reach186.8 m3/day during the 5-year hydrate production.Reservoirs with smaller slope angles show higher gas production rates.The depressurization propagation and hydrate dissociation mainly develop along the direction parallel to the slope.Besides,the mean effective stress of reservoirs is concentrated in the near-wellbore area with the on-going hydrate production,and gradually decreases with the increase of the slope angle.Different from the effective stress distribution law,the total reservoir settlement amount first decreases and then increases with the increase of the slope angle.The maximum settlement of reservoirs with a 0°slope angle is up to 3.4 m,and the displacement in the near-wellbore area is as high as2.2 m after 5 years of hydrate production.It is concluded that the pore pressure drop region of low-permeability reservoirs in the South China Sea is limited,and various slope angles further lead to differences in effective stress and strain of reservoirs during hydrate production,resulting in severe uneven settlement of reservoirs.

关键词： effective stress low‐permeability reservoirs natural gas hydrate production numerical simulation settlement slope angle the South China

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A large-scale experimental simulator for natural gas hydrate recovery and its experimental applications

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Petroleum 2023年第4期9卷 607-612页

作者： Yang Ge Qingping Li Xin Lv Mingqiang Chen Bo Yang Benjian song Jiafei Zhao yongchen song State Key Laboratory of Natural Gas Hydrates Beijing100028China Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of TechnologyDalian116024China China National Offshore Oil Corporation Research Institute Co.Ltd Beijing100028China

To facilitate the recovery of natural gas hydrate(NGH)deposits in the South China Sea,we have designed and developed the world's largest publicly reported experimental simulator for NGH recovery.This system can also be used to perform CO_(2) capture and sequestration experiments and to simulate NGH recovery using CH_(4)/CO_(2) replacement.This system was used to prepare a shallow gas and hydrate reservoir,to simulate NGH recovery via depressurization with a horizontal well.A set of experimental procedures and data analysis methods were prepared for this system.By analyzing the measurements taken by each probe,we determined the temperature,pressure,and acoustic parameter trends that accompany NGH recovery.The results demonstrate that the temperature fields,pressure fields,acoustic characteristics,and electrical impedances of an NGH recovery experiment can be precisely monitored in real time using the aforementioned experimental system.Furthermore,fluid production rates can be calculated at a high level of precision.It was concluded that(1)the optimal production pressure differential ranges from 0.8 to 1.0 MPa,and the wellbore will clog if the pressure differential reaches 1.2 MPa;and(2)during NGH decomposition,strong heterogeneities will arise in the surrounding temperature and pressure fields,which will affect the shallow gas stratum.

关键词： Natural gas hydrate(NGH) Experimental NGH recovery simulator Recovery by depressurization Wellbore clogging Shallow gas

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Turning gas hydrate nucleation with oxygen-containing groups on size-selected graphene oxide flakes

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Journal of Energy Chemistry 2023年第12期87卷 351-358,I0009页

作者： Huiquan Liu Changrui Shi Zherui Chen Shuai Wang Mingjun Yang Jiafei Zhao Cong Chen yongchen song Zheng Ling Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education School of Energy&Power EngineeringDalian University of TechnologyDalian 116024LiaoningChina Ningbo Institute of Dalian University of Technology Ningbo 315016ZhejiangChina

Gas hydrate is a promising alternative for gas capture and storage due to its high gas storage capacity achieved with only structured water molecules.Nucleation is the critical controlling step in gas hydrate formation.Adding an alien solid surface is an effective approach to regulate gas hydrate nucleation.However,how the solid surface compositions control the gas hydrate nucleation remains unclear.Benefiting from the fact that the surface compositions of graphene oxide(GO)can be finely tuned,we report the effect of functional groups of size-selected GO flakes on methane hydrate nucleation.The carbonyl and carboxyl of GO flakes showed a more prominent promotion for methane hydrate nucleation than the hydroxyl of GO flakes.Surface energy,zeta potential,Raman spectra,and molecular dynamics simulation analysis were used to reveal the regulation mechanism of the functional groups of size-selected GO flakes on methane hydrate nucleation.The GO flakes with abundant carbonyl and carboxyl exhibited higher charge density than those enriched in hydroxyl.The negatively charged GO flakes can induce water molecules to form an ordered hydrogen-bonded arrangement via charge-dipole interactions.Therefore,the water molecules surrounding the carboxyl and carbonyl showed a more ordered hydrogen-bonded structure than those around the hydroxyl of GO flakes.The ordered water arrangement,similar to methane hydrate cages,significantly accelerated methane hydrate nucleation.Our study shows how the surface chemistry of solids control gas hydrate nucleation and sheds light on the design of effective heterogeneous nucleators for gas hydrate.

