In order to discuss the role and influence of water during the generation of natural gas,the participation mechanism of water during the evolution of organic matter and its influences were summarized.In addition,we ca...In order to discuss the role and influence of water during the generation of natural gas,the participation mechanism of water during the evolution of organic matter and its influences were summarized.In addition,we carried out an anhydrous cracking experiment of oil extracted from the Feixianguan Formation source rock in a closed system,which led to the establishment of the kinetic models for describing carbon and hydrogen isotopic fractionation during gas generation from organic matter.The models were calibrated and then applied to the northeastern Sichuan Basin.By combining a series of gas generation experiments from octadecane pyrolysis without water or with distilled water in varying mass proportions,several results were proved:(1) the hydrogen isotopic composition of natural gas becomes lighter with the participation of formation water;(2) we can quantitatively study the hydrogen isotopic fractionation with the kinetic model for describing carbon isotopic fractionation; (3) more abundant and reliable geological information can be obtained through the combined application of carbon and hydrogen isotopic indices.展开更多
Hydrogen isotopic compositions of pyroxenes in peridotite xenoliths from the Nushan volcano, Anhui Province, SE China have been obtained using an ion probe (Cameca 1270). D/H ratios are constant within a single grain ...Hydrogen isotopic compositions of pyroxenes in peridotite xenoliths from the Nushan volcano, Anhui Province, SE China have been obtained using an ion probe (Cameca 1270). D/H ratios are constant within a single grain and among the different grains from the same sample. The lack of correlation between the D/H ratios and the hydrogen contents indicates that the hydrogen isotopic compositions are inherited from their mantle source. Combining with the δD values of coexisting amphiboles, it is inferred that the Nushan mantle experienced at least a two-stage metasomatic event. One was responsible for formation of amphiboles with extremely variable δD values, and the other was probably responsible for the high δD values (up to ?20‰) of some clinopyroxenes from peridotites, clinopyroxene and mica megacrysts. High δD values point to a subduction-related fluid being involved in one metasomatic event. The primary δD values (?90‰ to ?140‰) of the Nushan pyroxenes, together with data gleaned from the literature, suggest that the D/H ratios of the nominally anhydrous mineral reservoir might have differed from that of the other mantle hydrogen in being relatively depleted in D.展开更多
The hydrogen isotopic composition of plant leaf wax(δDwax) is used as an important tool for paleohydrologic reconstruction. However, the understanding of the relative importance of environmental and biological fact...The hydrogen isotopic composition of plant leaf wax(δDwax) is used as an important tool for paleohydrologic reconstruction. However, the understanding of the relative importance of environmental and biological factors in determining δDwax values still remains incomplete. To identify the effects of soil moisture and plant physiology on δDwax values in an arid ecosystem, and to explore the implication of these values for paleoclimatic reconstruction, we measured δD values of soil water(δDwater) and δDwax values in surface soils along two distance transects extending from the lakeshore to wetland to dryland around Lake Qinghai and Lake Gahai on the northeast Qinghai-Tibetan Plateau. The results showed that the δDwater values were negatively correlated with soil water content(SWC)(R^2=0.9166), and ranged from –67‰ to –46‰ with changes in SWC from 6.2% to 42.1% in the arid areas of the Gangcha(GCh) and Gahai(GH) transects. This indicated that evaporative D-enrichment in soil water was sensitive to soil moisture in an arid ecosystem. Although the shift from grasses to shrubs with increasing aridity occurred in the arid area of the GH transect, the δDwax values in surface soils from the arid areas of the two transects still showed a negative correlation with SWC(R^2=0.6835), which may be due to the controls of primary evaporative D-enrichment in the soil water and additional transpirational D-enrichment in the leaf water on the δDwaxvalues. Our preliminary research suggested that δDwax values can potentially be applied as a paleo-humidity indicator on the northeast Qinghai-Tibetan Plateau.展开更多
The reconstruction of paleo-elevation serves a dual purpose to enhance our comprehension of geodynamic processes affecting terrestrial landforms and to contribute significantly to the interpretation of atmospheric cir...The reconstruction of paleo-elevation serves a dual purpose to enhance our comprehension of geodynamic processes affecting terrestrial landforms and to contribute significantly to the interpretation of atmospheric circulation and biodiversity.The oxygen(δ~(18)O_w)and deuterium(δD_w)isotopes in atmospheric precipitation are systematically depleted with the increase of altitude,which are typical and widely applicated paleo-altimeters.The utilization of hydrogen isotope of hydrous silicate minerals within the shear zone system,volcanic glass,and plant leaf wax alkanes offers valuable insights for addressing evaporation and diagenesis.In this paper,we review the principle,application conditions,and influencing factors of the hydrogen isotope paleo-altimeter.In addition,we discuss the feasibility of utilizing this technique for quantitatively estimating the paleo-elevation of the southeastern Tibetan Plateau,where multiple shear zones extend over hundred kilometers parallel to the topographic gradient.展开更多
Hydrogen storage alloys(HSAs)are attracting widespread interest in the nuclear industry because of the generation of stable metal hydrides after tritium absorption,thus effectively preventing the leakage of radioactiv...Hydrogen storage alloys(HSAs)are attracting widespread interest in the nuclear industry because of the generation of stable metal hydrides after tritium absorption,thus effectively preventing the leakage of radioactive tritium.Commonly used HSAs in the hydrogen isotopes field are Zr2M(M=Co,Ni,Fe)alloys,metallic Pd,depleted U,and ZrCo alloy.Specifically,Zr2M(M=Co,Ni,Fe)alloys are considered promising tritium-getter materials,and metallic Pd is utilized to separate and purify hydrogen isotopes.Furthermore,depleted U and ZrCo alloy are well suited for storing and delivering hydrogen isotopes.Notably,all the aforementioned HSAs need to modulate their hydrogen storage properties for complex operating conditions.In this review,we present a comprehensive overview of the reported modification methods applied to the above alloys.Alloying is an effective amelioration method that mainly modulates the properties of HSAs by altering their local geometrical/electronic structures.Besides,microstructural modifications such as nano-sizing and nanopores have been used to increase the specific surface area and active sites of metallic Pd and ZrCo alloys for enhancing de-/hydrogenation kinetics.The combination of metallic Pd with support materials can significantly reduce the cost and enhance the pulverization resistance.Moreover,the poisoning resistance of ZrCo alloy is improved by constructing active surfaces with selective permeability.Overall,the review is constructive for better understanding the properties and mechanisms of hydrogen isotope storage alloys and provides effective guidance for future modification research.展开更多
