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kerogen Kinetic Distributions and Simulations Provide Insights into Petroleum Transformation Fraction (TF) Profiles of Organic-Rich Shales

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Journal of Earth Science 2024年第3期35卷 747-757页

作者： David A.Wood DWA Energy Limited Lincoln LN59JPUnited Kingdom

Two hundred and fifty single first-order Arrhenius reactions are simulated to generate S2 pyrograms at three heating rates 25,15,and 5°C·min-1.The activation energy(E)and pre-exponential factor(A)of the reactions simulated follow a long-established trend of those variable values displayed by shales and kerogens.The characteristics of the transformation fraction(TF)profiles(product generation window temperatures)of the simulated single reactions are compared to the TF profiles of recorded shale pyrograms generated by multiple reactions with different E-A values lying near the defined E-A trend.Important similarities and differences are observed between the TF profile values of the two datasets.The similarities support the spread of E-A values involved in shale pyrogram best fits.The differences are most likely explained by the complexity of the multiple kerogen first-order and second-order reactions contributing to the recorded shale pyrograms versus the simplicity and crispness of the single first-order reactions simulated.The results also justify the validity of using the previously described“variable E-A pyrogram-fitting method”of multi-heating-rate shale pyrograms enabling optimizers to choose multiple reactions from an unlimited range of E-A values.In contrast,further doubt is cast on the validity of the constant-A pyrogram-fitting method used by the Easy%Ro technique,in that a distribution of reactions with a single A value is unlikely to represent the complex variety of kerogen macerals observed in shale formations.TF profiles generated by the variable E-A pyrogram-fitting method lie close to the established E-A trend and are likely to provide more realistic TF generation window temperatures than TF profiles generated by the constant-A pyrogram-fitting method.

关键词： transformation fraction profiles simulated S2 pyrograms multiple heating rates kerogen/shale kinetics S2 pyrogram fitting techniques kerogen petroleum research.

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Geochemical prerequisites for the formation of oil and gas accumulation zones in the South Turgay basin,Kazakhstan

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Acta Geochimica 2024年第3期43卷 520-534页

作者： Rima Kopbosynkyzy Madisheva Vassiliy Sergeevich Portnov Gulmadina Bulatovna Amangeldiyeva Akmaral Bakhytbekovna Demeuova Yessimkhan Sherekhanovich Seitkhaziyev Dulat Kalimovich Azhgaliev Department Geology and Exploration of Mineral Deposits Abylkas Saginov Karaganda Technical University NPJSCKaragandaRepublic of Kazakhstan Laboratory of Geochemical Studies of Oil Water and RockAtyrauRepublic of Kazakhstan Geological and Mineralogical Sciences Atyrau University of Oil and Gas Named After SafiUtebayevAtyrauRepublic of Kazakhstan

This study predicts favorable oil and gas source-rock formation conditions in the Aryskum Depression of the South Turgay Basin,Kazakhstan.This study assesses the thermal maturity and characteristics of organic matter by determining its environmental conditions using data from geochemical analysis of core(pyrolysis)and oil(biomarkers and carbon isotopic compositions)samples.According to the geochemical parameters obtained by pyrolysis,the oil generation potential of the original rocks of most studied samples varies from poor to rich.The facies–genetic organic matter is predominantly humic and less frequently humus–sapropel,indicating organic matter accumulation in the studied samples were under moderately reducing conditions(kerogenⅢand Ⅱ types)and coastal–marine environments(kerogen typeⅠ).The carbon isotopic compositions of oils derived from the Jurassic deposits of the Aryskum Depression also indicate the sapropelic and mixed humic–sapropelic type of organic matter(kerogenⅡandⅠ).Biomarker analysis of oils indicates original organic matter formation in an anoxic environment.

