In recent years,terbium radioisotopes have been investigated for their potential therapeutic and diagnostic applications in nuclear medicine.This study aimed to investigate the production of ^(152) Tb and ^(155) Tb by...In recent years,terbium radioisotopes have been investigated for their potential therapeutic and diagnostic applications in nuclear medicine.This study aimed to investigate the production of ^(152) Tb and ^(155) Tb by alpha-induced reactions in detail,with a specific focus on determining the optimum production parameters and testing existing nuclear models.Given the limited number of experiments conducted on reactions related to terbium isotope production,it is necessary to perform theoretical calculations of cross sections over a wide energy range to gain a detailed understanding of terbium isotope production.To achieve this objective,the cross sections of the ^(151)Eu(α,n)^(154) Tb reactions were calculated up to 60 MeV using the TALYS computer code with 432 different combinations of optical model parameters,level density,and strength function models.The theoretical reaction cross-section results were compared with the experimental results in the literature.The best input parameters were determined using the Threshold Logic Unit method,and these parameters were used in all isotope production calculations.Once the optimal model combination was determined,the total activity production and isotopic fraction of ^(152) Tb and ^(155) Tb isotopes were calculated in detail for beam energies of 17–50 MeV,different irradiation times,and varying ^(151) Eu and ^(153) Eu target thicknesses.展开更多
CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and sec...CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and secondary sulfides within the Aguas Zarcas(CM2)chondrite,investigating their formation mechanisms based on their morphology,textures,and compositions.Moreover,we infer the formation temperatures of the sulfides from 230 to 500℃ for primary and from 100 to 135℃ for secondary.We select representative grains and conduct Fe isotope measurements on them.The primary sulfides with δ^(56/54)Fe ranging from -2.44‰ to +0.69‰are associated with sulfidesilicate melt segregation,while secondary sulfides with δ^(56/54)Fe values between -1.83‰ and -0.14‰ are linked to aqueous alteration.Overall,the Ni content of the grains is positively correlated with δ^(56/54)Fe.It might be related to the changes in crystal structure and chemical bond lengths due to the increase in nickel content.Fe isotopes provide a new perspective on sulfide formation and the evolution of a carbonaceous chondrite parent body.展开更多
Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural ga...Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural gases.We used the GC-Py-GC-IRMS method to study TSR and obtained a novel finding related to intramolecular carbon isotope fractionation in natural propane.The results show that theΔC-T(δ^(13)C_(central)-13 C_(terminal))andδ^(13)C_(central)values significantly increased to 44.7‰and 11.9‰,respectively,with increasing TSR alteration.In contrast,the 13 C_(terminal)values of propane remained largely unaltered by the TSR reaction.This difference in position-specific isotope fractionation can be attributed to the central carbon’s reactivity being higher than that of terminal carbon during TSR.In sum,the results indicate that theδ^(13)C_(terminal)values of propane can serve as robust indicators for source rock identification of natural gas altered by post-generation reactions such as TSR and anaerobic microbial oxidation.展开更多
We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-...We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.展开更多
Based on geochemical data from natural gas samples across spring water systems and sedimentary basins,including Songliao,Bohai Bay,Sanshui,Sichuan,Ordos,Tarim and Ying-Qiong,this paper systematically compares the geoc...Based on geochemical data from natural gas samples across spring water systems and sedimentary basins,including Songliao,Bohai Bay,Sanshui,Sichuan,Ordos,Tarim and Ying-Qiong,this paper systematically compares the geochemical compositions of abiogenic versus biogenic gases.Emphasis is placed on the diagnostic signatures of abiogenic gases in terms of gas composition,and carbon,hydrogen and helium isotopes.The main findings are as follows.(1)In hydrothermal spring systems,abiogenic alkane gases are extremely scarce.Methane concentrations are typically less than 1%,with almost no detectable C^(2+)hydrocarbons.The gas is dominantly composed of CO_(2),while N_(2)is the major component in a few samples.(2)Abiogenic alkane gases display distinct isotopic signatures,including enriched methane carbon isotopic compositions(δ^(13)C_(1)>-25‰generally),complete carbon isotopic reversal(δ^(13)C_(1)>δ^(13)C_(2)>δ^(13)C_(3)>δ^(13)C_(4)),and enriched helium isotope(R/Ra>0.5,CH_(4)/^(3)He≤10^(6)generally).(3)The hydrogen isotopic composition of abiogenic alkane gases may be characterized by a positive sequence(δD_(1)<δD_(2)<δD_(3)),or a complete reversal(δD_(1)>δD_(2)>δD_(3)),or a V-shaped distribution(δD_(1)>δD_(2),δD_(2)<δD_(3)).The hydrogen isotopic compositions of methane generally show limited variation(about 9‰),possibly due to hydrogen isotopic exchange with connate water.(4)In terms of identifying gas origin,CH_(4)/^(3)He-R/Ra andδ^(13)CCO_(2)-R/Ra charts are more effective than CO_(2)/^(3)He-R/Ra chart.These new geological insights provide theoretical clues and diagnostic charts for the genetic identification of natural gas and further research on abiogenic gases.展开更多