The Yueguang gold deposit is located in Fengjia,Xinhua County,Hunan Province,South China.It represents a recently discovered small-scale gold deposit situated in the southwestern region of the Jiangnan Orogenic Belt,w...The Yueguang gold deposit is located in Fengjia,Xinhua County,Hunan Province,South China.It represents a recently discovered small-scale gold deposit situated in the southwestern region of the Jiangnan Orogenic Belt,west of the Baimashan granitic batholith.In order to discern the characteristics of the ore-formingfluids,the underlying mineralization processes,and establish a foundation for the origin of the Yueguang gold depositfluid inclusion micro-thermometry,as well as quartz hydrogen and oxygen isotope analysis,have been carried out on samples obtained from various stages of mineralization.The hydrothermal miner-alization stages within the Yueguang gold deposit can be categorized into three stages:(i)the barren,pre-ore quartz-pyrite stage(Stage Ⅰ),the quartz-pyrite-gold stage(Stage Ⅱ),and the post-ore quartz-carbonate stage(Stage Ⅲ),with the second stage being the main mineralization stage.Thefluid inclusions identified in samples from the main min-eralization stage can predominantly be described with the NaCl–H_(2)O and CO_(2)–NaCl–H_(2)O systems.These inclusions display homogenization temperatures ranging from 158.8 to 334.9℃,and thefluid salinity ranges from 0.3%to 4.0%(wt.%NaCl equiv.).Laser Raman spectroscopy analysis of individual inclusions further reveals the presence of gas-phases such as CO_(2),CH_(4),and N_(2).Isotopic analysis indicatesδ^(18)Ofluid values ranging from 3.95 to 6.7‰ and δDH_(2)O values ranging from-71.9 to-55.7‰.These results indi-cate that the ore-formingfluid of the Yueguang gold deposit belongs to metamorphic hydrothermalfluids of middle-low temperature and low salinity.In the process of ore formation,gold is transported in the form of Au(HS)2-complexes,with gold deposition being driven byfluid immiscibility.Therefore,the Yueguang gold deposit is categorized as an orogenic gold deposit dominated by metamorphic hydrother-malfluid.It may become a new target for gold exploration in the Baimashan region,central Hunan Province.展开更多
The influences of water media on the hydrogen isotopic composition of organic-thermogenic natural gas were tested in three series of experiments on coal pyrolysis, with no water, deionized water (δDH2O-58‰), and s...The influences of water media on the hydrogen isotopic composition of organic-thermogenic natural gas were tested in three series of experiments on coal pyrolysis, with no water, deionized water (δDH2O-58‰), and seawater (δSDn2O=-4.8‰) added, respectively. The experimental results show that the productivities of H2 and CO2 obviously increased under hydrous conditions and that the productivity of CH4 also remarkably increased in the high-evolution phase of hydrous experiments. Water was involved in the chemical reaction of hydrocarbon generation, and then the hydrogen isotopic composition of methane was affected. There is a linear correlation between the hydrogen isotopic composition of methane and its productivity, as reflected in the three series of experiments. In the case of the same CH4 productivity, the hydrogen isotopic composition of the methane produced in anhydrous experiments was the heaviest, that of the methane produced in seawater-adding experiments came second, and that of the methane produced in deionized water-adding experiments was the ligbtest. The hydrogen isotopic composition of natural gas/methane is affected by the following factors: 1) the characteristics of hydrogen isotopic composition of organic matter in source rocks, 2) the thermal evolution extent of organic matter, and 3) fossil-water media in the natural gas-generation period. The experimental results show that the influence of the fossil-water medium in the natural gas-generation period was lower than that of the other factors.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
Recent studies suggest that the hydrogen and oxygen isotopic compositions of clay minerals can indicate paleoclimate.Here,we report mineralogy and stable isotopic records(d D and δ^(18)O_(OH))of a weathering profile ...Recent studies suggest that the hydrogen and oxygen isotopic compositions of clay minerals can indicate paleoclimate.Here,we report mineralogy and stable isotopic records(d D and δ^(18)O_(OH))of a weathering profile located in the Fujian Province,aiming to validate whether hydroxyl stable isotopes can indicate paleo-precipitation and paleo-temperature.Our results indicate that the d D and δ^(18)O_(OH)changes in the kaolinite hydroxyl of the weathering profile are basically determined by the isotopic composition of paleo-meteoric water and paleotemperature,respectively.Nevertheless,whether the d D and δ^(18)O_(OH)of kaolinite can quantitatively indicate paleo-precipitation and paleo-temperature needs to be verified further,and especially,the structural oxygen isotopic composition that is the essential element for the kaolinite formation temperature calculation has to be constrained in future work.展开更多
The hydrocarbon gases in the L1 gas field of the Lishui-Jiaojiang Sag have been commonly interpreted to be an accumulation of pure sapropelic-type thermogenic gas.In this study,chemical components,stable isotopic comp...The hydrocarbon gases in the L1 gas field of the Lishui-Jiaojiang Sag have been commonly interpreted to be an accumulation of pure sapropelic-type thermogenic gas.In this study,chemical components,stable isotopic compositions,and light hydrocarbons were utilized to shed light on the origins of the hydrocarbon fluids in the L1gas pool.The hydrocarbon fluids in the L1 gas pool are proposed to be a mixture of three unique components:mid-maturity oil from the middle Paleocene coastal marine Lingfeng source rock,oil-associated(late oil window)gas generated from the lower Paleocene lacustrine Yueguifeng source rock,and primary microbial gas from the paralic deposits of the upper Paleocene Mingyuefeng source rock.Here,for the first time,the hydrocarbon gases in the L1 gas pool are diagnosed as mixed oil-associated sapropelic-type gas and microbial gas via four pieces of principal evidence:(1)The abnormal carbon isotopic distributions of all methane homologues from C_(1)(CH_(4)or methane)to C_(5)(C_(5)H_(12)or pentane)shown in the Chung plot;(2)the diagnostic~(13)C-depleted C_(1)compared with the thermogenic sapropelic-type gas model,whileδ^(13)C_(2)(C_(2)H_(6)or ethane)andδ^(13)C_(3)(C_(3)H_(8)or propane)both fit perfectly;(3)the excellent agreement of the calculated carbon isotopic compositions of the pure thermogenic gas with the results of the thermal simulated gas from the type-II1 kerogen-rich Yueguifeng source rock;and(4)the oil-associated gas inferred from various binary genetic diagrams with an abnormally elevated gas oil ratio.Overall,the natural gases of the L1 gas pool were quantified in this study to comprise approximately 13%microbial gas,nearly 48%oil-associated sapropelic-type gas,and 39%of nonhydrocarbon gas.The microbial gas is interpreted to have been codeposited and entrained in the humic-kerogen-rich Mingyuefeng Formation under favorable lowtemperature conditions during the late Paleocene-middle Eocene.The microbial gas subsequently leaked into the structurally and stratigraphically complex L1 trap with oil-associated sapropelic-type gas from the Yueguifeng source rock during the late Eocene-Oligocene uplifting event.A small amount of humic-kerogen-generated oil in the L1 gas pool is most likely to be derived from the underlying Lingfeng source rock.The detailed geological and geochemical considerations of source rocks are discussed to explain the accumulation history of hydrocarbon fluids in the L1 gas pool.This paper,therefore,represents an effort to increase the awareness of the pitfalls of various genetic diagrams,and an integrated geochemical and geological approach is required for hydrocarbonsource correlation.展开更多