关键词： South Turgay Basin Oil and gas potential Source rock Organic matter kerogen

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Biodegradation of occluded hydrocarbons and kerogen macromolecules of the Permian Lucaogou shales,Junggar Basin,NW China

能源地球科学(英文)

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能源地球科学(英文) 2023年第1期4卷 179-184页

作者： Yan'e Chen Longlong Li Zhirong Zhang Paul F.Greenwood Yumin Liu Wuxi Branch of SINOPEC Petroleum Exploration and Development Research Institute WuxiJiangsu214126China SINOPEC Key Laboratory of Petroleum Accumulation Mechanisms WuxiJiangsu214126China Hubei Key Laboratory of Petroleum Geochemistry and Environment Yangtze UniversityWuhanHubei430100China School of Earth Sciences University of Western AustraliaCrawleyWA6009Australia Western Australia Organic and Isotope Geochemistry Centre School of Earth and Planetary SciencesCurtin UniversityGPO Box U1987PerthWA6845Australia Hubei Key Laboratory of Petroleum Geochemistry and Environment(Yangtze University) Yangtze UniversityWuhan430100China

Three kerogen samples(JJZG-1,JJZG-2 and JJZG-3)isolated from the Permian Lucaogou shales of varying biodegradation levels(BLs≈0,3 and 7,respectively)were subjected to sequential stepwise pyrolysis combined with on-line detection of gas chromatography-mass spectrometry(GC-MS).Occluded fractions(bitumenⅡ)released at low-temperature steps(≥410℃)show consistent biodegradative signatures with that reported for solvent-extracted fractions(bitumenⅠ)of the original shales,e.g.,broad range of abundant n-alkanes,isoprenoids and regular hopanes for the non-biodegraded JJZG-1;trace n-alkanes and abundant hopanes for the moderately biodegraded JJZG-2;and no n-alkanes but still prominent hopanes including the microbially produced 25-nohopanes for the severely biodegraded JJZG-3.This consistency between bitumenⅡand bitumenⅠfractions indicates the biodegradability of the kerogenoccluded bitumenⅡwith limited protection from host kerogen.A minor level of protection was suggested by the trace distribution of n-alkanes in the bitumenⅡof JJZG-2,whereas the bitumenⅠhad no nalkanes.The kerogen itself was more resistant to biodegradation as reflected by the persistence of high abundances of both n-alkanes and hopanes in the high temperature(≥460℃)products of all three kerogen samples.However,the relative abundances of these product groups did show some evidence of biodegradation alteration,e.g.,ratios of n-C_(15)alkene/C_(27)hop-17(21)-ene at 510℃pyrolysis decreased by order of magnitude from the non-biodegraded(JJZG-1=27.4)to highly biodegraded(0.3 for JJZG-3)samples.The reduced biodegradation impact on the kerogen fraction(Cf.bitumen fractions)was also evident by the absence of 25-norhopanes in the high-temperature analysis of the JJZG-3 kerogen.

关键词： Biodegradation Stepwise pyrolysis Occluded hydrocarbon BitumenⅡ kerogen Source rock Permian Lucaogou shale Junggar Basin

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Molecular insight into the oil displacement mechanism of CO_(2) flooding in the nanopores of shale oil reservoir

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Petroleum Science 2023年第6期20卷 3516-3529页

作者： Xiao-Hu Dong Wen-Jing Xu Hui-Qing Liu Zhang-Xing Chen Ning Lu State Key Laboratory of Petroleum Resources and Engineering China University of PetroleumBeijing102249China MOE Key Laboratory of Petroleum Engineering China University of PetroleumBeijing102249China Department of Chemical and Petroleum Engineering University of CalgaryCalgaryAlbertaT2N 1N4Canada

With the increasing demand for petroleum,shale oil with considerable reserves has become an important part of global oil resources.The shale oil reservoir has a large number of nanopores and a complicated mineral composition,and the effect of nanopore confinement and pore type usually makes the effective development of shale oil challenging.For a shale oil reservoir,CO_(2) flooding can effectively reduce the oil viscosity and improve the reservoir properties,which can thus improve the recovery performance.In this study,the method of non-equilibrium molecular dynamics(NEMD)simulation is used to simulate the CO_(2) flooding process in the nanoscale pores of shale oil reservoir.The performance difference between the organic kerogen slit nanopore and four types of inorganic nanopores is discussed.Thus,the effects of nanopore type and displacement velocity on the nanoscale displacement behavior of CO_(2) are analyzed.Results indicate that the CO_(2) flooding process of different inorganic pores is different.In comparison,the displacement efficiency of light oil components is higher,and the transport distance is longer.The intermolecular interaction can significantly affect the CO_(2) displacement behavior in nanopores.The CO_(2) displacement efficiency is shown as montmorillonite,feldspar>quartz>calcite>kerogen.On the other hand,it is found that a lower displacement velocity can benefit the miscibility process between alkane and CO_(2),which is conducive to the overall displacement process of CO_(2).The displacement efficiency can significantly decrease with the increase in displacement velocity.But once the displacement velocity is very high,the strong driving force can promote the alkane to move forward,and the displacement efficiency will recover slightly.This study further reveals the microscopic oil displacement mechanism of CO_(2) in shale nanopores,which is of great significance for the effective development of shale oil reservoirs by using the method of CO_(2) injection.

