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
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
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
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 isotope composition in precipitation has been widely considered as a tracer of monsoon activity.Compared with the coastal region,the monsoon margin usually has limited precipitation with large fluctuation and is u...The isotope composition in precipitation has been widely considered as a tracer of monsoon activity.Compared with the coastal region,the monsoon margin usually has limited precipitation with large fluctuation and is usually sensitive to climate change.The water resource management in the monsoon margin should be better planned by understanding the composition of precipitation isotope and its influencing factors.In this study,the precipitation samples were collected at five sampling sites(Baiyin City,Kongtong District,Maqu County,Wudu District,and Yinchuan City)of the monsoon margin in the northwest of China in 2022 to analyze the characteristics of stable hydrogen(δD)and oxygen(δ18O)isotopes.We analyzed the impact of meteorological factors(temperature,precipitation,and relative humidity)on the composition of precipitation isotope at daily level by regression analysis,utilized the Hybrid Single-Particle Lagrangian Integrated Trajectory(HYSPLIT)-based backward trajectory model to simulate the air mass trajectory of precipitation events,and adopted the potential source contribution function(PSCF)and concentration weighted trajectory(CWT)to analyze the water vapor sources.The results showed that compared with the global meteoric water line(GMWL),the slope of the local meteoric water line(LMWL;δD=7.34δ^(18)O-1.16)was lower,indicating the existence of strong regional evaporation in the study area.Temperature significantly contributed toδ18O value,while relative humidity had a significant negative effect onδ18O value.Through the backward trajectory analysis,we found eight primary locations that were responsible for the water vapor sources of precipitation in the study area,of which moisture from the Indian Ocean to South China Sea(ITSC)and the western continental(CW)had the greatest influence on precipitation in the study area.The hydrogen and oxygen isotopes in precipitation are significantly influenced by the sources and transportation paths of air mass.In addition,the results of PSCF and CWT analysis showed that the water vapor source areas were primarily distributed in the south and northwest direction of the study area.展开更多
The different reservoirs in deep Songliao Basin have non-homogeneous lithologies and include multiple layers with a high content of hydrogen gas.The gas composition and stable isotope characteristics vary significantl...The different reservoirs in deep Songliao Basin have non-homogeneous lithologies and include multiple layers with a high content of hydrogen gas.The gas composition and stable isotope characteristics vary significantly,but the origin analysis of different gas types has previously been weak.Based on the geochemical parameters of gas samples from different depths and the analysis of geological settings,this research covers the diverse origins of natural gas in different strata.The gas components are mainly methane with a small amount of C_(2+),and non-hydrocarbon gases,including nitrogen(N_(2)),hydrogen(H_(2)),carbon dioxide(CO_(2)),and helium(He).At greater depth,the carbon isotope of methane becomes heavier,and the hydrogen isotope points to a lacustrine sedimentary environment.With increasing depth,the origins of N_(2)and CO_(2)change gradually from a mixture of organic and inorganic to inorganic.The origins of hydrogen gas are complex and include organic sources,water radiolysis,water-rock(Fe^(2+)-containing minerals)reactions,and mantle-derived.The shales of Denglouku and Shahezi Formations,as source rocks,provide the premise for generation and occurrence of organic gas.Furthermore,the deep faults and fluid activities in Basement Formation control the generation and migration of mantle-derived gas.The discovery of a high content of H_(2)in study area not only reveals the organic and inorganic association of natural-gas generation,but also provides a scientific basis for the exploration of deep hydrogen-rich gas.展开更多
Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to wat...Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.展开更多
An in-house code,CONTHAC-3D,was developed to calculate and analyze thermal-hydraulic phenomena in containments during severe accidents.CONTHAC-3D is a three-dimensional computational fluid dynamics code that can be ap...An in-house code,CONTHAC-3D,was developed to calculate and analyze thermal-hydraulic phenomena in containments during severe accidents.CONTHAC-3D is a three-dimensional computational fluid dynamics code that can be applied to predict gas flow,diffusion,and steam condensation in a containment during a severe hypothetical accident,as well as to obtain an estimate of the local hydrogen concentration in various zones of the containment.CONTHAC-3D was developed using multiple models to simulate the features of the proprietary systems and equipment of HPR1000 and ACP100,such as the passive cooling system,passive autocatalytic recombiners and the passive air cooling system.To validate CONTHAC-3D,a GX6 test was performed at the Battelle Model Containment facility.The hydrogen concentration and temperature monitored by the GX6 test are accurately predicted by CONTHAC-3D.Subsequently,the hydrogen distribution in the HPR1000 containment during a severe accident was studied.The results show that the hydrogen removal rates calculated using CONTHAC-3D for different types of PARs agree well with the theoretical values,with an error of less than 1%.As the accident progresses,the hydrogen concentration in the lower compartment becomes higher than that in the large space,which implies that the lower compartment has a higher hydrogen risk than the dome and large space at a later stage of the accident.The amount of hydrogen removed by the PARs placed on the floor of the compartment is small;therefore,raising the installation height of these recombiners appropriately is recommended.However,we do not recommend installing all autocatalytic recombiners at high positions.The study findings in regard to the hydrogen distribution in the HPR1000 containment indicate that CONTHAC-3D can be applied to the study of hydrogen risk containment.展开更多
