Coal is a solid combustible mineral,and coal-bearing strata have important hydrocarbon generation potential and contribute to more than 12%of the global hydrocarbon resources.However,the deposition and hydrocarbon evo...Coal is a solid combustible mineral,and coal-bearing strata have important hydrocarbon generation potential and contribute to more than 12%of the global hydrocarbon resources.However,the deposition and hydrocarbon evolution process of ancient coal-bearing strata is characterized by multiple geological times,leading to obvious distinctions in their hydrocarbon generation potential,geological processes,and production,which affect the evaluation and exploration of hydrocarbon resources derived from coaly source rocks worldwide.This study aimed to identify the differences on oil-generated parent macerals and the production of oil generated from different coaly source rocks and through different oil generation processes.Integrating with the analysis of previous tectonic burial history and hydrocarbon generation history,high-temperature and high-pressure thermal simulation experiments,organic geochemistry,and organic petrology were performed on the Carboniferous-Permian(C-P)coaly source rocks in the Huanghua Depression,Bohai Bay Basin.The oil-generated parent macerals of coal's secondary oil generation process(SOGP)were mainly hydrogen-rich collotelinite,collodetrinite,sporinite,and cutinite,while the oil-generated parent macerals of tertiary oil generation process(TOGP)were the remaining small amount of hydrogen-rich collotelinite,sporinite,and cutinite,as well as dispersed soluble organic matter and unexhausted residual hydrocarbons.Compared with coal,the oil-generated parent macerals of coaly shale SOGP were mostly sporinite and cutinite.And part of hydrogen-poor vitrinite,lacking hydrocarbon-rich macerals,and macerals of the TOGP,in addition to some remaining cutinite and a small amount of crude oil and bitumen from SOGP contributed to the oil yield.The results indicated that the changes in oil yield had a good junction between SOGP and TOGP,both coal and coaly shale had higher SOGP aborted oil yield than TOGP starting yield,and coaly shale TOGP peak oil yield was lower than SOGP peak oil yield.There were significant differences in saturated hydrocarbon and aromatic parameters in coal and coaly shale.Coal SOGP was characterized by a lower Ts/Tm and C31-homohopane22S/(22S+22R)and a higher Pr/n C17compared to coal TOGP,while the aromatic parameter methyl dibenzothiophene ratio(MDR)exhibited coaly shale TOGP was higher than coaly shale SOGP than coaly TOGP than coaly SOGP,and coal trimethylnaphthalene ratio(TNR)was lower than coaly shale TNR.Thus,we established oil generation processes and discriminative plates.In this way,we distinguished the differences between oil generation parent maceral,oil generation time,and oil production of coaly source rocks,and therefore,we provided important support for the evaluation,prediction,and exploration of oil resources from global ancient coaly source rocks.展开更多
Natural gas and condensate derived from Carboniferous-Permian(C-P)coaly source rocks discovered in the Dagang Oilfield in the Bohai Bay Basin(east China)have important implications for the potential exploration of C-P...Natural gas and condensate derived from Carboniferous-Permian(C-P)coaly source rocks discovered in the Dagang Oilfield in the Bohai Bay Basin(east China)have important implications for the potential exploration of C-P coaly source rocks.This study analyzed the secondary,tertiary,and dynamic characteristics of hydrocarbon generation in order to predict the hydrocarbon potentials of different exploration areas in the Dagang Oilfield.The results indicated that C-P oil and gas were generated from coaly source rocks by secondary or tertiary hydrocarbon generation and characterized by notably different hydrocarbon products and generation dynamics.Secondary hydrocarbon generation was completed when the maturity reached vitrinite reflectance(Ro)of 0.7%-0.9%before uplift prior to the Eocene.Tertiary hydrocarbon generation from the source rocks was limited in deep buried sags in the Oligocene,where the products consisted of light oil and gas.The activation energies for secondary and tertiary hydrocarbon generation were 260-280 kJ/mol and 300-330 kJ/mol,respectively,indicating that each instance of hydrocarbon generation required higher temperature or deeper burial than the previous instance.Locations with secondary or tertiary hydrocarbon generation from C-P coaly source rocks were interpreted as potential oil and gas exploration regions.展开更多
Coaly graphite is an important natural graphite resource that derived from coal under a natural process that associated with igneous intrusion.Flake graphite is usually used for the chemical synthesis of graphene oxid...Coaly graphite is an important natural graphite resource that derived from coal under a natural process that associated with igneous intrusion.Flake graphite is usually used for the chemical synthesis of graphene oxide(GO),the main precursor for preparation of graphene,but few papers pay attention to preparing GO using coaly graphite.In this paper,four kinds of natural coaly graphite with different graphitization degrees were exposed to a modified Hummer’s oxidation method to prepare GO.The flake graphite sample was also used for comparison.The results showed that the structural change process from graphite to GO were significantly affected by the graphitization degree of the original coaly graphite.The relationship between yields of GO and graphitization degrees of the coaly graphite was explored.The mechanism of why the graphite with low graphitization degrees cannot be totally oxidized was proposed.Coaly graphite with a graphitization degree of higher than 80% was easier to be oxidized and yielded the same amount of GO as the flake graphite did,suggesting it is the potential substitute for the flake graphite to produce GO in bulk quantities.展开更多