By studying the light isotopic compositions of carbon,oxygen,and hydrogen,combined with previous research results on the ore-forming source of the deposit,the authors try to uncover its metallogenic origin.The δ^(18)...By studying the light isotopic compositions of carbon,oxygen,and hydrogen,combined with previous research results on the ore-forming source of the deposit,the authors try to uncover its metallogenic origin.The δ^(18)O and δ^(13)C isotope signatures of dolomite samples vary between 10.2 and 13.0‰,and between−7.2 and−5.2‰,respectively,implying that the carbon derives from the upper mantle.δD and δ^(18) O of quartz,biotite,and muscovite from diff erent ore veins of the deposit vary between−82 and−59‰,and between 11.6 and 12.4‰,respectively,implying that the metallogenic solutions are mainly magmatic.According to the relevant research results of many isotope geologists,the fractionation degree of hydrogen isotopes increases as the depth to the Earth’s core increases,and the more diff erentiated the hydrogen isotopes are,the lower their values will be.In other words,mantle-derived solutions can have extremely low hydrogen isotope values.This means that the δD‰ value−134 of the pyrrhotite sample numbered SD-34 in this article may indicate mantle-derived oreforming fl uid of the deposit.The formation of the Dashuigou tellurium deposit occurred between 91.71 and 80.19 Ma.展开更多
Hundreds of precipitation samples collected from meteorological stations in the Ordos Basin from January 1988 to December 2005 were used to set up a local meteoric water line and to calculate weighted average isotopic...Hundreds of precipitation samples collected from meteorological stations in the Ordos Basin from January 1988 to December 2005 were used to set up a local meteoric water line and to calculate weighted average isotopic compositions of modern precipitation. Oxygen and hydrogen isotopes, with averages of-7.8‰ and -53.0‰ for δ^18O and δD, respectively, are depleted in winter and rich in spring, and gradually decrease in summer and fall, illustrating that the seasonal effect is considerable. They also show that the isotopic difference between south portion and north portion of the Ordos Basin are not obvious, and the isotope in the middle portion is normally depleted. The isotope compositions of 32 samples collected from shallow groundwater (less than a depth of 150 m) in desert plateau range from -10.6‰ to -6.0‰ with an average of-8.4‰ for δ^18O and from -85‰ to -46‰ with an average of-63‰ for δD. Most of them are identical with modern precipitation. The isotope compositions of 22 middle and deep groundwaters (greater than a depth of 275 m) fall in ranges from -11.6‰ to -8.8‰ with an average of -10.2‰ for δ^18O and from -89‰ to -63‰ with an average of -76‰ for δD. The average values are significantly less than those of modern precipitation, illustrating that the middle and deep groundwaters were recharged at comparatively lower air temperatures. Primary analysis of ^14C shows that the recharge of the middle and deep groundwaters started at late Pleistocene. The isotopes of 13 lake water samples collected from eight lakes define a local evaporation trend, with a relatively flat slope of 3.77, and show that the lake waters were mainly fed by modern precipitation and shallow groundwater.展开更多
The intermetallic compound Zr1-xTixCo was prepared and its suitability for hydrogen storage was investigated. The alloys obtained by magnetic levitation melting with the composition of Zr1-xTixCo (x=0, 0.1, 0.2 and 0....The intermetallic compound Zr1-xTixCo was prepared and its suitability for hydrogen storage was investigated. The alloys obtained by magnetic levitation melting with the composition of Zr1-xTixCo (x=0, 0.1, 0.2 and 0.3, at.%) show single cubic phase by X-ray diffraction. A single sloping plateau was observed on each isothermal, and pressure-composition-temperature (PCT) measurement results show that the equilibrium hydrogen desorption pressure of Zr1-xTixCo alloy increases with increasing Ti content. The desorption temperatures for supplying 100 kPa hydrogen are about 665, 642, 621 and 614 K for ZrCo, Zr0.9Ti0.1Co, Zr0.8Ti0.2Co and Zr0.7Ti0.3Co alloy, respectively. Repeated hydrogen absorption and desorption cycles do not generate separated ZrCo, TiCo and ZrH2 phases, indicating that alloys have good thermal and hydrogen stabilization.展开更多
In order to recognize the impact of aqueous medium on gas yields and the kinetic behaviors of hydrogen isotope fractionation during organic matter thermal degradation, the gold tube apparatus was used to conduct therm...In order to recognize the impact of aqueous medium on gas yields and the kinetic behaviors of hydrogen isotope fractionation during organic matter thermal degradation, the gold tube apparatus was used to conduct thermal simulation experiments by mixing the nC18 with the water of different properties and proportions. The yields of natural gas components, the relation among hydrogen isotope composition of each component and the experimental temperatures vs. heating rates have been obtained, and the results indicate that under the higher temperature conditions, the hydrous experiment has obvious impact on gas yields, such as when more water is added, higher amounts of hydrocarbon gas and H2 are yielded, and the existence of water obviously prolongs the temperature interval with the existence of heavy hydrocarbon gas. It also shows that the hydrogen isotope of hydrocarbon gas generated by the hydrous experiment is obviously lighter than that generated by the anhydrous experiment, and with the increasing amount of added water, the δD value of hydrocarbon gas gradually decreases. Compared with gas yields, the variation of δD value is more sensitive to aqueous medium in the thermal simulation experiment. However, compared with the amount of the added water, the aqueous medium property has smaller impact on the gas yields, which still shows the inherit effect on hydrogen isotope composition of aqueous medium. Through the model simulation and the isotope fractionation behavior analysis, it is validated that the hydrogen isotope fractionation process can be well described by the chemical kinetic model. The difference of reaction fraction of normal methane and D-containing methane is large, corresponding to the same activation energy. The content of normal methane is obviously higher in the part with lower activation energy, while the content of D-containing methane is higher in the part with higher activation energy. Therefore, it will result in larger hydrogen isotope fractionation amplitude, and the δD values will be more sensitive to the variation of maturity. Meanwhile, the average activation energy of methane generation from nC18 in the hydrous experiment is higher than that in the anhydrous experiment, and the greater amount of added water, the larger the average activation energy of methane generation reaction. This has laid foundation for its exploratory application in the study of gas reservoir forming history and the gassource correlation, which indicates the research and application prospects in this orientation.展开更多