Understanding the hydrogen and oxygen stable isotope composition and characteristics of different water bodies in soil-plant-atmosphere continuum is of significance for revealing regional hydrological processes and wa...Understanding the hydrogen and oxygen stable isotope composition and characteristics of different water bodies in soil-plant-atmosphere continuum is of significance for revealing regional hydrological processes and water cycle mechanisms.In this study,we analyzed the stable isotopic composition,relationship and indicative significance of precipitation,soil water(0~100 cm depth)and xylem water of Qinghai spruce(Picea crassifolia)forest in the eastern Qilian Mountains,and explored the circulation process among different water bodies.The results show that the stable isotopes of precipitation vary greatly during the entire observation period.The values ofδ2H andδ^(18)O in the precipitation in the warm season are richer than those in the cold season,and the slope and intercept of local meteoric water line(LMWL,δ2H=6.79δ18O+7.13)are both smaller than global meteoric water line(GMWL,δ2H=8.17δ18O+10.56).The stable isotopes of soil water at different depths underwent different degrees of evaporative fractionation,and theδ18O andδ2H of shallow soil water varied greatly,while the deep soil water tended to be similar.The topsoil(0~10 cm)can respond quickly to precipitation,and the response of the deep soil has a time lag.In the whole growing season,0~30 cm and 60~100 cm soil water are the main water sources of Qinghai spruce.The water source of Qinghai spruce was from all soil layers in May and September,mainly from the shallow soil layer(0~30 cm)in August and October,and mainly from the deep soil layer(60~100 cm)in June and July.展开更多
Two-dimensional materials with active sites are expected to replace platinum as large-scale hydrogen production catalysts.However,the rapid discovery of excellent two-dimensional hydrogen evolution reaction catalysts ...Two-dimensional materials with active sites are expected to replace platinum as large-scale hydrogen production catalysts.However,the rapid discovery of excellent two-dimensional hydrogen evolution reaction catalysts is seriously hindered due to the long experiment cycle and the huge cost of high-throughput calculations of adsorption energies.Considering that the traditional regression models cannot consider all the potential sites on the surface of catalysts,we use a deep learning method with crystal graph convolutional neural networks to accelerate the discovery of high-performance two-dimensional hydrogen evolution reaction catalysts from two-dimensional materials database,with the prediction accuracy as high as 95.2%.The proposed method considers all active sites,screens out 38 high performance catalysts from 6,531 two-dimensional materials,predicts their adsorption energies at different active sites,and determines the potential strongest adsorption sites.The prediction accuracy of the two-dimensional hydrogen evolution reaction catalysts screening strategy proposed in this work is at the density-functional-theory level,but the prediction speed is 10.19 years ahead of the high-throughput screening,demonstrating the capability of crystal graph convolutional neural networks-deep learning method for efficiently discovering high-performance new structures over a wide catalytic materials space.展开更多
We present a quantum dynamics study on the isotope effects of hydro-gen transfer isomerization in the formic acid dimer,and this is achieved by multidimensional dy-namics calculations with an efficient quantum mechani...We present a quantum dynamics study on the isotope effects of hydro-gen transfer isomerization in the formic acid dimer,and this is achieved by multidimensional dy-namics calculations with an efficient quantum mechanical theoretical scheme developed by our group,on a full-dimensional neural network ab initio potential energy surface.The ground-state and fundamental tun-neling splittings for four deuterium isotopologues of formic acid dimer are considered,and the calculated results are in very good general agreement with the avail-able experimental measurements.Strong isotope effects are revealed,the mode-specific funda-mental excitation effects on the tunneling rate are evidently influenced by the deuterium sub-stitution of H atom with the substitution on the OH bond being more effective than on the CH bond.Our studies are helpful for acquiring a better understanding of isotope effects in the double-hydrogen transfer processes.展开更多