关键词： Displacement behavior Nanopores NEMD simulation Shale oil CO_(2) kerogen

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Distribution and geochemical significance of trace elements in kerogens from Ediacaran–Lower Cambrian strata in South China

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Acta Geochimica 2023年第1期42卷 50-62页

作者： Qian Deng Guanyu Zhao Haozhe Wang Bin Cheng Zewen Liao State Key Laboratory of Organic Geochemistry Guangzhou Institute of GeochemistryChinese Academy of SciencesGuangzhou 510640China CAS Center for Excellence in Deep Earth Science Guangzhou 510640China University of Chinese Academy of Sciences Beijing 100049China

Some trace elements(TEs),both bio-essential and redox-sensitive,are promising tracers of Earth’s surface processes.As an essential sedimentary organic matter,kerogen may have inherited and retained the key TEs from organisms.In this study,the distribution of TEs in kerogens from two sections(Dongkanshang and Fengtan) in South China was analyzed to explore its biogeochemical significance during Ediacaran-Lower Cambrian.Compared with V and Zn,the relative concentrations of Co,Ni,Cu,and Mo were generally higher in kerogens than in the whole rocks.Enrichment of TEs in the kerogen was involved in the selective utilization of TEs by different organic precursors and the competition of sulfide in the depositional environment.The significant content of TEs in the kerogens from deep-water facies corresponded to a more negative δ^(13) Ckeras a result of the dominant taxa of chemo autotrophs with tremendous bioaccumulation potential for trace metals and the reduction conditions favorable for organic matter preservation.Furthermore,the content variations of trace elements in the kerogens coincided with the rise and fall of the Ediacaran biota,implying that the trace elements might have played an important role in early life evolution.

关键词： Trace elements kerogen Ediacaran-Early Cambrian Biogeochemical significance South China

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The Biomarkers in the Mesoproterozoic Organic-rich Rocks of North China Craton:Implication for the Precursor and Preservation of Organism in the Prokaryotic Realm

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Acta Geologica Sinica(English Edition) 2022年第1期96卷 293-308页

作者： MA Sihong ZHANG Shuichang SU Jin WANG Xiaomei HE Kun FANG Yu MI Jingkui Key Laboratory of Petroleum Geochemistry Research Institute of Petroleum Exploration and DevelopmentChina National Petroleum CorporationBeijing 100083China

Mesoproterozoic marine organic-rich rocks are widely distributed in the North China Craton,include the Gaoyuzhuang(GYZ),the Hongshuizhuang(HSZ),and the Xiamaling(XML)formations.According to the T;value and isomerisation ratio of C;homohopanes,the XML,HSZ,and GYZ samples were in low mature,mature and high mature stage,respectively.Biomarker distribution in extractable organic matter(EOM)of three Mesoproterozoic organic-rock samples in different maturity were analysed to reveal the organic precursor and preservation pathway of in the Mesoproterozoic Combined with gold-tube pyrolysates of three Mesoproterozoic samples,it could further illuminate the chemical composition of Mesoproterozoic kerogen,given excluding.The results indicated that the three formations were all deposited under reducing condition and their organic precursors mainly were some aquatic organisms.High content of rearranged hopanes was detected in EOM of XML and HSZ samples,whereas they were relatively low in the high mature GYZ sample.Contrast to that in EOM,the relative concentration of rearranged hopanes sharply decreased in the gold-tube pyrolysates of the XML kerogen,then slightly increased but was still significantly lower than the EOM of XML sample,which indicated that catalysis of clay minerals in the early diagenesis only changed the chemical composition of the unstable functional groups of the kerogen during the preservation.Due to the thriving heterotrophic microbes and low sink rate of particulate organic matter during the Mesoproterozoic,primary producers suffered extensive degradation during sinking process,only some resistant biopolymers lacking of lipid compounds survived from heterotrophic degradation,while heterotrophic microbes contained more proportion of organic precursors.Abundant pristane(Pr)and phytane(Ph)were only released in high mature stage because of the protection of the macromolecular structure of resistant biopolymers which prevented biomarkers from being altered by the thermal stress.The absence of 13α(n-alkyl)-tric