Medical isotopes are the foundation material for nuclear medicine and are primarily produced through in-reactor irradia-tion.Neutron spectrum regulation is the main technical approach for enhancing the production of m...Medical isotopes are the foundation material for nuclear medicine and are primarily produced through in-reactor irradia-tion.Neutron spectrum regulation is the main technical approach for enhancing the production of medical isotopes,and it requires determining the optimal neutron spectrum and quantifying the values of neutrons in different energy regions.We calculated the neutron energy region values for 20 medical isotopes(^(14)C,^(32)P,^(47)Sc,^(60)Co,^(64)Cu,^(67)Cu,^(89)Sr,^(90)Y,^(99)Mo,^(125)I,^(131)I,^(153)Sm,^(161)Tb,^(166)Ho,^(177)Lu,^(186)Re,^(188)Re,^(92)Ir,^(225)Ac,and ^(252)Cf).The entire energy range was divided into 238 energy regions to improve the energy spectrum resolution,and both fast and thermal reactors were simulated to enhance universal applicability.A dataset of neutron energy region values across the entire energy range was built,which identifies the positive and negative-energy regions and guides the neutron spectrum regulation process during in-reactor medical isotope produc-tion.We conducted neutron spectrum regulation based on this dataset,which effectively improved the production efficiency of medical isotopes and demonstrated the correctness and feasibility of the dataset.展开更多
Hydrocarbons are one of the important fluids within the Earth's crust,and different biotic and abitoic processes can generate hydrocarbon during geological periods.Tracing the sources and sinks of hydrocarbons can...Hydrocarbons are one of the important fluids within the Earth's crust,and different biotic and abitoic processes can generate hydrocarbon during geological periods.Tracing the sources and sinks of hydrocarbons can help us better understand the carbon cycle of the earth.In this study,an improved approach of adsorbed hydrocarbons extraction from sediments was established.The improved thermal desorption approach,compound-specific isotope analysis and position-specific isotope analysis were integrated to investigate the molecular and intramolecular isotope fractionation between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The isotopic compositions of the terminal position carbon of propane(δ^(13)C_(terminal))serves as a correlation indicator between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The tight sandstone gas from the Turpan-Hami Basin is a first case study for the application of this novel method to trace hydrocarbon origins.The results showed that the hydrocarbons in the tight sandstone gases in the study area most likely originated from humic organic matter(typeⅢkerogen)at an early mature stage.δ^(13)C_(terminal)values of the thermally desorbed propane gases from different source rocks were distinguishable and the values of the tight sandstone gases significantly overlap with those of the Lower Jurassic Sangonghe source rocks,suggesting their genetic relationship.Overall,the results provided novel position-specific carbon isotopic constraints on origins of hydrocarbons.展开更多
The Metal Stable Isotope Geochemistry Laboratory(MSIGL)at the University of Science and Technology of China has developed state-of-the-art analytical methods for twelve stable isotope systems,including Mg,Si,V,Fe,Cu,Z...The Metal Stable Isotope Geochemistry Laboratory(MSIGL)at the University of Science and Technology of China has developed state-of-the-art analytical methods for twelve stable isotope systems,including Mg,Si,V,Fe,Cu,Zn,Rb,Sr,Ag,Cd,Ba,and U.Geological and biological samples were first digested by acid dissolution or alkali dissolution.The target element was subsequently purified by the column chromatography method.A Neptune Plus MC-ICP-MS was used to measure isotope compositions and the isotope bias caused during measurements was calibrated by standard bracketing and/or the double spike method.The analytical procedure was carefully checked to ensure the high precision and accuracy of the data.Here,we summarized the protocol of these established methods and compiled the standard data measured at our lab as well as those reported in literature.This comprehensive dataset can serve as a reliable benchmark for calibration,method validation,and quality assurance in metal stable isotope analyses.展开更多