As typical quarternary copper-based chalcogenides,Cu–Zn–Sn–S nanocrystals(CZTS NCs)have emerged as a newfashioned electrocatalyst in hydrogen evolution reactions(HERs).Oleylamine(OM),a reducing surfactant and solve...As typical quarternary copper-based chalcogenides,Cu–Zn–Sn–S nanocrystals(CZTS NCs)have emerged as a newfashioned electrocatalyst in hydrogen evolution reactions(HERs).Oleylamine(OM),a reducing surfactant and solvent,plays a significant role in the assisting synthesis of CZTS NCs due to the ligand effect.Herein,we adopted a facile one-pot colloidal method for achieving the structure evolution of CZTS NCs from 2D nanosheets to 1D nanorods assisted through the continuous addition of OM.During the process,the mechanism of OM-induced morphology evolution was further discussed.When merely adding pure 1-dodecanethiol(DDT)as the solvent,the CZTS nanosheets were obtained.As OM was gradually added to the reaction,the CZTS NCs began to grow along the sides of the nanosheets and gradually shrink at the top,followed by the formation of stable nanorods.In acidic electrolytic conditions,the CZTS NCs with 1.0 OM addition display the optimal HER activity with a low overpotential of 561 m V at 10 m A/cm^(2) and a small Tafel slope of 157.6 m V/dec compared with other CZTS samples.The enhancement of HER activity could be attributed to the contribution of the synergistic effect of the diverse crystal facets to the reaction.展开更多
The catalytic hydrogenation of D-glucose over a 3 wt% Ru/C catalyst was studied varying the operating conditions in mild conditions range to optimize the obtention of D-sorbitol. The stirring speed, temperature, press...The catalytic hydrogenation of D-glucose over a 3 wt% Ru/C catalyst was studied varying the operating conditions in mild conditions range to optimize the obtention of D-sorbitol. The stirring speed, temperature, pressure, and initial glucose concentration were varied between 250 - 700 rpm, 343 - 383 K, 0.5 - 2 MPa, and 0.033 - 0.133 M, respectively. To verify the absence of mass transport limitations, the diffusion of reagents in the gas-liquid interface, the liquid-solid interface, and the internal diffusion in the particles were evaluated. Under the operating conditions studied, the reaction rate showed an order with respect to H<sub>2</sub> of 0.586 and with respect to glucose of 0.406. The kinetic data were adjusted using 3 general models and 19 different sub-models based on Langmuir-Hinshelwood-Hougen-Watson (LHHW) kinetics. Model 3a was the best one interpreting the aqueous phase hydrogenation of glucose (both reagents competitively adsorbed on the catalyst). The H<sub>2</sub> adsorption is dissociative and the rate-limiting step is the surface chemical reaction.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
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
To study the composition, affecting factors of the stable hydrogen isotopes of alkane gases and their application to identification of the natural gas origin and maturities, the chemical and isotopic compositions of 1...To study the composition, affecting factors of the stable hydrogen isotopes of alkane gases and their application to identification of the natural gas origin and maturities, the chemical and isotopic compositions of 118 gas samples of Carboniferous- Permian in the Ordos Basin, and of Triassic in the Sichuan Basin, combined with 68 gas samples from the Sinian and Cambrian reservoirs in the Sichuan Basin, and Ordovician and Siliurian reservoirs of Tarim Basin, are analyzed comprehensively. The following conclusions are obtained:(1) Natural gases in the study area and strata of the Ordos and Sichuan basins are dominated by alkane gases, and the dryness coefficients and maturities of the Carboniferous-Permian gases in the Ordos Basin are higher than the gases in the Triassic Xujiahe Formation of the Sichuan Basin, while the hydrogen isotopes of the latter ones are much enriched in 2H than the former.(2) The δ2HCH4-C1/C2+3 genetic identification diagram of natural gas was drawn, and the diagrams of hydrogen isotopic differences between the heavy alkane gases and methane vs. hydrogen isotopes of alkane gases can also be used in natural gas genetic identification.(3) The δ2HCH4-Ro formulas of coal-formed gas in different areas of the two basins are given, and the δ2HC2H6-δ2HCH4 is a new index for maturity, and the (δ2HC2H6-δ2HCH4)-Ro formula of the coal-formed gas can be used to calculate the maturity of the natural gas.(4) The stable hydrogen isotopes of alkane gases are affected by parent materials in source rocks, maturity, mixing and the aqueous medium conditions, among which the aqueous paleo-salinity is the key factor. To sum up, the hydrogen isotopes of alkane gases are affected by multiple factors, and they are significant to the identification of the origin, and maturity of natural gas, and the water environment during the deposition of source rocks.展开更多
According to the hydrochemical characteristics, hydrogen and oxygen isotope characteristics and the ratio of noble gas isotopes of the sandstone aquifer and basalt aquifer, this study calculated the recharge temperatu...According to the hydrochemical characteristics, hydrogen and oxygen isotope characteristics and the ratio of noble gas isotopes of the sandstone aquifer and basalt aquifer, this study calculated the recharge temperature and residence time of groundwater in the Weishan area of Wudalianchi, also calculating the contribution of noble gas components from different sources to the samples. Based on the characteristics of hydrogen and oxygen isotopes and noble gases Xe and Ne, the recharge altitude and recharge temperature of the two aquifers were estimated, and the recharge temperature fitting with the NGT model as verified, the results showing that the main recharge altitude of groundwater in the region was 500–600 m, the recharge temperature being 2–7°C. He_(eq) and He_(ea) of the samples have been simulated using the OD model, the content of radioactive ~4He in the crust being obtained, the groundwater ages under the two conditions(closed condition and open condition) both being simulated. The results show that groundwater from the sandstone layer water is older than groundwater from the basalt layer. Hydrochemical characteristics and noble gas isotope ratios indicate that in the basalt aquifer and sandstone aquifer in the Weishan area, in addition to atmospheric and crustal helium, there is also an input of mantle-derived helium. The fault constitutes the uplift channel for groundwater containings mantle components, which results in the mantle source composition in water samples near the fault being much higher than those form non-fault areas.展开更多