关键词： biomarker kerogen rearranged hopanes primary producer heterotrophic microbe Mesoproterozoic North China Craton

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Hydrocarbon generation mechanism of lamalginite- and telalginite-dominated source rocks in a saline lake basin: A case study of the Permian Lucaogou formation in the Jimusaer Sag, Junggar Basin

能源地球科学(英文)

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能源地球科学(英文) 2023年第3期4卷 220-232页

作者： Lichang Chen Jingqiang Tan Haisu Cui Xiao Ma Xueqi Song Qiang Yuan Jin Liu Key Laboratory of Metallogenic Prediction of Nonferrous Metals and Geological Environment Monitoring(Central South University) Ministry of EducationChangsha410083China School of Civil Engineering(Central South University) Changsha410083China Research Institute of Experiment and Testing PetroChina Xinjiang Oilfield CompanyKaramay834000China

The hydrocarbon generation of source rocks is significantly influenced by organic matter type, chemical element composition, and structural characteristics of kerogen. We classified the organic matter types in the shale of the Lucaogou Formation, Jimusar Sag, Junggar Basin, using organic petrology and rock pyrolysis as well as kerogen element and Fourier transform infrared (FT-IR) spectroscopy analyses, and compared the hydrocarbon generation mechanisms of source rocks with different types of organic matter. The organic matter of the Lucaogou Formation contains mostly two types of hydrocarbon generating macerals, the lamalginite and the telalginite based on physical and optical properties (texture, fluorescence, and optical reflectance). The lamalginite is a continuous sheet of less than 5 μm thick and greater than 50 μm in length. It has strong yellow fluorescence. The telalginite occurs as discontinuous short strips or pear-shaped objects with length of 10–30 μm and relatively weak fluorescence. The lamalginite-dominated shale has higher atomic H/C and lower atomic O/C ratios, indicating better hydrocarbon generation potential, whereas the telalginite-dominated shale has higher N and S heteroatom contents. The results of FT-IR spectroscopy of the kerogen indicate that the lamalginite-dominated shale is rich in aliphatic groups with long linear methylene sequences. The aromatic groups content is relatively low, but the carboxyl/carbon group (Cdouble bondO) content is high. The aliphatic group content of the telalginite-dominated shale is relatively low, with short-branched chains. The aromatic group content is relatively high. The methyl vibration signal directly connected to the benzene ring is strong, and the sulfoxide (Sdouble bondO) group has a high-intensity peak. Our results provide new insights into distinguishing organic matter types in the Lucaogou Formation and understanding the hydrocarbon generation mechanisms of source rocks in saline lake basins.

关键词： Luca ogou formnation Larnalginite Telalginite kerogen Fourier transformn infared spectroscopy

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kerogen——as a sort of organic bearer of gold in gold-bearing formations

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Chinese Science Bulletin 1999年第11期44卷 1045-1050页

作者： Kai Hu Jianping Zhai Yingjun Liu Henian Wang Nanjing Univ Dept Earth Sci Nanjing 210093 Peoples R China Nanjing Univ State Key Lab Mineral Deposits Res Nanjing 210093 Peoples R China

Organic component, organic carbon and gold content analyses were used to study the relationship between gold mineralization and organic matter in major host rocks of three different chronological gold-bearing formations of South China. The results show that the organic matter of host rocks in various chronological major gold-bearing formations of South China has associated with gold mineralization in genesis. There is a positive correlation between gold and organic carbon in the host rocks of gold-bearing formations. Gold element was mainly enriched in insoluble organic matter——kerogen. Gold content of the kerogen is commonly higher from a few tens to several hundred times than that of the whole rocks, up to 5%—40% gold of the whole rocks. Gold remaining in the kerogen was considered an organic group of the kerogen to combine with ionic gold in solution through surface absorption, ion exchange complex reaction and chelation so that the kerogen could have become an important sort of organic bearer

关键词： kerogen gold-bearing formation organic bearer asphaltene.

