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The mechanism and kinetics of oil shale pyrolysis in the presence of water

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Carbon Resources Conversion 2018年第2期1卷 160-164页

作者： Yue Ma shuyuan li State Key Laboratory of Heavy oil Processing College of ScienceChina University of PetroleumBeijing 102249China

The hydrous thermo-simulation experiments on oil shale sample from liushuhe basin have been performed using *** mechanism and kinetics of oil shale pyrolysis were *** formation mechanism of pyrolysates including retorting gas,oil and bitumen,were evaluated in the presence of saturated and unsaturated water,*** results show that the physicochemical properties of water have greatly changed in high temperature and *** the same time,water has three kinds of effect on the oil shale pyrolysis,including the protection of free radical,catalytic action and *** pyrolysis temperature was carried out about 70C earlier,and the generated processing of hydrocarbon would be easier under the *** consecutive first order reaction model involving bitumen as an intermediate product was used in the data analysis in order to determine the pyrolysis kinetic *** was found that the apparent activation energy of kerogen pyrolysis was lower than bitumen pyrolysis.

关键词： Oil shale Mechanism Free radicalreaction Carbocation reaction Kinetics Aqueous medium

Study of simulation experiments on the TSR system and its effect on the natural gas destruction

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Science China Earth Sciences 2005年第8期48卷 1197-1202页

作者： YUE Changtao li shuyuan DING Kangle ZHONG Ningning State Key Lab of Heavy Oil Processing University of Petroleum Beijing 102249 China State Key Lab of Heavy Oil Processing University of Petroleum Beijing 102249 China State Key Lab of Heavy Oil Processing University of Petroleum Beijing 102249 China State Key Lab of Heavy Oil Processing University of Petroleum Beijing 102249 China

The TSR process may be one of the reasons to result in the natural gas destruction in deep carbonate reservoirs. The work on this field has been the subject of much research in recent years. In this paper, thermal simulation experiments on the reaction of CH4-CaSO4 were carried out using autoclave at high temperature and high pressure. The products were charac-terized by some advanced analytical methods. The thermodynamics and kinetics were discussed and the reaction mechanism was investigated tentatively. It is found that the reaction can pro-ceed spontaneously to produce H2S, H2O and CaCO3 as the main products at the temperature range of 550―700℃ . The activation energy and geological reaction rate calculated from the ki-netic model can be compared with those from previous work. The results obtained in this paper can provide important information on the explanation of geochemical depth limit for natural gas and on the exploration of gas reservoirs.

关键词： natural gas destruction, TSR, simulation experiments, kinetics.

New concept on coal structure and new consideration for the generation mechanism of oil from coal

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Chinese Science Bulletin 1998年第24期43卷 2025-2035页

作者： Kuangzong Qin Shaohui Guo shuyuan li Univ Petr Beijing 100083 Peoples R China

The traditional two_phase structural model of coal based on the chemical covalence bonding has to be revised since recent discoveries of powerful mixed solvent such as CS-2/C-5H-9N, giving extra high yields in coal extraction at room temperature. It is believed that the physically associated interactions play important roles in the structure of coal. A composite model of coal is suggested. The organic matter of coal is mainly composed of some parts: the rigid 3_D macromolecules linked with chemical bonds; the polar molecules of high and moderate molecular weights, corresponding to asphaltenes and resins; the hydrocarbons with lower molecular weights. The polar molecules are associated by physical interactions (such as hydrogen bonding, charge transfer interactions, π_π interactions of aromatic sheets, etc.) each other and with macromolecules to form the network structure, in which some smaller nonpolar molecules are trapped. Based on the new concept of the composite coal model, some considerations for the generation mechanism of oil from coal have approached. Since the energy level of physical association is much lower than the chemical covalent bonding, the upper threshold of oil window for the generation of oil from coal seems not to be limited strictly after the theory of oil generation at the latter stage of the kerogen maturation. It looks reasonable to pay more attention to the geological conditions including the salt, water, minerals and environments of the sedimentation. The evolution process of physically associated interactions in the composite structure of coal and the generation of oil is thought to be intimately influenced by these factors.

关键词： Oil from coal coal structure generation mechanism of oil

Pyrolysis characteristics of a North Korean oil shale

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Petroleum Science 2014年第3期11卷 432-438页

作者： Wang Wei li shuyuan li linyue Ma Yue Yue Changtao He Jilai State Key Laboratory of Heavy Oil Processing China University of Petroleum Shandong Energy Long-kou Mining Group Co. Ltd.