New oxygen and hydrogen isotope ratios of chert from middle, intraformational breccias, and upper breccia members of the Sixtymile Formation(SMF) in eastern Grand Canyon National Park(AZ) yield palaeoclimate estim...New oxygen and hydrogen isotope ratios of chert from middle, intraformational breccias, and upper breccia members of the Sixtymile Formation(SMF) in eastern Grand Canyon National Park(AZ) yield palaeoclimate estimates between 27 and 33℃. The isotopic compositions of cherts define a domain approximately parallel to the meteoric water line when plotted on a δD–δ-(18)O diagram; these data indicate that meteoric water was involved during formation of the chert. In thin section, the absence of interlocking mega quartz(〉35 lm) and silicafilled fractures and veins, along with preserved micromorphological silica fabrics, suggest that the chert has not been permeated by later hydrothermal fluids. Petrographic observations in thin section such as cyclic silica precipitation phases and glaebular micromorphologic fabrics lend support to the interpretation that meteoric waters were involved during chert precipitation. The post 742 Ma SMF has been correlated with diamictite(transition) beds of the Kingston Peak Formation(CA), which in turn have been interpreted to have been deposited during the Sturtian Ice Age(-750–700 Ma). Absence of facetted and striated clasts and other diagnostic glaciogenic features in the SMF,an unconformable contact with the stratigraphically older Chuar Group, coupled with warm palaeotemperature data inferred from stable isotope values of chert, tentatively suggest that deposition of sediment in the SMF likely did not take place during the Sturtian Ice Age.展开更多
Antarctica’s marginal seas are of great importance to atmosphere-ocean-ice interactions and are sensitive to global climate change.Multiple factors account for the freshwater budget in these regions,including glacier...Antarctica’s marginal seas are of great importance to atmosphere-ocean-ice interactions and are sensitive to global climate change.Multiple factors account for the freshwater budget in these regions,including glacier melting,seasonal formation/decay of sea ice,and precipitation.Hydrogen(H)and oxygen(O)isotopes represent useful proxies for determining the distribution and migration of water masses.We analyzed the H and O isotopic compositions of 190 seawater samples collected from the Amundsen Sea during the 34th Chinese Antarctic Research Expedition in 2017/2018.The upper-oceanic structure(<400 m)and freshwater(meteoric water and sea ice melt)distribution in the Amundsen Sea were identified based on conductivity-temperature-depth data and the H and O isotopic composition.Antarctic Surface Water,characterized as cold and fresh with low H and O isotopic ratios,was found distributed mainly in the upper~150 m between the Antarctic Slope Front and Polar Front,where it had been affected considerably by upwelled Upper Circumpolar Deep Water(UCDW)between 68°S and 71°S.A three-endmember(meteoric water,sea ice melt,and Circumpolar Deep Water)mixing model indicated that waters with relatively high proportions(>3%)of freshwater generally lie in the upper~50 m and extend from Antarctica to~65°S in the meridional direction(anomalously low freshwater proportion occurred between 68°S and 71°S).Winter Water mainly occupied the layer between 50 and 150 m south of 71°S in the western Amundsen Sea.The water structure and spatial distribution of freshwater in the upper Amundsen Sea were found influenced mainly by the rates of basal and surficial melting of ice shelves,seasonal alternation of sea ice melt/formation,wind forcing,and regional bathymetry.Owing to the distance between heavy sea ice boundary(HSIB)and ice shelves is much shorter in the western HSIB than the east HSIB,the western part of the heavy sea ice boundary includes a higher proportion of freshwater than the eastern region.This study,which highlighted the distribution and extent of freshwater derived from ice(ice shelves and sea ice)melt,provides important evidence that the offshore drift pathway of cold and fresh Antarctic continental shelf water is likely interrupted by upwelled UCDW in the Amundsen Sea.展开更多
The Ordovician was an important transitional period for global climate and organic evolution,the global was in the flood and glacial,Onganism was extinction(Zhan,2007;Trotter et al.,2008;Axel et al.,2010).Under the in...The Ordovician was an important transitional period for global climate and organic evolution,the global was in the flood and glacial,Onganism was extinction(Zhan,2007;Trotter et al.,2008;Axel et al.,2010).Under the influence展开更多
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 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supported by the National Natural Science Foundation of China(42161007)the Scientific Research Program for Higher Education Institutions of Gansu Province(2021B-081)the Natural Science Foundation of Gansu Province(22JR5RA074).