Although various coaly source rocks widely developed in the Carboniferous-Permian(C-P)of the Bohai Bay Basin,their geochemical characteristics and hydrocarbon generation potential are poorly understood.This study aims...Although various coaly source rocks widely developed in the Carboniferous-Permian(C-P)of the Bohai Bay Basin,their geochemical characteristics and hydrocarbon generation potential are poorly understood.This study aims to discriminate the contribution of hydrocarbon generation from different C-P coaly source rocks and clarify the differences within generated oils using organic geochemistry,organic petrology,and thermal simulation experiments.The coaly source rocks containt coal clarain and durain,carbonaceous shale,and shale deposited in deltaic and lagoonal environment.The results indicated that clarain,durain,and carbonaceous shale exhibited higher hydrogen index and liquid-gas hydrocarbon yields than lagoonal and deltaic shales,which was mainly associated with the concentrations of sporinite,cutinite,and hydrogen-rich collodetrinite.Aliphatic hydro-carbons originated firom coal and carbonaceous shale presented lower Ts/(Ts+Tm),Ga/17α(H)21β(H)-C_(30)hopane,18α(H)-oleanane/17α(H)21β(H)-C_(30)hopane ratios,and higher 17β3(H)21α(H)-C_(30)Morane/17α(H)21β(H)-C_(30)hopane than deltaic lagoonal shales.Parameters of aromatic hydrocarbons generated from five lithologies of coaly source rocks trended as clear group distribution,e.g.,clarain and durain showing lower MNR,DBT/Fluorene(F)ratios and higher DBF/F ratio than coaly shales.The distinct descending trend of hydrocarbon potential is obtained from clarain,durain,carbonaceous shale to lagoonal and deltaic shales,implying dominated the petroleum and natural gas supplement from coal and carbonaceous shale.The difference between aliphatic and aromatic hydrocarbons provides a significant contribution to analyze the generic relationship between coaly source rock and lacustrine shale.Our results illustrate the importance of coaly source rocks for the in-depth oil-gas exploration of the Bohai Bay Basin and understanding hydrocarbon generation potential of source rocks in coal bearing strata.展开更多
基金supported by the Certificate of National Science and Technology Major Project of the Ministry of Science and Technology of China(No.2016ZX05006007-004)the National Natural Science Foundation of China(Nos.42172145,42072130)。
文摘Coal is a solid combustible mineral,and coal-bearing strata have important hydrocarbon generation potential and contribute to more than 12%of the global hydrocarbon resources.However,the deposition and hydrocarbon evolution process of ancient coal-bearing strata is characterized by multiple geological times,leading to obvious distinctions in their hydrocarbon generation potential,geological processes,and production,which affect the evaluation and exploration of hydrocarbon resources derived from coaly source rocks worldwide.This study aimed to identify the differences on oil-generated parent macerals and the production of oil generated from different coaly source rocks and through different oil generation processes.Integrating with the analysis of previous tectonic burial history and hydrocarbon generation history,high-temperature and high-pressure thermal simulation experiments,organic geochemistry,and organic petrology were performed on the Carboniferous-Permian(C-P)coaly source rocks in the Huanghua Depression,Bohai Bay Basin.The oil-generated parent macerals of coal's secondary oil generation process(SOGP)were mainly hydrogen-rich collotelinite,collodetrinite,sporinite,and cutinite,while the oil-generated parent macerals of tertiary oil generation process(TOGP)were the remaining small amount of hydrogen-rich collotelinite,sporinite,and cutinite,as well as dispersed soluble organic matter and unexhausted residual hydrocarbons.Compared with coal,the oil-generated parent macerals of coaly shale SOGP were mostly sporinite and cutinite.And part of hydrogen-poor vitrinite,lacking hydrocarbon-rich macerals,and macerals of the TOGP,in addition to some remaining cutinite and a small amount of crude oil and bitumen from SOGP contributed to the oil yield.The results indicated that the changes in oil yield had a good junction between SOGP and TOGP,both coal and coaly shale had higher SOGP aborted oil yield than TOGP starting yield,and coaly shale TOGP peak oil yield was lower than SOGP peak oil yield.There were significant differences in saturated hydrocarbon and aromatic parameters in coal and coaly shale.Coal SOGP was characterized by a lower Ts/Tm and C31-homohopane22S/(22S+22R)and a higher Pr/n C17compared to coal TOGP,while the aromatic parameter methyl dibenzothiophene ratio(MDR)exhibited coaly shale TOGP was higher than coaly shale SOGP than coaly TOGP than coaly SOGP,and coal trimethylnaphthalene ratio(TNR)was lower than coaly shale TNR.Thus,we established oil generation processes and discriminative plates.In this way,we distinguished the differences between oil generation parent maceral,oil generation time,and oil production of coaly source rocks,and therefore,we provided important support for the evaluation,prediction,and exploration of oil resources from global ancient coaly source rocks.