A gold tube simulation device was used to study the cleavage of representative compounds into gas.The goal of this study is to investigate hydrogen isotope composition change of gaseous hydrocarbons during maturity.Ga...A gold tube simulation device was used to study the cleavage of representative compounds into gas.The goal of this study is to investigate hydrogen isotope composition change of gaseous hydrocarbons during maturity.Gas chromatography and isotopic analyses were conducted to determine how the yield of natural gas components and their hydrogen isotopic composition were related to experimental temperature and heating rate.A chemical kinetic model for the generation of each component of the natural gas and for the hydrogen isotopic fractionation was established and calibrated based on the results.Results indicate that the hydrogen isotopic fractionation during the evolution of various gas-forming organic materials can be satisfactorily described by chemical kinetic models.During regular methane generation,the reactions at low-activation-energy region had a greater contribution than the high-activation-energy region.While the reactions with high-activation-energy region had greater contribution of deuterium-rich methane.Compared with carbon isotope fractionation,this results in a greater hydrogen isotopic fractionation,which is more sensitive to changes in maturity.This study lays a foundation for further investigations of genesis and maturity of natural gas provided by hydrogen isotopic fractionation.It also provides fundamental knowledge for investigating the filling history of natural gas reservoir and for identifying.展开更多
Crop root system plays an important role in the water cycle of the soil-plant-atmosphere continuum. In this study, com- bined isotope techniques, root length density and root cell activity analysis were used to invest...Crop root system plays an important role in the water cycle of the soil-plant-atmosphere continuum. In this study, com- bined isotope techniques, root length density and root cell activity analysis were used to investigate the root water uptake mechanisms of winter wheat (Triticum aesfivum L.) under different irrigation depths in the North China Plain. Both direct inference approach and multisource linear mixing model were applied to estimate the distribution of water uptake with depth in six growing stages. Results showed that winter wheat under land surface irrigation treatment (Ts) mainly absorbed water from 10-20 cm soil layers in the wintering and green stages (66.9 and 72.0%, respectively); 0-20 cm (57.0%) in the jointing stage; 0-40 (15.3%) and 80-180 cm (58.1%) in the heading stage; 60-80 (13.2%) and 180-220 cm (35.5%) in the filling stage; and 0-40 (46.8%) and 80-100 cm (31.0%) in the ripening stage. Winter wheat under whole soil layers irrigation treatment (Tw) absorbed more water from deep soil layer than Ts in heading, filling and ripening stages. Moreover, root cell activity and root length density of winter wheat under TW were significantly greater than that of Ts in the three stages. We concluded that distribution of water uptake with depth was affected by the availability of water sources, the root length density and root cell activity. Implementation of the whole soil layers irrigation method can affect root system distribution and thereby increase water use from deeper soil and enhance water use efficiency.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
The separation of hydrogen and deuterium by cryogenic adsorption was conducted, using the molecular sieve 5A as adsorbent, helium as the carder gas in a fixed column. The breakthrough curves of hydrogen, deuterium and...The separation of hydrogen and deuterium by cryogenic adsorption was conducted, using the molecular sieve 5A as adsorbent, helium as the carder gas in a fixed column. The breakthrough curves of hydrogen, deuterium and the mixture of two components in helium carder gas were measured, a separation factor, approximately 2, for the hydrogen-deuterium binary mixture was obtained. The equilibrium model was built for simulation of the concentration distribution for single hydrogen, deuterium and their mixture with helium carder in the fixed column, and the simulation compared well with the experimental results.展开更多
The variation of stable isotope ratios in natural waters provides valuable information that can be used to trace water movement. Evaporation plays a crucial role in determining the variation of stable isotopes. In thi...The variation of stable isotope ratios in natural waters provides valuable information that can be used to trace water movement. Evaporation plays a crucial role in determining the variation of stable isotopes. In this paper, several evaporation experiments were conducted in order to study the stable isotopic fractionation mechanism of water and analyze the influence of different temperatures on evaporation fractionation. Three group experiments of water evaporation under different temperatures and initial isotopic values were carried out. The results show that fractionation factors of hydrogen and oxygen may increase with temperature, and the average enrichment degree of hydrogen isotope D is 3.432 times that of oxygen isotope 18O. The results also show that the isotopic composition of the initial water has little influence on water evaporation fractionation, which is mainly affected by the state variables in the evaporation process, such as temperature. This research provides experimental data for further understanding the evaporation fractionation mechanism.展开更多
In this paper, by using an ingenious method, the hydrogen isotope solubilities and diffusivities in GWHER-1 stainless steel have been determined by a vacuum heating degassing approach at the temperature range of 597-1...In this paper, by using an ingenious method, the hydrogen isotope solubilities and diffusivities in GWHER-1 stainless steel have been determined by a vacuum heating degassing approach at the temperature range of 597-1022 K on a set of specimens with different sizes previously charged for 24 h under a hydrogen isotope pressure of 105 Pa in the temperature range of 800-1000 K. The permeabilities are then derived from the relation Φ = DKs. It is found D = 1.52 ×10^-6exp(-54100/RT), Ks = 2.2×10^-exp(-5400/RT) and Φ = 3.3 ×10^-12exp(-59500/RT) for hydrogen, where Ks (Sieverts' constant) is given in Pa^-1/2, D in m2.s^-1.Pa^-1/2, T in K and R=8.31 J.mol^-1.K^-1. By taking isotope effects into account, the corresponding Arrhenius relations for deuterium and tritium are also deduced.展开更多
基金financially aided by the National Natural Science Foundation of China(No.41002044)the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20102322120003)the Foundation for University Key Teacher of Heilongjiang Province of China(No.1251G003)
文摘In order to discuss the role and influence of water during the generation of natural gas,the participation mechanism of water during the evolution of organic matter and its influences were summarized.In addition,we carried out an anhydrous cracking experiment of oil extracted from the Feixianguan Formation source rock in a closed system,which led to the establishment of the kinetic models for describing carbon and hydrogen isotopic fractionation during gas generation from organic matter.The models were calibrated and then applied to the northeastern Sichuan Basin.By combining a series of gas generation experiments from octadecane pyrolysis without water or with distilled water in varying mass proportions,several results were proved:(1) the hydrogen isotopic composition of natural gas becomes lighter with the participation of formation water;(2) we can quantitatively study the hydrogen isotopic fractionation with the kinetic model for describing carbon isotopic fractionation; (3) more abundant and reliable geological information can be obtained through the combined application of carbon and hydrogen isotopic indices.