Stable Sr isotopic composition(δ^(88/86)Sr)can be used to study magmatic processes,but their fractionation mechanism during magmatic evolution remains unclear.To understand the fractionation behaviors of the stable S...Stable Sr isotopic composition(δ^(88/86)Sr)can be used to study magmatic processes,but their fractionation mechanism during magmatic evolution remains unclear.To understand the fractionation behaviors of the stable Sr isotopes during magmatism,we report theδ^(88/86)Sr values of the Huili granitic pluton,which was subjected to intensive crystal-melt separation.The Huili pluton consists of K-feldspar granite and more evolved albite granite,and the albite granite exhibits significantly higherδ^(88/86)Sr values(+0.36‰to+0.52‰)than that of K-feldspar granite(+0.11‰to+0.25‰).K-feldspar,which contributes most of the Sr budget of the K-feldspar granite,has slightly lowerδ^(88/86)Sr values(−0.01‰to+0.17‰)than the whole rock.Theδ^(88/86)Sr variation of the Huili granites can be explained by separation of melt from K-feldspar-dominated crystals,because crystallization of K-feldspar can result in heavy Sr isotopic composition of the extracted interstitial melt.Stable Sr and Ba isotopic ratios in the Huili granites are highly coupled toward the heavy direction,refl ecting their similar element partitioning and isotope fractionation behaviors between the crystalline K-feldspar and melt.This study indicates that melt extraction plays a key role in granitic magma evolution.展开更多
Significant progress has been made in exploring shale gas resources in the middle-upper Permian strata of western Hubei.However,the unclear geochemical characteristics and origins of the gas have hindered a comprehens...Significant progress has been made in exploring shale gas resources in the middle-upper Permian strata of western Hubei.However,the unclear geochemical characteristics and origins of the gas have hindered a comprehensive understanding of reservoir evolution and have constrained integrated resource development.This study involved a 28-h desorption experiment in which gases released from shales of the Dalong and Gufeng Formations were systematically collected for compositional and carbon—hydrogen isotope analyses.Comparing the compositional and geochemical characteristics of the desorbed gases and investigating their genetic origins resulted in four main findings:(1)Gas composition during the middle stage of desorption,excluding H_(2)S,best represents the original reservoir fluid,with component variations linked to adsorption and diffusion capacities.(2)Both shales display similar gas compositions with trace H_(2)S;the Dalong shale contains lower CH_(4),CO_(2),and H_(2)S but higher C_(2)H_(6)and N_(2).(3)Carbon and hydrogen isotopes indicate oil-type thermogenic gases,with carbon isotope reversal reflecting tectonic uplift,depressurization,and the mixing of primary kerogen-derived and secondary oil-/condensate-derived gases.(4)N_(2)likely originates from ammonium-bearing silicate decomposition,CO_(2)is mainly inorganic,from thermal carbonate decomposition with minor organic contribution,and H_(2)S may result from oil cracking or thermochemical sulfate reduction.This study provides a comprehensive record of the fluid characteristics of middle-upper Permian shale gas reservoirs and enhances the understanding of their formation and evolution.展开更多
In this study,we systematically explored the environmental significance of stable isotope characteristics and the controlling factors of precipitation stable isotopes in the source region of the Three Rivers(SRTR),the...In this study,we systematically explored the environmental significance of stable isotope characteristics and the controlling factors of precipitation stable isotopes in the source region of the Three Rivers(SRTR),the transitional zone of the Qinghai-Tibet Plateau in China.A total of 862 precipitation samples were collected from six fixed-point sampling locations between 2019 and 2021 in the SRTR.In June,the values of hydrogen(δD)and oxygen(δ^(18)O)stable isotopes were most enriched.The deuterium-excess(d-excess)in atmospheric precipitation was>0 in the SRTR;however,the maximum value of d-excess occurred in October.Moreover,the slopes of the local meteoric water line(LMWL)for Dari,Zaduo,Maduo,Qumalai,and Tuotuohe sites were lower than those of the global met-eoric water line(GMWL).In contrast,the slope of the LMWL for Zhimenda was higher than that of the GMWL.The altitude effects of oxygen(δ^(18)O)and hydrogen(δD)isotopes of precipitation were 0.70‰/100 m and 5.22‰/100 m,respectively.When the temperature was≤5℃,there was a significant temperature effect on stable oxygen isotope of precipitation(0.24‰/℃,P<0.05).Furthermore,even a minor increase(1%)in the weight of raindrops after falling results in a 0.82%rise in the evaporation enrichment rate ofδ^(18)O.Success-ive precipitation events also had a substantial influence on precipitation in the transitional region of the Qinghai-Tibet Plateau.The res-ults of this study provide a theoretical basis for revealing the impact mechanism of precipitation in the transitional zone of the Qinghai-Tibet Plateau under a warming climate.展开更多