文摘The isotope composition in precipitation has been widely considered as a tracer of monsoon activity.Compared with the coastal region,the monsoon margin usually has limited precipitation with large fluctuation and is usually sensitive to climate change.The water resource management in the monsoon margin should be better planned by understanding the composition of precipitation isotope and its influencing factors.In this study,the precipitation samples were collected at five sampling sites(Baiyin City,Kongtong District,Maqu County,Wudu District,and Yinchuan City)of the monsoon margin in the northwest of China in 2022 to analyze the characteristics of stable hydrogen(δD)and oxygen(δ18O)isotopes.We analyzed the impact of meteorological factors(temperature,precipitation,and relative humidity)on the composition of precipitation isotope at daily level by regression analysis,utilized the Hybrid Single-Particle Lagrangian Integrated Trajectory(HYSPLIT)-based backward trajectory model to simulate the air mass trajectory of precipitation events,and adopted the potential source contribution function(PSCF)and concentration weighted trajectory(CWT)to analyze the water vapor sources.The results showed that compared with the global meteoric water line(GMWL),the slope of the local meteoric water line(LMWL;δD=7.34δ^(18)O-1.16)was lower,indicating the existence of strong regional evaporation in the study area.Temperature significantly contributed toδ18O value,while relative humidity had a significant negative effect onδ18O value.Through the backward trajectory analysis,we found eight primary locations that were responsible for the water vapor sources of precipitation in the study area,of which moisture from the Indian Ocean to South China Sea(ITSC)and the western continental(CW)had the greatest influence on precipitation in the study area.The hydrogen and oxygen isotopes in precipitation are significantly influenced by the sources and transportation paths of air mass.In addition,the results of PSCF and CWT analysis showed that the water vapor source areas were primarily distributed in the south and northwest direction of the study area.
基金supported by the National Natural Science Foundation of China(Grant No.42072168)the National Key R&D Program of China(Grant No.2019YFC0605405)the Fundamental Research Funds for the Central Universities(Grant No.2023ZKPYDC07)。
文摘The different reservoirs in deep Songliao Basin have non-homogeneous lithologies and include multiple layers with a high content of hydrogen gas.The gas composition and stable isotope characteristics vary significantly,but the origin analysis of different gas types has previously been weak.Based on the geochemical parameters of gas samples from different depths and the analysis of geological settings,this research covers the diverse origins of natural gas in different strata.The gas components are mainly methane with a small amount of C_(2+),and non-hydrocarbon gases,including nitrogen(N_(2)),hydrogen(H_(2)),carbon dioxide(CO_(2)),and helium(He).At greater depth,the carbon isotope of methane becomes heavier,and the hydrogen isotope points to a lacustrine sedimentary environment.With increasing depth,the origins of N_(2)and CO_(2)change gradually from a mixture of organic and inorganic to inorganic.The origins of hydrogen gas are complex and include organic sources,water radiolysis,water-rock(Fe^(2+)-containing minerals)reactions,and mantle-derived.The shales of Denglouku and Shahezi Formations,as source rocks,provide the premise for generation and occurrence of organic gas.Furthermore,the deep faults and fluid activities in Basement Formation control the generation and migration of mantle-derived gas.The discovery of a high content of H_(2)in study area not only reveals the organic and inorganic association of natural-gas generation,but also provides a scientific basis for the exploration of deep hydrogen-rich gas.
基金supported by the Australian Research Council (DE220100521 and DP200101217)supported by Fellow research grant of National University of Mongolia (No.P2021-4197)+2 种基金the support of Griffith University internal grantssupport from King Abdullah University of Science and Technology (KAUST)through the Ibn Rushd Postdoctoral Fellowship Awardsupport from the US Office of Naval Research (ONR),Office of Naval Research Global (ONRG)under the grant N62909-23-1-2035。
文摘Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.