Pyrolysis characteristics of a North Korean oil shale and its pyrolysates were investigated in this paper. The pyrolysis experiments were conducted below 600 ℃ at a heating rate of 10, 15, 20 and 25 ℃/min, respectively. The kinetics data were calculated using both integral and differential methods with the assumption of first order kinetics. The results show that the averaged oil content of the North Korean oil shale is about 12.1 wt% and its heat value is 13,400 kJ/kg. The oil yields at different retorting temperatures show that the higher the retorting temperature the greater the oil and retorting gas yields. The optimal retorting temperature for the North Korean oil shale is about 500 ℃. The properties of the North Korean shale oil including density, viscosity, flash point and freezing point are found to be relatively low compared with those of shale oil from FuShun, China. The gasoline fraction, diesel fraction and heavy oil fraction account for 11.5 wt%, 41.5 wt% and 47 wt%, respectively. The major pyrolysis gases are ca4 （the most abundant）, H2, CO2, H2S, CO, and C2-C5 hydrocarbons. The heat value of retorting gas is more than 900 kJ/mol, and the retorting gas has high sulfur content.

关键词： Shale oil pyrolysis properties oil shale retorting kinetics

A comparative study on characteristics of sulfur and nitrogen transformation and gaseous emission for combustion of bituminous coal and char

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Carbon Resources Conversion 2018年第1期1卷 86-93页

作者： Jili Hou Yue Ma shuyuan li Wenzhi Shang a State Key Laboratory of Heavy Oil Processing China University of Petroleum-BeijingBeijing 102249PR China Shenmu Sanjiang Coal Chemical Industry Co. Ltd.Shenmu 719300PR China

The characteristics of sulfur and nitrogen transformation and the emissions’comparison of sulfurous and nitrogenous gas were investigated using SEM,XPS,TG-FTIR and TG-gas analyzer during the combustion process of Shenmu bituminous coal(SM coal)and its *** indicated that porosity and specific surface area of char were enlarged after coal pyrolysis and a large amount of space could be provided for the oxidation reaction of various sulfur species with oxide during the combustion *** sulfur and nitrogen species of the two samples analyzed by XPS showed that,pyritic sulfur,organic sulfide sulfur,sulfone and sulfoxide sulfur in coal were partly transformed to thiophenic sulfur and sulfate sulfur in the pyrolysis of coal,and the total sulfur content in char was ***,the sulfur and nitrogen species’changes in SM coal,char and the ashes determined by XPS showed that sulfur fixation effect was enhanced in the presence of calcium oxide during *** component analysis of the gas during combustion via TG-FTIR indicated that SO2 and NO2 began to escape at 300C and reached maximum at about 1100C,by contrast,the emissions of SO2 and NO2 of char were below that of SM coal throughout the whole combustion *** wide range of TG-gas analyzer analysis revealed that the SO2 and NOx emissions of SM coal were 2.51 and 1.71 times as much as char burning,respectively.

关键词： Coal Char S/N Combustion Transformation XPS TG-FTIR

Simulation experiments on the reaction system of CH_4-MgSO_4-H_2O

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Chinese Science Bulletin 2008年第7期53卷 1071-1078页

作者： DING KangLe li shuyuan YUE ChangTao ZHONG NingNing State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 China Faculty of Natural Resource and Information Technology China University of Petroleum Beijing 102249 China

H2S-rich gas in carbonate reservoirs is usually attributed to thermochemical sulfate reduction (TSR). In this paper, thermal simulation experiments on the reaction system of CH4-MgSO4-H2O were carried out using autoclave at 425℃―525℃. The threshold temperature for initiating TSR is much lower than our previous studies (550 ℃ ). Properties of the reaction products were analyzed by microcoulometry, gas-chromatography (GC), Fourier transform-infrared spectrometry (FT-IR) and X-ray diffraction (XRD) methods. Thermodynamics and reaction kinetics of TSR processes were investigated on the basis of the experimental data. The results show that thermochemical reduction of magnesium sulfate with methane can proceed spontaneously to produce magnesium oxide, hydrogen sulfur, and carbon diox-ide as the main products, and high temperature is thermodynamically favorable to the reaction. Ac-cording to the reaction model, the calculated activation energy of TSR is 101.894 kJ/mol, which is lower than that by most previous studies. Mg2+ may have played a role of catalytic action in the process of TSR. The elementary steps of TSR and reaction mechanism were discussed tentatively. The study can provide important information on the explanation of geochemical depth limit for natural gas and on the generation of high H2S gas in deep carbonates reservoirs.