基金supported by the Certificate of National Science and Technology Major Project of the Ministry of Science and Technology of China(2016ZX05006007-004,2016ZX05014)National Natural Science Foundation of China(41702139,U1663204,41602138,41602142)+1 种基金Natural Science Foundation of Shandong Province(ZR2017BD036,ZR2017LD005)Fundamental Research Funds for the Central Universities(18CX02008A)。
文摘Natural gas and condensate derived from Carboniferous-Permian(C-P)coaly source rocks discovered in the Dagang Oilfield in the Bohai Bay Basin(east China)have important implications for the potential exploration of C-P coaly source rocks.This study analyzed the secondary,tertiary,and dynamic characteristics of hydrocarbon generation in order to predict the hydrocarbon potentials of different exploration areas in the Dagang Oilfield.The results indicated that C-P oil and gas were generated from coaly source rocks by secondary or tertiary hydrocarbon generation and characterized by notably different hydrocarbon products and generation dynamics.Secondary hydrocarbon generation was completed when the maturity reached vitrinite reflectance(Ro)of 0.7%-0.9%before uplift prior to the Eocene.Tertiary hydrocarbon generation from the source rocks was limited in deep buried sags in the Oligocene,where the products consisted of light oil and gas.The activation energies for secondary and tertiary hydrocarbon generation were 260-280 kJ/mol and 300-330 kJ/mol,respectively,indicating that each instance of hydrocarbon generation required higher temperature or deeper burial than the previous instance.Locations with secondary or tertiary hydrocarbon generation from C-P coaly source rocks were interpreted as potential oil and gas exploration regions.
基金the financial support provided by the National Natural Science Foundation of China(41672150).
文摘Coaly graphite is an important natural graphite resource that derived from coal under a natural process that associated with igneous intrusion.Flake graphite is usually used for the chemical synthesis of graphene oxide(GO),the main precursor for preparation of graphene,but few papers pay attention to preparing GO using coaly graphite.In this paper,four kinds of natural coaly graphite with different graphitization degrees were exposed to a modified Hummer’s oxidation method to prepare GO.The flake graphite sample was also used for comparison.The results showed that the structural change process from graphite to GO were significantly affected by the graphitization degree of the original coaly graphite.The relationship between yields of GO and graphitization degrees of the coaly graphite was explored.The mechanism of why the graphite with low graphitization degrees cannot be totally oxidized was proposed.Coaly graphite with a graphitization degree of higher than 80% was easier to be oxidized and yielded the same amount of GO as the flake graphite did,suggesting it is the potential substitute for the flake graphite to produce GO in bulk quantities.
基金supported by the Certificate of National Science and Technology Major Project of the Ministry of Science and Technology of China(No.2016ZX05006-007-004)National Natural Science Foundation of China(Grant Nos.41702139,420772164,42072130,and U1762217)+2 种基金Natural Science Foundation of Shandong Province(No.ZR2017BD036)the Fundamental Research Funds for the Central Universities(No.18CX02008A)Taishan Scholar Program of Shandong Province(No.TSQN201812030).
文摘Although various coaly source rocks widely developed in the Carboniferous-Permian(C-P)of the Bohai Bay Basin,their geochemical characteristics and hydrocarbon generation potential are poorly understood.This study aims to discriminate the contribution of hydrocarbon generation from different C-P coaly source rocks and clarify the differences within generated oils using organic geochemistry,organic petrology,and thermal simulation experiments.The coaly source rocks containt coal clarain and durain,carbonaceous shale,and shale deposited in deltaic and lagoonal environment.The results indicated that clarain,durain,and carbonaceous shale exhibited higher hydrogen index and liquid-gas hydrocarbon yields than lagoonal and deltaic shales,which was mainly associated with the concentrations of sporinite,cutinite,and hydrogen-rich collodetrinite.Aliphatic hydro-carbons originated firom coal and carbonaceous shale presented lower Ts/(Ts+Tm),Ga/17α(H)21β(H)-C_(30)hopane,18α(H)-oleanane/17α(H)21β(H)-C_(30)hopane ratios,and higher 17β3(H)21α(H)-C_(30)Morane/17α(H)21β(H)-C_(30)hopane than deltaic lagoonal shales.Parameters of aromatic hydrocarbons generated from five lithologies of coaly source rocks trended as clear group distribution,e.g.,clarain and durain showing lower MNR,DBT/Fluorene(F)ratios and higher DBF/F ratio than coaly shales.The distinct descending trend of hydrocarbon potential is obtained from clarain,durain,carbonaceous shale to lagoonal and deltaic shales,implying dominated the petroleum and natural gas supplement from coal and carbonaceous shale.The difference between aliphatic and aromatic hydrocarbons provides a significant contribution to analyze the generic relationship between coaly source rock and lacustrine shale.Our results illustrate the importance of coaly source rocks for the in-depth oil-gas exploration of the Bohai Bay Basin and understanding hydrocarbon generation potential of source rocks in coal bearing strata.