基金supported by the National Natural Science Foundation of China(Grants 49803002 and 40473007)Program for New Century Excellent Talents in University(NCET)the CAS-CNRS-CNR cooperative project.
文摘Hydrogen isotopic compositions of pyroxenes in peridotite xenoliths from the Nushan volcano, Anhui Province, SE China have been obtained using an ion probe (Cameca 1270). D/H ratios are constant within a single grain and among the different grains from the same sample. The lack of correlation between the D/H ratios and the hydrogen contents indicates that the hydrogen isotopic compositions are inherited from their mantle source. Combining with the δD values of coexisting amphiboles, it is inferred that the Nushan mantle experienced at least a two-stage metasomatic event. One was responsible for formation of amphiboles with extremely variable δD values, and the other was probably responsible for the high δD values (up to ?20‰) of some clinopyroxenes from peridotites, clinopyroxene and mica megacrysts. High δD values point to a subduction-related fluid being involved in one metasomatic event. The primary δD values (?90‰ to ?140‰) of the Nushan pyroxenes, together with data gleaned from the literature, suggest that the D/H ratios of the nominally anhydrous mineral reservoir might have differed from that of the other mantle hydrogen in being relatively depleted in D.
基金supported by the National Basic Research Program of China (2013CB955901)the National Natural Science Foundation of China (41073018)
文摘The hydrogen isotopic composition of plant leaf wax(δDwax) is used as an important tool for paleohydrologic reconstruction. However, the understanding of the relative importance of environmental and biological factors in determining δDwax values still remains incomplete. To identify the effects of soil moisture and plant physiology on δDwax values in an arid ecosystem, and to explore the implication of these values for paleoclimatic reconstruction, we measured δD values of soil water(δDwater) and δDwax values in surface soils along two distance transects extending from the lakeshore to wetland to dryland around Lake Qinghai and Lake Gahai on the northeast Qinghai-Tibetan Plateau. The results showed that the δDwater values were negatively correlated with soil water content(SWC)(R^2=0.9166), and ranged from –67‰ to –46‰ with changes in SWC from 6.2% to 42.1% in the arid areas of the Gangcha(GCh) and Gahai(GH) transects. This indicated that evaporative D-enrichment in soil water was sensitive to soil moisture in an arid ecosystem. Although the shift from grasses to shrubs with increasing aridity occurred in the arid area of the GH transect, the δDwax values in surface soils from the arid areas of the two transects still showed a negative correlation with SWC(R^2=0.6835), which may be due to the controls of primary evaporative D-enrichment in the soil water and additional transpirational D-enrichment in the leaf water on the δDwaxvalues. Our preliminary research suggested that δDwax values can potentially be applied as a paleo-humidity indicator on the northeast Qinghai-Tibetan Plateau.
基金supported by the National Key Research and Development program of China(Grant No.2021YFC3000604)National Natural Science Foundation of China(Grant Nos.42030305,42272257)sponsored by State Key Laboratory of Earthquake Dynamics,Institute of Geology,China Earthquake Administration(Grant No.LED2022B04)。
文摘The reconstruction of paleo-elevation serves a dual purpose to enhance our comprehension of geodynamic processes affecting terrestrial landforms and to contribute significantly to the interpretation of atmospheric circulation and biodiversity.The oxygen(δ~(18)O_w)and deuterium(δD_w)isotopes in atmospheric precipitation are systematically depleted with the increase of altitude,which are typical and widely applicated paleo-altimeters.The utilization of hydrogen isotope of hydrous silicate minerals within the shear zone system,volcanic glass,and plant leaf wax alkanes offers valuable insights for addressing evaporation and diagenesis.In this paper,we review the principle,application conditions,and influencing factors of the hydrogen isotope paleo-altimeter.In addition,we discuss the feasibility of utilizing this technique for quantitatively estimating the paleo-elevation of the southeastern Tibetan Plateau,where multiple shear zones extend over hundred kilometers parallel to the topographic gradient.
基金supported by the National Key Research and Development Program of China(2022YFE03170002)the National Natural Science Foundation of China(52071286 and U2030208)the Scientific Research Fund of Zhejiang Provincial Education Department(Y202353551).
文摘Hydrogen storage alloys(HSAs)are attracting widespread interest in the nuclear industry because of the generation of stable metal hydrides after tritium absorption,thus effectively preventing the leakage of radioactive tritium.Commonly used HSAs in the hydrogen isotopes field are Zr2M(M=Co,Ni,Fe)alloys,metallic Pd,depleted U,and ZrCo alloy.Specifically,Zr2M(M=Co,Ni,Fe)alloys are considered promising tritium-getter materials,and metallic Pd is utilized to separate and purify hydrogen isotopes.Furthermore,depleted U and ZrCo alloy are well suited for storing and delivering hydrogen isotopes.Notably,all the aforementioned HSAs need to modulate their hydrogen storage properties for complex operating conditions.In this review,we present a comprehensive overview of the reported modification methods applied to the above alloys.Alloying is an effective amelioration method that mainly modulates the properties of HSAs by altering their local geometrical/electronic structures.Besides,microstructural modifications such as nano-sizing and nanopores have been used to increase the specific surface area and active sites of metallic Pd and ZrCo alloys for enhancing de-/hydrogenation kinetics.The combination of metallic Pd with support materials can significantly reduce the cost and enhance the pulverization resistance.Moreover,the poisoning resistance of ZrCo alloy is improved by constructing active surfaces with selective permeability.Overall,the review is constructive for better understanding the properties and mechanisms of hydrogen isotope storage alloys and provides effective guidance for future modification research.