关键词： Methane hydrate Methane storage Energy storage Surface energy Hydrogen-bonded water

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A review of the gas hydrate phase transition with a microfluidic approach

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能源评论(英文) 2023年第1期2卷 1-15页

作者： Qingbin Liu Yingying Liu Jintao Xu Ying Teng Zheng Ling Yi Zhang Lanlan Jiang yongchen song Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of TechnologyDalian116024China Shenzhen Key Laboratory of Deep Engineering Sciences and Green Energy Institute of Deep Earth Sciences and Green EnergyCollege of Civil and Transportation EngineeringShenzhen UniversityShenzhen518060China Guangdong Provincial Key Laboratory of Deep Earth Sciences and Geothermal Energy Exploitation and Utilization Shenzhen UniversityShenzhen518060China

Over the years,natural gas hydrates(NGHs)have attracted significant attention as an emerging energy resource.Microfluidics is a novel technology used to observe the behaviour of NGHs in microchannels directly and has been applied to hydrates.Gas hydrate distributions and phase transitions are key parameters for exploitation and application.In this paper,advances in related research with microfluidics-based technology are reviewed,including the hydrate phase transition process and its mechanism of influence.Hydrate formation and decomposition directly influence the efficiency and sustainability of exploitation.In addition,studies of the hydrate phase transition provide basic data for future commercial exploitation.Moreover,extended applications,further developments and potential improvements in microfluidic techniques are also discussed.We believe that with an improved understanding of the hydrate phase transition mechanism,commercial exploitation of hydrates can be expected soon.

关键词： Clathrate hydrate Microfluidics Morphology Experimental CO_(2)sequestration

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An improved model for predicting hydrate phase equilibrium in marine sediment environment

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Journal of Natural Gas Chemistry 2010年第3期19卷 241-245页

作者： yongchen song Mingjun Yang Yongjun Chen Qingping Li Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of Technology Dalian 116024 Liaoning China CNOOC Research Center Beijing 100027 China

Based on the models of hydrate phase equilibrium in bulk water and porous media, an improved model was proposed to predict the methane hydrate equilibrium in marine sediment environment. In the suggested model, mechanical equilibrium of force between the interfaces in hydrate-liquid-vapor system was considered. When electrolyte was present in pore water, interfacial energy between hydrate and liquid was corrected by an equation that is expressed as the function of temperature and electrolyte concentration. The activity of water is calculated based on the Pitzer model and the interfacial energy between liquid and gas is solved using the Li method. The prediction results show good agreement with the experimental data. By comparison with other models, it is proved that this model can improve the accuracy for predicting hydrate phase equilibrium in marine sediment environment.

关键词： hydrate equilibrium interfacial energy marine sediment

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Numerical studies of hydrate dissociation and gas production behavior in porous media during depressurization process

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Journal of Natural Gas Chemistry 2012年第4期21卷 381-392页

作者： Xuke Ruan Mingjun Yang yongchen song Haifeng Liang Yanghui Li Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of TechnologyDalian 116023LiaoningChina College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina

In this study, a numerical model is developed to investigate the hydrate dissociation and gas production in porous media by depressurization. A series of simulation runs are conducted to study the impacts of permeability characteristics, including permeability reduction exponent, absolute permeability, hydrate accumulation habits and hydrate saturation, sand average grain size and irreducible water saturation. The effects of the distribution of hydrate in porous media are examined by adapting conceptual models of hydrate accumulation habits into simulations to govern the evolution of permeability with hydrate decomposition, which is also compared with the conventional reservoir permeability model, i.e. Corey model. The simulations show that the hydrate dissociation rate increases with the decrease of permeability reduction exponent, hydrate saturation and the sand average grain size. Compared with the conceptual models of hydrate accumulation habits, our simulations indicate that Corey model overpredicts the gas production and the performance of hydrate coating models is superior to that of hydrate filling models in gas production, which behavior does follow by the order of capillary coating〉pore coating〉pore filling〉capillary filling. From the analysis of tl/2, some interesting results are suggested as follows：（1） there is a ＂switch＂ value （the ＂switch＂ absolute permeability） for laboratory-scale hydrate dissociation in porous media, the absolute permeability has almost no influence on the gas production behavior when the permeability exceeds the ＂switch＂ value. In this study, the ＂switch＂ value of absolute permeability can be estimated to be between 10 and 50 md. （2） An optimum value of initial effective water saturation Sw,e exists where hydrate dissociation rate reaches the maximum and the optimum value largely coincides with the value of irreducible water saturation Swr,e. For the case of Sw,e〈,Swr,e, or Sw,e〉Swr,e, there are different control mechanisms dominating the process of hydrate dissociation and ga

