To investigate the influence of diagenetic water media on the hydrogen isotopes of individual sedimentary aromatic compounds,a series of hydrous pyrolyses were conducted on herbaceous peat.Polycyclic aromatic hydrocar...To investigate the influence of diagenetic water media on the hydrogen isotopes of individual sedimentary aromatic compounds,a series of hydrous pyrolyses were conducted on herbaceous peat.Polycyclic aromatic hydrocarbons(PAHs)in hydrous pyrolysed samples and their hydrogen isotopic composition characteristics were studied.The aqueous medium demonstrated a significant influence on the hydrogen isotopic composition of the individual PAHs generated during pyrolysis.The results showed that the PAHs formed after pyrolysis in the presence of a saltwater medium with high δD value from a salt lake had a heavy hydrogen isotopic composition.The PAHs formed after pyrolysis in the presence of a fresh water medium with low δD value from a swamp had a light hydrogen isotopic composition.The difference in the average PAHδD value between the two hydrous experiments varied from -174‰ to -109‰,suggesting that the hydrogen isotopic composition of individual sedimentary PAHs can reflect the source of the diagenetic water medium.In addition,a comparative study found that the hydrogen isotopes of PAHs were superior to those of n-alkanes in the same sample for diagenetic water indications.The results indicated that the exchange of water-derived inorganic hydrogen and organic hydrogen was more intensive in freshwater experiments than in saltwater experiments.With an increase in the simulation temperature,the average δD value of PAHs generated in the hydrous simulation experiments showed an increasing trend,reflecting that the δD value of sedimentary PAHs formed with the participation of diagenetic water media was still closely related to the thermal maturity of organic matter.Comparative studies showed that theδD values of different types of organic compounds produced by hydrous pyrolysis of peat were in the order,PAHs>n-alkanes>methane.展开更多
To understand the influence of the diagenetic water medium on the isotopic compositions of thermogenic coalbed gas, both hydrous and anhydrous closed-system pyrolyses were performed at temperatures of 250°C to 65...To understand the influence of the diagenetic water medium on the isotopic compositions of thermogenic coalbed gas, both hydrous and anhydrous closed-system pyrolyses were performed at temperatures of 250°C to 650°C on an herbaceous marsh peat. Compared to the results of anhydrous pyrolysis, the hydrocarbon gases generated from hydrous pyrolyses have very different hydrogen isotopic compositions. However, the carbon isotopic compositions of the hydrocarbon gases became only slightly heavier in hydrous pyrolysis, compared to that from anhydrous pyrolysis. With the progress of thermal evolution from peat to a more advanced thermal maturity of vitrinite reflectance values(Ro) of 5.5% during the pyrolysis, the difference in the average δD value increased from 52‰ to 64‰ between the hydrous pyrolysis with saltwater and anhydrous pyrolysis and increased from 18‰ to 29‰ between the hydrous pyrolysis with freshwater and anhydrous pyrolysis, respectively. The difference in the average δ^(13)C value was only 1‰–2‰ between the hydrous and anhydrous pyrolysis. The relationships between the δD values of the generated hydrocarbon gases and Ro values as well as among δD values of the hydrocarbon gas species are established. The close relationships among these parameters suggest that the water medium had a significant effect on the hydrogen isotopic composition and a minimal effect on the carbon isotopic composition of the hydrocarbon gases. The results of these pyrolyses may provide information for the understanding of the genesis of coalbed gas from herbaceous marsh material with the participation of different diagenetic water media.展开更多
To understand the thermal evolution of lacustrine sedimentary n-alkane hydrogen isotopic composition(δD),especially bacterially derived n-alkanes,anhydrous thermal simulation experiments were performed with sediments...To understand the thermal evolution of lacustrine sedimentary n-alkane hydrogen isotopic composition(δD),especially bacterially derived n-alkanes,anhydrous thermal simulation experiments were performed with sediments from Lake Gahai(Gannan,China).We analyzed the original and pyrolysis-generated n-alkanes and theirδD values.The results showed that thermal maturity and n-alkane origins significantly affected the distribution of pyrolysis-generated n-alkanes.In immature to post-mature sediments,the bacterial-derived medium-chain n-alkanes generally had depletedδD values.The maximum difference in averageδD values between the bacterial-and herbaceous plant-derived medium-chain n-alkanes was 32‰,and the maximum difference in δD values among individual n-alkanes was 59‰.We found that the averageδD value of pyrolysis-generated n-alkanes from different latitude was significantly different in immature to highly mature sediments,but similar in post-mature ssediments.The hydrogen isotopes of sedimentary n-alkanes can be used as indicators for paleoclimate/paleo-environment conditions only when sediments are immature to highly mature.During thermal evolution,the δD value of generated individual n-alkanes and the averageδD value increased with thermal maturity,indicating that hydrogen isotopes of sedimentary n-alkanes can be used as an index of organic matter maturity.We established mathematical models of average δD values of generated n-alkanes from immature to post-mature sediments using n C_(21)^(-)/nC_(21)^(+)and average chain lengths.These results improve our understanding of the distribution andδD value of sedimentary n-alkanes derived from herbaceous plants in mid-latitude plateau cold regions.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.41972110 and 41772108)。