文摘An in-house code,CONTHAC-3D,was developed to calculate and analyze thermal-hydraulic phenomena in containments during severe accidents.CONTHAC-3D is a three-dimensional computational fluid dynamics code that can be applied to predict gas flow,diffusion,and steam condensation in a containment during a severe hypothetical accident,as well as to obtain an estimate of the local hydrogen concentration in various zones of the containment.CONTHAC-3D was developed using multiple models to simulate the features of the proprietary systems and equipment of HPR1000 and ACP100,such as the passive cooling system,passive autocatalytic recombiners and the passive air cooling system.To validate CONTHAC-3D,a GX6 test was performed at the Battelle Model Containment facility.The hydrogen concentration and temperature monitored by the GX6 test are accurately predicted by CONTHAC-3D.Subsequently,the hydrogen distribution in the HPR1000 containment during a severe accident was studied.The results show that the hydrogen removal rates calculated using CONTHAC-3D for different types of PARs agree well with the theoretical values,with an error of less than 1%.As the accident progresses,the hydrogen concentration in the lower compartment becomes higher than that in the large space,which implies that the lower compartment has a higher hydrogen risk than the dome and large space at a later stage of the accident.The amount of hydrogen removed by the PARs placed on the floor of the compartment is small;therefore,raising the installation height of these recombiners appropriately is recommended.However,we do not recommend installing all autocatalytic recombiners at high positions.The study findings in regard to the hydrogen distribution in the HPR1000 containment indicate that CONTHAC-3D can be applied to the study of hydrogen risk containment.
基金supported by the National Natural Science Foundation of China(Grant Nos.41761047,41861040 and 41861034).
文摘Understanding the hydrogen and oxygen stable isotope composition and characteristics of different water bodies in soil-plant-atmosphere continuum is of significance for revealing regional hydrological processes and water cycle mechanisms.In this study,we analyzed the stable isotopic composition,relationship and indicative significance of precipitation,soil water(0~100 cm depth)and xylem water of Qinghai spruce(Picea crassifolia)forest in the eastern Qilian Mountains,and explored the circulation process among different water bodies.The results show that the stable isotopes of precipitation vary greatly during the entire observation period.The values ofδ2H andδ^(18)O in the precipitation in the warm season are richer than those in the cold season,and the slope and intercept of local meteoric water line(LMWL,δ2H=6.79δ18O+7.13)are both smaller than global meteoric water line(GMWL,δ2H=8.17δ18O+10.56).The stable isotopes of soil water at different depths underwent different degrees of evaporative fractionation,and theδ18O andδ2H of shallow soil water varied greatly,while the deep soil water tended to be similar.The topsoil(0~10 cm)can respond quickly to precipitation,and the response of the deep soil has a time lag.In the whole growing season,0~30 cm and 60~100 cm soil water are the main water sources of Qinghai spruce.The water source of Qinghai spruce was from all soil layers in May and September,mainly from the shallow soil layer(0~30 cm)in August and October,and mainly from the deep soil layer(60~100 cm)in June and July.
基金The authors are grateful for the financial support provided by the National Key Laboratory of Science and Technology on Micro/Nano Fabrication of China,the National Natural Science Foundation of China (No.21901157)the SJTU Global Strategic Partnership Fund (2020 SJTU-HUJI)the National Key R&D Program of China (2021YFC2100100).
文摘Two-dimensional materials with active sites are expected to replace platinum as large-scale hydrogen production catalysts.However,the rapid discovery of excellent two-dimensional hydrogen evolution reaction catalysts is seriously hindered due to the long experiment cycle and the huge cost of high-throughput calculations of adsorption energies.Considering that the traditional regression models cannot consider all the potential sites on the surface of catalysts,we use a deep learning method with crystal graph convolutional neural networks to accelerate the discovery of high-performance two-dimensional hydrogen evolution reaction catalysts from two-dimensional materials database,with the prediction accuracy as high as 95.2%.The proposed method considers all active sites,screens out 38 high performance catalysts from 6,531 two-dimensional materials,predicts their adsorption energies at different active sites,and determines the potential strongest adsorption sites.The prediction accuracy of the two-dimensional hydrogen evolution reaction catalysts screening strategy proposed in this work is at the density-functional-theory level,but the prediction speed is 10.19 years ahead of the high-throughput screening,demonstrating the capability of crystal graph convolutional neural networks-deep learning method for efficiently discovering high-performance new structures over a wide catalytic materials space.
基金supported by the National Natural Sci-ence Foundation of China(No.21973098 and No.22133003)the Beijing National Laboratory for Molecular SciencesJianwei Cao acknowledges the Youth Innovation Promotion Association CAS(No.2018045).
文摘We present a quantum dynamics study on the isotope effects of hydro-gen transfer isomerization in the formic acid dimer,and this is achieved by multidimensional dy-namics calculations with an efficient quantum mechanical theoretical scheme developed by our group,on a full-dimensional neural network ab initio potential energy surface.The ground-state and fundamental tun-neling splittings for four deuterium isotopologues of formic acid dimer are considered,and the calculated results are in very good general agreement with the avail-able experimental measurements.Strong isotope effects are revealed,the mode-specific funda-mental excitation effects on the tunneling rate are evidently influenced by the deuterium sub-stitution of H atom with the substitution on the OH bond being more effective than on the CH bond.Our studies are helpful for acquiring a better understanding of isotope effects in the double-hydrogen transfer processes.