关键词：反作用系统 TSR 热化学化学反应

Reaction mechanism and kinetics of pressurized pyrolysis of Chinese oil shale in the presence of water

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Petroleum Science 2012年第4期9卷 532-534页

作者： FANG Chaohe li shuyuan MA Guili WANG Hongyan HUANG Zhilong China University of Petroleum ChangpingBeijing 102249China Research Institute of Petroleum Exploration and Development-Langfang Hebei 065007China Shenhua Ningxia Coal Industry Group Coal-Chemical Company Ningxia 951000China

A study of reaction mechanisms and chemical kinetics of pressurized pyrolysis of Chinese liushuhe oil shale in the presence of water were conducted using an autoclave for simulating and modeling in-situ underground thermal *** was found that the oil shale was first pyrolyzed to form pyrobitumen,shale oil,shale gas and residue,then the pyrobitumen was further pyrolyzed to form more shale oil,shale gas,and *** means that there are two consecutive and parallel *** increasing temperature,the pyrobitumen yield,as intermediate,first reached a maximum,then decreased to approximately *** kinetics results show that both these reactions are first *** activation energy of pyrobitumen formation from oil shale is lower than that of shale oil formation from pyrobitumen.

关键词： Oil shale pyrobitumen pressurized pyrolysis in-situ underground retorting reaction mechanism chemical kinetics

Study of CH_(4)and CO_(2)competitive adsorption on shale in Yibin,Sichuan Province of China

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Carbon Resources Conversion 2019年第1期2卷 35-42页

作者： Yue Ma Changtao Yue shuyuan li Xinyi Xu Yue Niu State Key Laboratory of Heavy Oil Processing College of ScienceChina University of PetroleumBeijing 102249China

Shale gas is an unconventional gas source with substantial development *** this study,Longmaxi Formation shale from the Silurian system in Yibin,Sichuan Province was collected for characterizing total organic carbon(TOC),clay mineral content,and other reservoir *** pore structure of shale was analyzed by field-emission scanning electron microscopy and low-temperature N_(2) adsorption–desorption *** adsorption experiments for CH_(4)and CO_(2)mixtures in shale samples were *** second Virial coefficient was used to calculate for the compressibility factor of the gas *** influencing factors of gas adsorption capacity of shale were ***,the CH_(4)and CO_(2)adsorption capacities and selection of shale samples were *** low pressure,the total gas mixture capacity of shale samples was positively correlated with *** the pressure increased to a certain extent,the growth trend of gas mixture adsorption capacity of shale samples *** mixed gas adsorption volume is high at 50℃ for all the *** the same temperature and pressure,the CO_(2)adsorption of shale samples is higher than the CH_(4)*** competitive adsorption,shale prefers to adsorb CO_(2).Therefore,CO_(2)is easier to be adsorbed by shale and this causes CH_(4)to be released from the adsorption site.

关键词： CH_(4) CO_(2) Competitive adsorption Second Virial coefficient

Heat Transfer and Kinetics Study of Moroccan Oil Shale Pyrolysis Process

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China Petroleum Processing & Petrochemical Technology 2021年第2期23卷 28-33页

作者： Zhan Chenyu Ma Yue Yue Changtao li shuyuan Tang Xun Wen Hua China University of Petroleum Beijing 102249 Beijing Guodian Longyuan Environmental Protection Engineering Co. Ltd.Beijing 102249

The basic properties of Moroccan oil shale were analyzed in this *** experiments at different heating rates were carried out by *** results show that the pyrolysis process of Moroccan oil shale can be divided into three steps.A shrink-nuclear model that considers the internal heat transfer of particles was established,which can better simulate the pyrolysis process of oil *** pyrolysis kinetic parameters of Moroccan oil shale were calculated based on heat transfer data and basic physical *** results show that the apparent activation energy of the reaction is around 120 kJ/mol,and the apparent frequency factor is around 2×10^(14) mol/(s•m^(2)).

关键词： kinetics oil shale pyrolysis shrink-nuclear model