基金support from several sources,including the Backbone Teacher Training Program(10912-SJGG2021-04233)the Teaching Reform Project of Chengdu University of Technology(JG2130131)+1 种基金the University-Industry Collaborative Education Project,Ministry of Education,China(22097130210756)National Natural Science Foundation of China(42272129).
文摘The Yueguang gold deposit is located in Fengjia,Xinhua County,Hunan Province,South China.It represents a recently discovered small-scale gold deposit situated in the southwestern region of the Jiangnan Orogenic Belt,west of the Baimashan granitic batholith.In order to discern the characteristics of the ore-formingfluids,the underlying mineralization processes,and establish a foundation for the origin of the Yueguang gold depositfluid inclusion micro-thermometry,as well as quartz hydrogen and oxygen isotope analysis,have been carried out on samples obtained from various stages of mineralization.The hydrothermal miner-alization stages within the Yueguang gold deposit can be categorized into three stages:(i)the barren,pre-ore quartz-pyrite stage(Stage Ⅰ),the quartz-pyrite-gold stage(Stage Ⅱ),and the post-ore quartz-carbonate stage(Stage Ⅲ),with the second stage being the main mineralization stage.Thefluid inclusions identified in samples from the main min-eralization stage can predominantly be described with the NaCl–H_(2)O and CO_(2)–NaCl–H_(2)O systems.These inclusions display homogenization temperatures ranging from 158.8 to 334.9℃,and thefluid salinity ranges from 0.3%to 4.0%(wt.%NaCl equiv.).Laser Raman spectroscopy analysis of individual inclusions further reveals the presence of gas-phases such as CO_(2),CH_(4),and N_(2).Isotopic analysis indicatesδ^(18)Ofluid values ranging from 3.95 to 6.7‰ and δDH_(2)O values ranging from-71.9 to-55.7‰.These results indi-cate that the ore-formingfluid of the Yueguang gold deposit belongs to metamorphic hydrothermalfluids of middle-low temperature and low salinity.In the process of ore formation,gold is transported in the form of Au(HS)2-complexes,with gold deposition being driven byfluid immiscibility.Therefore,the Yueguang gold deposit is categorized as an orogenic gold deposit dominated by metamorphic hydrother-malfluid.It may become a new target for gold exploration in the Baimashan region,central Hunan Province.
基金supported jointly by National Natural Science Foundation of China (Grant No. 40703001) the "Western Doctors’ Project under the Western Light Program" sponsored by the Chinese Academy of Sciences
文摘The influences of water media on the hydrogen isotopic composition of organic-thermogenic natural gas were tested in three series of experiments on coal pyrolysis, with no water, deionized water (δDH2O-58‰), and seawater (δSDn2O=-4.8‰) added, respectively. The experimental results show that the productivities of H2 and CO2 obviously increased under hydrous conditions and that the productivity of CH4 also remarkably increased in the high-evolution phase of hydrous experiments. Water was involved in the chemical reaction of hydrocarbon generation, and then the hydrogen isotopic composition of methane was affected. There is a linear correlation between the hydrogen isotopic composition of methane and its productivity, as reflected in the three series of experiments. In the case of the same CH4 productivity, the hydrogen isotopic composition of the methane produced in anhydrous experiments was the heaviest, that of the methane produced in seawater-adding experiments came second, and that of the methane produced in deionized water-adding experiments was the ligbtest. The hydrogen isotopic composition of natural gas/methane is affected by the following factors: 1) the characteristics of hydrogen isotopic composition of organic matter in source rocks, 2) the thermal evolution extent of organic matter, and 3) fossil-water media in the natural gas-generation period. The experimental results show that the influence of the fossil-water medium in the natural gas-generation period was lower than that of the other factors.
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funded by the National Natural Science Foundation of China(NSFC)(Grant Nos.41225020 and41376049)National Programme on Global Change and Air-Sea Interaction(GASI-GEOGE-03)
文摘Recent studies suggest that the hydrogen and oxygen isotopic compositions of clay minerals can indicate paleoclimate.Here,we report mineralogy and stable isotopic records(d D and δ^(18)O_(OH))of a weathering profile located in the Fujian Province,aiming to validate whether hydroxyl stable isotopes can indicate paleo-precipitation and paleo-temperature.Our results indicate that the d D and δ^(18)O_(OH)changes in the kaolinite hydroxyl of the weathering profile are basically determined by the isotopic composition of paleo-meteoric water and paleotemperature,respectively.Nevertheless,whether the d D and δ^(18)O_(OH)of kaolinite can quantitatively indicate paleo-precipitation and paleo-temperature needs to be verified further,and especially,the structural oxygen isotopic composition that is the essential element for the kaolinite formation temperature calculation has to be constrained in future work.