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Molecular Structure of kerogen in the Longmaxi Shale: Insights from Solid State NMR, FT-IR, XRD and HRTEM

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Acta Geologica Sinica(English Edition) 2019年第4期93卷 1015-1024页

作者： WANG Xiaoqi ZHU Yanming LIU Yu LI Wu Key Laboratory of Coalbed Methane Resources and Reservoir Formation on Process Ministry of EducationChina University of Mining and TechnologyXuzhou 221008JiangsuChina School of Resources and Geosciences China University of Mining and TechnologyXuzhou 221116JiangsuChina

kerogen plays an important role in shale gas adsorption,desorption and diffusion.Therefore,it is necessary to characterize the molecular structure of kerogen.In this study,four kerogen samples were isolated from the organic-rich shale of the Longmaxi Formation.Raman spectroscopy was used to determine the maturity of these kerogen samples.Highresolution transmission electron microscopy(HRTEM),13 C nuclear magnetic resonance(13 C NMR),X-ray diffraction(XRD)and Fourier transform infrared(FT-IR)spectroscopy were conducted to characterize the molecular structure of the shale samples.The results demonstrate that VReqv of these kerogen samples vary from 2.3%to 2.8%,suggesting that all the kerogen samples are in the dry gas window.The macromolecular carbon skeleton of the Longmaxi Formation kerogen is mainly aromatic(fa’=0.56).In addition,the aromatic structural units are mainly composed of naphthalene(23%),anthracene(23%)and phenanthrene(29%).However,the aliphatic structure of the kerogen macromolecules is relatively low(fal*+falH=0.08),which is presumed to be distributed in the form of methyl and short aliphatic chains at the edge of the aromatic units.The oxygen-containing functional groups in the macromolecules are mainly present in the form of carbonyl groups(fac=0.23)and hydroxyl groups or ether groups(falO=0.13).The crystallite structural parameters of kerogen,including the stacking height(Lc=22.84?),average lateral size(La=29.29?)and interlayer spacing(d002=3.43?),are close to the aromatic structural parameters of anthracite or overmature kerogen.High-resolution transmission electron microscopy reveals that the aromatic structure is well oriented,and more than 65%of the diffractive aromatic layers are concentrated in the main direction.Due to the continuous deep burial,the longer aliphatic chains and oxygen-containing functional groups in the kerogen are substantially depleted.However,the ductility and stacking degree of the aromatic structure increases during thermal evolution.This study provides quantitative in

关键词： organic-rich shale molecular structure kerogen HRTEM Sichuan Basin

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Pore structure characterization and its effect on methane adsorption in shale kerogen

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Petroleum Science 2021年第2期18卷 565-578页

作者： Tian-Yu Wang Shou-Ceng Tian Qing-Ling Liu Gen-Sheng Li Mao Sheng Wen-Xi Ren Pan-Pan Zhang State Key Laboratory of Petroleum Resources and Prospecting China University of Petroleum(Beijing)Beijing102249China Harvard SEAS-CUPB Joint Laboratory on Petroleum Science 29 Oxford StreetCambridgeMA02138USA China National Oil and Gas Exploration and Development Company Ltd Beijing100034China State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum UniversityChengdu610500China

Pore structure characterization and its effect on methane adsorption on shale kerogen are crucial to understanding the fundamental mechanisms of gas storage,transport,and reserves evaluation.In this study,we use 3D scanning confocal microscopy,scanning electron microscopy(SEM),X-ray nano-computed tomography(nano-CT),and low-pressure N2 adsorption analysis to analyze the pore structures of the shale.Additionally,the adsorption behavior of methane on shales with different pore structures is investigated by molecular simulations.The results show that the SEM image of the shale sample obviously displays four different pore shapes,including slit pore,square pore,triangle pore,and circle pore.The average coordination number is 4.21 and the distribution of coordination numbers demonstrates that pores in the shale have high connectivity.Compared with the adsorption capacity of methane on triangle pores,the adsorption capacity on slit pore,square pore,and circle pore are reduced by 9.86%,8.55%,and 6.12%,respectively.With increasing pressure,these acute wedges fill in a manner different from the right or obtuse angles in the other pores.This study offers a quantitative understanding of the effect of pore structure on methane adsorption in the shale and provides better insight into the evaluation of gas storage in geologic shale reservoirs.

关键词： Shale Methane adsorption Pore structure kerogen Molecular simulation

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