文摘To investigate the influence of diagenetic water media on the hydrogen isotopes of individual sedimentary aromatic compounds,a series of hydrous pyrolyses were conducted on herbaceous peat.Polycyclic aromatic hydrocarbons(PAHs)in hydrous pyrolysed samples and their hydrogen isotopic composition characteristics were studied.The aqueous medium demonstrated a significant influence on the hydrogen isotopic composition of the individual PAHs generated during pyrolysis.The results showed that the PAHs formed after pyrolysis in the presence of a saltwater medium with high δD value from a salt lake had a heavy hydrogen isotopic composition.The PAHs formed after pyrolysis in the presence of a fresh water medium with low δD value from a swamp had a light hydrogen isotopic composition.The difference in the average PAHδD value between the two hydrous experiments varied from -174‰ to -109‰,suggesting that the hydrogen isotopic composition of individual sedimentary PAHs can reflect the source of the diagenetic water medium.In addition,a comparative study found that the hydrogen isotopes of PAHs were superior to those of n-alkanes in the same sample for diagenetic water indications.The results indicated that the exchange of water-derived inorganic hydrogen and organic hydrogen was more intensive in freshwater experiments than in saltwater experiments.With an increase in the simulation temperature,the average δD value of PAHs generated in the hydrous simulation experiments showed an increasing trend,reflecting that the δD value of sedimentary PAHs formed with the participation of diagenetic water media was still closely related to the thermal maturity of organic matter.Comparative studies showed that theδD values of different types of organic compounds produced by hydrous pyrolysis of peat were in the order,PAHs>n-alkanes>methane.
基金supported by the National Natural Science Foundation of China(Grant nos.41772108 and 41472121)
文摘To understand the influence of the diagenetic water medium on the isotopic compositions of thermogenic coalbed gas, both hydrous and anhydrous closed-system pyrolyses were performed at temperatures of 250°C to 650°C on an herbaceous marsh peat. Compared to the results of anhydrous pyrolysis, the hydrocarbon gases generated from hydrous pyrolyses have very different hydrogen isotopic compositions. However, the carbon isotopic compositions of the hydrocarbon gases became only slightly heavier in hydrous pyrolysis, compared to that from anhydrous pyrolysis. With the progress of thermal evolution from peat to a more advanced thermal maturity of vitrinite reflectance values(Ro) of 5.5% during the pyrolysis, the difference in the average δD value increased from 52‰ to 64‰ between the hydrous pyrolysis with saltwater and anhydrous pyrolysis and increased from 18‰ to 29‰ between the hydrous pyrolysis with freshwater and anhydrous pyrolysis, respectively. The difference in the average δ^(13)C value was only 1‰–2‰ between the hydrous and anhydrous pyrolysis. The relationships between the δD values of the generated hydrocarbon gases and Ro values as well as among δD values of the hydrocarbon gas species are established. The close relationships among these parameters suggest that the water medium had a significant effect on the hydrogen isotopic composition and a minimal effect on the carbon isotopic composition of the hydrocarbon gases. The results of these pyrolyses may provide information for the understanding of the genesis of coalbed gas from herbaceous marsh material with the participation of different diagenetic water media.
基金supported by the National Natural Science Foundation of China(Grant Nos.41772108 and 41972110)。
文摘To understand the thermal evolution of lacustrine sedimentary n-alkane hydrogen isotopic composition(δD),especially bacterially derived n-alkanes,anhydrous thermal simulation experiments were performed with sediments from Lake Gahai(Gannan,China).We analyzed the original and pyrolysis-generated n-alkanes and theirδD values.The results showed that thermal maturity and n-alkane origins significantly affected the distribution of pyrolysis-generated n-alkanes.In immature to post-mature sediments,the bacterial-derived medium-chain n-alkanes generally had depletedδD values.The maximum difference in averageδD values between the bacterial-and herbaceous plant-derived medium-chain n-alkanes was 32‰,and the maximum difference in δD values among individual n-alkanes was 59‰.We found that the averageδD value of pyrolysis-generated n-alkanes from different latitude was significantly different in immature to highly mature sediments,but similar in post-mature ssediments.The hydrogen isotopes of sedimentary n-alkanes can be used as indicators for paleoclimate/paleo-environment conditions only when sediments are immature to highly mature.During thermal evolution,the δD value of generated individual n-alkanes and the averageδD value increased with thermal maturity,indicating that hydrogen isotopes of sedimentary n-alkanes can be used as an index of organic matter maturity.We established mathematical models of average δD values of generated n-alkanes from immature to post-mature sediments using n C_(21)^(-)/nC_(21)^(+)and average chain lengths.These results improve our understanding of the distribution andδD value of sedimentary n-alkanes derived from herbaceous plants in mid-latitude plateau cold regions.