基金The“Seven Year Action Plan”East China Sea Special Project of CNOOC under contract No.CNOOC-KJ 135 ZDXM39 SH02。
文摘The hydrocarbon gases in the L1 gas field of the Lishui-Jiaojiang Sag have been commonly interpreted to be an accumulation of pure sapropelic-type thermogenic gas.In this study,chemical components,stable isotopic compositions,and light hydrocarbons were utilized to shed light on the origins of the hydrocarbon fluids in the L1gas pool.The hydrocarbon fluids in the L1 gas pool are proposed to be a mixture of three unique components:mid-maturity oil from the middle Paleocene coastal marine Lingfeng source rock,oil-associated(late oil window)gas generated from the lower Paleocene lacustrine Yueguifeng source rock,and primary microbial gas from the paralic deposits of the upper Paleocene Mingyuefeng source rock.Here,for the first time,the hydrocarbon gases in the L1 gas pool are diagnosed as mixed oil-associated sapropelic-type gas and microbial gas via four pieces of principal evidence:(1)The abnormal carbon isotopic distributions of all methane homologues from C_(1)(CH_(4)or methane)to C_(5)(C_(5)H_(12)or pentane)shown in the Chung plot;(2)the diagnostic~(13)C-depleted C_(1)compared with the thermogenic sapropelic-type gas model,whileδ^(13)C_(2)(C_(2)H_(6)or ethane)andδ^(13)C_(3)(C_(3)H_(8)or propane)both fit perfectly;(3)the excellent agreement of the calculated carbon isotopic compositions of the pure thermogenic gas with the results of the thermal simulated gas from the type-II1 kerogen-rich Yueguifeng source rock;and(4)the oil-associated gas inferred from various binary genetic diagrams with an abnormally elevated gas oil ratio.Overall,the natural gases of the L1 gas pool were quantified in this study to comprise approximately 13%microbial gas,nearly 48%oil-associated sapropelic-type gas,and 39%of nonhydrocarbon gas.The microbial gas is interpreted to have been codeposited and entrained in the humic-kerogen-rich Mingyuefeng Formation under favorable lowtemperature conditions during the late Paleocene-middle Eocene.The microbial gas subsequently leaked into the structurally and stratigraphically complex L1 trap with oil-associated sapropelic-type gas from the Yueguifeng source rock during the late Eocene-Oligocene uplifting event.A small amount of humic-kerogen-generated oil in the L1 gas pool is most likely to be derived from the underlying Lingfeng source rock.The detailed geological and geochemical considerations of source rocks are discussed to explain the accumulation history of hydrocarbon fluids in the L1 gas pool.This paper,therefore,represents an effort to increase the awareness of the pitfalls of various genetic diagrams,and an integrated geochemical and geological approach is required for hydrocarbonsource correlation.
基金Support for this study was received from Orient Resources Ltd.in Canada,Wuhan Institute of Technology,China,and College of Earth Sciences,Jilin University,China.
文摘By studying the light isotopic compositions of carbon,oxygen,and hydrogen,combined with previous research results on the ore-forming source of the deposit,the authors try to uncover its metallogenic origin.The δ^(18)O and δ^(13)C isotope signatures of dolomite samples vary between 10.2 and 13.0‰,and between−7.2 and−5.2‰,respectively,implying that the carbon derives from the upper mantle.δD and δ^(18) O of quartz,biotite,and muscovite from diff erent ore veins of the deposit vary between−82 and−59‰,and between 11.6 and 12.4‰,respectively,implying that the metallogenic solutions are mainly magmatic.According to the relevant research results of many isotope geologists,the fractionation degree of hydrogen isotopes increases as the depth to the Earth’s core increases,and the more diff erentiated the hydrogen isotopes are,the lower their values will be.In other words,mantle-derived solutions can have extremely low hydrogen isotope values.This means that the δD‰ value−134 of the pyrrhotite sample numbered SD-34 in this article may indicate mantle-derived oreforming fl uid of the deposit.The formation of the Dashuigou tellurium deposit occurred between 91.71 and 80.19 Ma.
基金supported by the China Geological Survey and International Atomic Energy Agency.
文摘Hundreds of precipitation samples collected from meteorological stations in the Ordos Basin from January 1988 to December 2005 were used to set up a local meteoric water line and to calculate weighted average isotopic compositions of modern precipitation. Oxygen and hydrogen isotopes, with averages of-7.8‰ and -53.0‰ for δ^18O and δD, respectively, are depleted in winter and rich in spring, and gradually decrease in summer and fall, illustrating that the seasonal effect is considerable. They also show that the isotopic difference between south portion and north portion of the Ordos Basin are not obvious, and the isotope in the middle portion is normally depleted. The isotope compositions of 32 samples collected from shallow groundwater (less than a depth of 150 m) in desert plateau range from -10.6‰ to -6.0‰ with an average of-8.4‰ for δ^18O and from -85‰ to -46‰ with an average of-63‰ for δD. Most of them are identical with modern precipitation. The isotope compositions of 22 middle and deep groundwaters (greater than a depth of 275 m) fall in ranges from -11.6‰ to -8.8‰ with an average of -10.2‰ for δ^18O and from -89‰ to -63‰ with an average of -76‰ for δD. The average values are significantly less than those of modern precipitation, illustrating that the middle and deep groundwaters were recharged at comparatively lower air temperatures. Primary analysis of ^14C shows that the recharge of the middle and deep groundwaters started at late Pleistocene. The isotopes of 13 lake water samples collected from eight lakes define a local evaporation trend, with a relatively flat slope of 3.77, and show that the lake waters were mainly fed by modern precipitation and shallow groundwater.
文摘The intermetallic compound Zr1-xTixCo was prepared and its suitability for hydrogen storage was investigated. The alloys obtained by magnetic levitation melting with the composition of Zr1-xTixCo (x=0, 0.1, 0.2 and 0.3, at.%) show single cubic phase by X-ray diffraction. A single sloping plateau was observed on each isothermal, and pressure-composition-temperature (PCT) measurement results show that the equilibrium hydrogen desorption pressure of Zr1-xTixCo alloy increases with increasing Ti content. The desorption temperatures for supplying 100 kPa hydrogen are about 665, 642, 621 and 614 K for ZrCo, Zr0.9Ti0.1Co, Zr0.8Ti0.2Co and Zr0.7Ti0.3Co alloy, respectively. Repeated hydrogen absorption and desorption cycles do not generate separated ZrCo, TiCo and ZrH2 phases, indicating that alloys have good thermal and hydrogen stabilization.
基金supported by grants from the Natural Science Foundation of China(40972101,40572079)the National Key Basic Research and Development Program (2009CB219306)
文摘In order to recognize the impact of aqueous medium on gas yields and the kinetic behaviors of hydrogen isotope fractionation during organic matter thermal degradation, the gold tube apparatus was used to conduct thermal simulation experiments by mixing the nC18 with the water of different properties and proportions. The yields of natural gas components, the relation among hydrogen isotope composition of each component and the experimental temperatures vs. heating rates have been obtained, and the results indicate that under the higher temperature conditions, the hydrous experiment has obvious impact on gas yields, such as when more water is added, higher amounts of hydrocarbon gas and H2 are yielded, and the existence of water obviously prolongs the temperature interval with the existence of heavy hydrocarbon gas. It also shows that the hydrogen isotope of hydrocarbon gas generated by the hydrous experiment is obviously lighter than that generated by the anhydrous experiment, and with the increasing amount of added water, the δD value of hydrocarbon gas gradually decreases. Compared with gas yields, the variation of δD value is more sensitive to aqueous medium in the thermal simulation experiment. However, compared with the amount of the added water, the aqueous medium property has smaller impact on the gas yields, which still shows the inherit effect on hydrogen isotope composition of aqueous medium. Through the model simulation and the isotope fractionation behavior analysis, it is validated that the hydrogen isotope fractionation process can be well described by the chemical kinetic model. The difference of reaction fraction of normal methane and D-containing methane is large, corresponding to the same activation energy. The content of normal methane is obviously higher in the part with lower activation energy, while the content of D-containing methane is higher in the part with higher activation energy. Therefore, it will result in larger hydrogen isotope fractionation amplitude, and the δD values will be more sensitive to the variation of maturity. Meanwhile, the average activation energy of methane generation from nC18 in the hydrous experiment is higher than that in the anhydrous experiment, and the greater amount of added water, the larger the average activation energy of methane generation reaction. This has laid foundation for its exploratory application in the study of gas reservoir forming history and the gassource correlation, which indicates the research and application prospects in this orientation.