基金partially supported by National Natural Science Foundation of China (12274021 and 62075005)。
文摘As typical quarternary copper-based chalcogenides,Cu–Zn–Sn–S nanocrystals(CZTS NCs)have emerged as a newfashioned electrocatalyst in hydrogen evolution reactions(HERs).Oleylamine(OM),a reducing surfactant and solvent,plays a significant role in the assisting synthesis of CZTS NCs due to the ligand effect.Herein,we adopted a facile one-pot colloidal method for achieving the structure evolution of CZTS NCs from 2D nanosheets to 1D nanorods assisted through the continuous addition of OM.During the process,the mechanism of OM-induced morphology evolution was further discussed.When merely adding pure 1-dodecanethiol(DDT)as the solvent,the CZTS nanosheets were obtained.As OM was gradually added to the reaction,the CZTS NCs began to grow along the sides of the nanosheets and gradually shrink at the top,followed by the formation of stable nanorods.In acidic electrolytic conditions,the CZTS NCs with 1.0 OM addition display the optimal HER activity with a low overpotential of 561 m V at 10 m A/cm^(2) and a small Tafel slope of 157.6 m V/dec compared with other CZTS samples.The enhancement of HER activity could be attributed to the contribution of the synergistic effect of the diverse crystal facets to the reaction.
文摘The catalytic hydrogenation of D-glucose over a 3 wt% Ru/C catalyst was studied varying the operating conditions in mild conditions range to optimize the obtention of D-sorbitol. The stirring speed, temperature, pressure, and initial glucose concentration were varied between 250 - 700 rpm, 343 - 383 K, 0.5 - 2 MPa, and 0.033 - 0.133 M, respectively. To verify the absence of mass transport limitations, the diffusion of reagents in the gas-liquid interface, the liquid-solid interface, and the internal diffusion in the particles were evaluated. Under the operating conditions studied, the reaction rate showed an order with respect to H<sub>2</sub> of 0.586 and with respect to glucose of 0.406. The kinetic data were adjusted using 3 general models and 19 different sub-models based on Langmuir-Hinshelwood-Hougen-Watson (LHHW) kinetics. Model 3a was the best one interpreting the aqueous phase hydrogenation of glucose (both reagents competitively adsorbed on the catalyst). The H<sub>2</sub> adsorption is dissociative and the rate-limiting step is the surface chemical reaction.
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.
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Supported by the China National Science and Technology Major Project(2016ZX05004-001)
文摘To study the composition, affecting factors of the stable hydrogen isotopes of alkane gases and their application to identification of the natural gas origin and maturities, the chemical and isotopic compositions of 118 gas samples of Carboniferous- Permian in the Ordos Basin, and of Triassic in the Sichuan Basin, combined with 68 gas samples from the Sinian and Cambrian reservoirs in the Sichuan Basin, and Ordovician and Siliurian reservoirs of Tarim Basin, are analyzed comprehensively. The following conclusions are obtained:(1) Natural gases in the study area and strata of the Ordos and Sichuan basins are dominated by alkane gases, and the dryness coefficients and maturities of the Carboniferous-Permian gases in the Ordos Basin are higher than the gases in the Triassic Xujiahe Formation of the Sichuan Basin, while the hydrogen isotopes of the latter ones are much enriched in 2H than the former.(2) The δ2HCH4-C1/C2+3 genetic identification diagram of natural gas was drawn, and the diagrams of hydrogen isotopic differences between the heavy alkane gases and methane vs. hydrogen isotopes of alkane gases can also be used in natural gas genetic identification.(3) The δ2HCH4-Ro formulas of coal-formed gas in different areas of the two basins are given, and the δ2HC2H6-δ2HCH4 is a new index for maturity, and the (δ2HC2H6-δ2HCH4)-Ro formula of the coal-formed gas can be used to calculate the maturity of the natural gas.(4) The stable hydrogen isotopes of alkane gases are affected by parent materials in source rocks, maturity, mixing and the aqueous medium conditions, among which the aqueous paleo-salinity is the key factor. To sum up, the hydrogen isotopes of alkane gases are affected by multiple factors, and they are significant to the identification of the origin, and maturity of natural gas, and the water environment during the deposition of source rocks.