关键词： gas hydrate numerical simulation permeability dissociation gas production depressurization

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The detection of tetrahydrofuran hydrate formation and saturation using magnetic resonance imaging technique

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Journal of Natural Gas Chemistry 2010年第3期19卷 224-228页

作者： Yu Liu yongchen song Yongjun Chen Lei Yao Qingping Li Key Lab of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of Technology Dalian 116024 Liaoning China Research Center of China National Offshore Oil Corporation Beijing 100027 China

Tetrahydrofuran（THF） hydrate was formed in bulk as well as in glass beads pack with a mean diameter of 3.0 mm by controlling the temperature under ambient pressure.Images of THF hydrate formation procedure were obtained using the magnetic resonance imaging（MRI） technique.The experiment results showed that MRI is an effective method for the detection of hydrate formation.Saturation of hydrate formed both in bulk and glass beads can be confirmed by intensity integration of MRI images.

关键词： tetrahydrofuran hydrate magnetic resonance imaging glass beads saturation

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Adsorption isotherms and kinetic characteristics of methane on block anthracite over a wide pressure range

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Journal of Energy Chemistry 2015年第2期24卷 245-256页

作者： Wanli Xing yongchen song Yi Zhang Weiguo Liu Lanlan Jiang Yanghui Li Yuechao Zhao Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education School of Energy and Power Engineering Dalian University of Technology

It is important to quantitatively understand the methane adsorption and transport mechanism in coal for an evaluation of the reserves and for its production forecast. In this work, a block coal sample was chosen to perform the CH_4 adsorption experiments using the gravimetric method at temperatures of 293.60 K, 311.26 K, 332.98 K and 352.55 K and pressures up to 19 MPa. The excess adsorption capacity of CH_4 in dry block anthracite increased, followed by a sequence decrease with the increasing pressure. High temperature restrained the growth of the excess adsorption due to that the adsorption is an intrinsically physical and exothermic process. The excess adsorption peak decreased slowly with the increase of temperature and intersected at a pressure of more than 18 MPa; meanwhile, the pressure at the excess adsorption peak increased. The existing correlations were exanfined in terms of density rather than pressure. The DR＋k correlation, with an average relative deviation of 4-0.51%, fitted our data better than the others, with an average relative deviation of up to 2.29%. The transportation characteristics of CH_4 adsorption was also investigated in this study, including the adsorption rate and diffusion in block coal. The kinetic data could be described by a modified unipore model. The adsorption rates were found to exhibit dependence on pressure and temperature at low pressures, while the calculated diffusivities exhibited little temperature dependence. In addition, the kinetic characteristics were compared between CH_4 and CO_2 adsorption on the block coal. The excess adsorption ratios of CO_2 to CH_4 obtained from the DR＋k model decreased with the increasing pressure.

关键词： adsorption isotherm thermodynamic model adsorption rate diffusion

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Water permeability in MXene membranes: Process matters

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Chinese Chemical Letters 2020年第6期31卷 1665-1669页

作者： Hang Zhou Yuwei Wang Fuqiang Wang Hao Deng yongchen song Changping Li Zheng Ling Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education School of Energy&Power EngineeringDalian University of TechnologyDalian 116024China Research Center for Eco-Environmental Engineering Dongguan University of TechnologyDongguan 523808China

Recent studies have shown impressive transport behaviors of water and ions within lamellar MXene membranes,which endows great promise in developing advanced separation application based high performance MXene membranes.However,most of the researches focused on modification of MXene nanoflakes and optimizing interlayer distance,leaving the impact of membrane fabrication process marginal.In this work,we studied the water flux of membranes made by vacuum filtration using delaminated MXene nanoflakes as the building-blocks.Our results show that the water permeability is extremely sensitive to the process,especially at the drying process,loading and deposit rate of nanoflakes(the feeding concentration).We find that the voids from less ordered stack rather than in-plane defects and interlayer galleries contribute to the large water permeability.The voids can be effectively avoided via deposition of MXene nanoflakes at a slow rate.Manipulating the stack of MXene nanoflakes during vacuum filtration and drying are critical for development of MXene membranes with desired performance for water permeation.

关键词： Exfoliation MXene Two-dimensional materials Water permeability Water treatment

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