基金the National Natural Science Foundation of China(41672130,41772131)the National Oil and Gas Major Project(2016ZX05061-003-001,2016ZX05029002-002)+1 种基金the Sinopec Scientific and Technological Research Project(P17027-3)the Ministry of Education’s Independent Innovation Fund Project(14CX02224A)for financial support of this study。
文摘A gold tube simulation device was used to study the cleavage of representative compounds into gas.The goal of this study is to investigate hydrogen isotope composition change of gaseous hydrocarbons during maturity.Gas chromatography and isotopic analyses were conducted to determine how the yield of natural gas components and their hydrogen isotopic composition were related to experimental temperature and heating rate.A chemical kinetic model for the generation of each component of the natural gas and for the hydrogen isotopic fractionation was established and calibrated based on the results.Results indicate that the hydrogen isotopic fractionation during the evolution of various gas-forming organic materials can be satisfactorily described by chemical kinetic models.During regular methane generation,the reactions at low-activation-energy region had a greater contribution than the high-activation-energy region.While the reactions with high-activation-energy region had greater contribution of deuterium-rich methane.Compared with carbon isotope fractionation,this results in a greater hydrogen isotopic fractionation,which is more sensitive to changes in maturity.This study lays a foundation for further investigations of genesis and maturity of natural gas provided by hydrogen isotopic fractionation.It also provides fundamental knowledge for investigating the filling history of natural gas reservoir and for identifying.
基金supported by the National Natural Science Foundation of China(50979065,51109154 and 51249002)the Natural Science Foundation of Shanxi Province,China(2012021026-2)+2 种基金the Program for Science and Technology Development of Shanxi Province,China(20110311018-1)the Specialized Research Fund for the Doctoral Program of Higher Education,China(20111402120006,20121402110009)the Program for Graduate Student Education and Innovation of Shanxi Province,China(2015BY27)
文摘Crop root system plays an important role in the water cycle of the soil-plant-atmosphere continuum. In this study, com- bined isotope techniques, root length density and root cell activity analysis were used to investigate the root water uptake mechanisms of winter wheat (Triticum aesfivum L.) under different irrigation depths in the North China Plain. Both direct inference approach and multisource linear mixing model were applied to estimate the distribution of water uptake with depth in six growing stages. Results showed that winter wheat under land surface irrigation treatment (Ts) mainly absorbed water from 10-20 cm soil layers in the wintering and green stages (66.9 and 72.0%, respectively); 0-20 cm (57.0%) in the jointing stage; 0-40 (15.3%) and 80-180 cm (58.1%) in the heading stage; 60-80 (13.2%) and 180-220 cm (35.5%) in the filling stage; and 0-40 (46.8%) and 80-100 cm (31.0%) in the ripening stage. Winter wheat under whole soil layers irrigation treatment (Tw) absorbed more water from deep soil layer than Ts in heading, filling and ripening stages. Moreover, root cell activity and root length density of winter wheat under TW were significantly greater than that of Ts in the three stages. We concluded that distribution of water uptake with depth was affected by the availability of water sources, the root length density and root cell activity. Implementation of the whole soil layers irrigation method can affect root system distribution and thereby increase water use from deeper soil and enhance water use efficiency.
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.
文摘The separation of hydrogen and deuterium by cryogenic adsorption was conducted, using the molecular sieve 5A as adsorbent, helium as the carder gas in a fixed column. The breakthrough curves of hydrogen, deuterium and the mixture of two components in helium carder gas were measured, a separation factor, approximately 2, for the hydrogen-deuterium binary mixture was obtained. The equilibrium model was built for simulation of the concentration distribution for single hydrogen, deuterium and their mixture with helium carder in the fixed column, and the simulation compared well with the experimental results.
基金supported by the National Natural Science Foundation of China (Grant No. 50679024)the Innovation Program for College Graduate of Jiangsu Province of 2007 (Grant No. CX07B_130Z)
文摘The variation of stable isotope ratios in natural waters provides valuable information that can be used to trace water movement. Evaporation plays a crucial role in determining the variation of stable isotopes. In this paper, several evaporation experiments were conducted in order to study the stable isotopic fractionation mechanism of water and analyze the influence of different temperatures on evaporation fractionation. Three group experiments of water evaporation under different temperatures and initial isotopic values were carried out. The results show that fractionation factors of hydrogen and oxygen may increase with temperature, and the average enrichment degree of hydrogen isotope D is 3.432 times that of oxygen isotope 18O. The results also show that the isotopic composition of the initial water has little influence on water evaporation fractionation, which is mainly affected by the state variables in the evaporation process, such as temperature. This research provides experimental data for further understanding the evaporation fractionation mechanism.
基金Project supported by the National Natural Science Foundation of China (Grant No 10275017).
文摘In this paper, by using an ingenious method, the hydrogen isotope solubilities and diffusivities in GWHER-1 stainless steel have been determined by a vacuum heating degassing approach at the temperature range of 597-1022 K on a set of specimens with different sizes previously charged for 24 h under a hydrogen isotope pressure of 105 Pa in the temperature range of 800-1000 K. The permeabilities are then derived from the relation Φ = DKs. It is found D = 1.52 ×10^-6exp(-54100/RT), Ks = 2.2×10^-exp(-5400/RT) and Φ = 3.3 ×10^-12exp(-59500/RT) for hydrogen, where Ks (Sieverts' constant) is given in Pa^-1/2, D in m2.s^-1.Pa^-1/2, T in K and R=8.31 J.mol^-1.K^-1. By taking isotope effects into account, the corresponding Arrhenius relations for deuterium and tritium are also deduced.