基金financially supported by the China Geological Survey (No. 1212011220014)。
文摘According to the hydrochemical characteristics, hydrogen and oxygen isotope characteristics and the ratio of noble gas isotopes of the sandstone aquifer and basalt aquifer, this study calculated the recharge temperature and residence time of groundwater in the Weishan area of Wudalianchi, also calculating the contribution of noble gas components from different sources to the samples. Based on the characteristics of hydrogen and oxygen isotopes and noble gases Xe and Ne, the recharge altitude and recharge temperature of the two aquifers were estimated, and the recharge temperature fitting with the NGT model as verified, the results showing that the main recharge altitude of groundwater in the region was 500–600 m, the recharge temperature being 2–7°C. He_(eq) and He_(ea) of the samples have been simulated using the OD model, the content of radioactive ~4He in the crust being obtained, the groundwater ages under the two conditions(closed condition and open condition) both being simulated. The results show that groundwater from the sandstone layer water is older than groundwater from the basalt layer. Hydrochemical characteristics and noble gas isotope ratios indicate that in the basalt aquifer and sandstone aquifer in the Weishan area, in addition to atmospheric and crustal helium, there is also an input of mantle-derived helium. The fault constitutes the uplift channel for groundwater containings mantle components, which results in the mantle source composition in water samples near the fault being much higher than those form non-fault areas.
基金provided by a grant from Chuck Baltzer,Environmental Support Servicesgraciously awarded by Grand Canyon National Park officials
文摘New oxygen and hydrogen isotope ratios of chert from middle, intraformational breccias, and upper breccia members of the Sixtymile Formation(SMF) in eastern Grand Canyon National Park(AZ) yield palaeoclimate estimates between 27 and 33℃. The isotopic compositions of cherts define a domain approximately parallel to the meteoric water line when plotted on a δD–δ-(18)O diagram; these data indicate that meteoric water was involved during formation of the chert. In thin section, the absence of interlocking mega quartz(〉35 lm) and silicafilled fractures and veins, along with preserved micromorphological silica fabrics, suggest that the chert has not been permeated by later hydrothermal fluids. Petrographic observations in thin section such as cyclic silica precipitation phases and glaebular micromorphologic fabrics lend support to the interpretation that meteoric waters were involved during chert precipitation. The post 742 Ma SMF has been correlated with diamictite(transition) beds of the Kingston Peak Formation(CA), which in turn have been interpreted to have been deposited during the Sturtian Ice Age(-750–700 Ma). Absence of facetted and striated clasts and other diagnostic glaciogenic features in the SMF,an unconformable contact with the stratigraphically older Chuar Group, coupled with warm palaeotemperature data inferred from stable isotope values of chert, tentatively suggest that deposition of sediment in the SMF likely did not take place during the Sturtian Ice Age.
基金supported by the Natural Science Foundation of China(Grant no.41806229)the Ministry of Natural Resources of the People’s Republic of China(Impact and Response of Antarctic Seas to Climate Change,Grant no.IRASCC 02-04-01).
文摘Antarctica’s marginal seas are of great importance to atmosphere-ocean-ice interactions and are sensitive to global climate change.Multiple factors account for the freshwater budget in these regions,including glacier melting,seasonal formation/decay of sea ice,and precipitation.Hydrogen(H)and oxygen(O)isotopes represent useful proxies for determining the distribution and migration of water masses.We analyzed the H and O isotopic compositions of 190 seawater samples collected from the Amundsen Sea during the 34th Chinese Antarctic Research Expedition in 2017/2018.The upper-oceanic structure(<400 m)and freshwater(meteoric water and sea ice melt)distribution in the Amundsen Sea were identified based on conductivity-temperature-depth data and the H and O isotopic composition.Antarctic Surface Water,characterized as cold and fresh with low H and O isotopic ratios,was found distributed mainly in the upper~150 m between the Antarctic Slope Front and Polar Front,where it had been affected considerably by upwelled Upper Circumpolar Deep Water(UCDW)between 68°S and 71°S.A three-endmember(meteoric water,sea ice melt,and Circumpolar Deep Water)mixing model indicated that waters with relatively high proportions(>3%)of freshwater generally lie in the upper~50 m and extend from Antarctica to~65°S in the meridional direction(anomalously low freshwater proportion occurred between 68°S and 71°S).Winter Water mainly occupied the layer between 50 and 150 m south of 71°S in the western Amundsen Sea.The water structure and spatial distribution of freshwater in the upper Amundsen Sea were found influenced mainly by the rates of basal and surficial melting of ice shelves,seasonal alternation of sea ice melt/formation,wind forcing,and regional bathymetry.Owing to the distance between heavy sea ice boundary(HSIB)and ice shelves is much shorter in the western HSIB than the east HSIB,the western part of the heavy sea ice boundary includes a higher proportion of freshwater than the eastern region.This study,which highlighted the distribution and extent of freshwater derived from ice(ice shelves and sea ice)melt,provides important evidence that the offshore drift pathway of cold and fresh Antarctic continental shelf water is likely interrupted by upwelled UCDW in the Amundsen Sea.
文摘The Ordovician was an important transitional period for global climate and organic evolution,the global was in the flood and glacial,Onganism was extinction(Zhan,2007;Trotter et al.,2008;Axel et al.,2010).Under the influence