Although the demand of ^(10)B separation has arisen in the 1930s,^(10)B/^(11)B are among the most difficult isotopes to separate due to the extremely similar relative atomic mass.Herein,we report an efficient separati...Although the demand of ^(10)B separation has arisen in the 1930s,^(10)B/^(11)B are among the most difficult isotopes to separate due to the extremely similar relative atomic mass.Herein,we report an efficient separation of ^(10)B isotopologue by engineering amino-galloyl synergistic materials via a selective adsorption and isotope exchange reaction,achieving a record-high single-stage separation factor of 1.048 with ^(10)B abundance up to 21.42%.^(11)B MAS NMR results and DFT calculations reveal that the galloyl groups exhibit inherent high affinity for B(OH)4-,forming tetrahedral sp^(3) B-galloyl complexes.The relatively higher ^(10)B–O bond energy of ^(10)B-galloyl complexes facilitates the isotope exchange between11B in B-galloyl complexes and ^(10)B in B(OH)_(3).Flowthrough dynamic separation in fixed-bed demonstrates the feasibility and potential of large-scale deployment of this method in real-world,suggesting a promising avenue for the exploitation of more efficient enrichment of ^(10)B for the sustainable nuclear energy and biomedical research.展开更多
Nitrogen-15 isotope-modified compounds are widely used in medicine, pharmacology, agriculture and various fields of science and their nomenclature is gradually increasing. Their widespread use depends on the availabil...Nitrogen-15 isotope-modified compounds are widely used in medicine, pharmacology, agriculture and various fields of science and their nomenclature is gradually increasing. Their widespread use depends on the availability of inexpensive and simple isotope analysis methods. The present article is an attempt to determine the nitrogen-15 isotope content directly in organic compounds without their conversion. The general principle of possibility of determination of the isotopes of nitrogen directly in organic compounds is proposed. Based on the study of mass-spectra of Carbamide Carbonyldiamide, isocyanic acid and nitrobenzene the mass peaks are selected, by which it is possible to determine the atomic fraction of the isotopes of nitrogen. The respective formulas are proposed.展开更多
The growth trajectory of hailstones within clouds has remained elusive due to the inability to trace them directly,impeding the comprehension of their underlying growth mechanisms.This study investigated hailstone ver...The growth trajectory of hailstones within clouds has remained elusive due to the inability to trace them directly,impeding the comprehension of their underlying growth mechanisms.This study investigated hailstone vertical growth trajectories by detecting the stable isotope signatures(2H and 18O compositions)of different shells in 27 hailstones from 9hailstorms,which allowed us to capture the ambient temperature during hailstone growth.The vertical growth trajectories were obtained by comparing the isotopic compositions of water condensate in clouds,derived from the Adiabatic Model,with those measured in hailstones.Although hailstone growth was primarily observed in the–10°C to–30°C temperature layer,the embryo formation height and subsequent growth trajectories significantly varied among hailstones.Embryos formed over a wide range of temperatures(–8.7°C to–33.4°C);four originated at temperatures above–15°C and 16originated at temperatures below–20°C,suggesting ice nuclei composed of bioproteins and mineral dust,respectively.Among the 27 measured hailstones,3 exhibited minimal vertical movement,16 exhibited a monotonic rise or fall,and the remaining 8 exhibited alternating up-down trajectories;only one experienced“recycling”during up-down drifting.Trajectory analysis revealed that similar-sized hailstones from a single storm tended to form at similar heights,whereas those larger than 25 mm in diameter exhibited at least one period of upward growth.Vertical trajectories derived from isotopic analysis were corroborated by radar hydrometeor observations.展开更多
Biomarker and stable carbon isotope analyses are presented for the Garau Formation of the Cretaceous Age,an important source rock in western Iran,to reveal its potential as an oilprone source rock.The C_(28)/C_(29)ste...Biomarker and stable carbon isotope analyses are presented for the Garau Formation of the Cretaceous Age,an important source rock in western Iran,to reveal its potential as an oilprone source rock.The C_(28)/C_(29)sterane ratio value range(0.72 to 0.83)of bitumen samples from the formation suggests that they were likely formed during phytoplankton blooms.Sterane,hopane,and isoprenoid/n-alkane ratios indicate that the formation's organic matter predominantly consists of algae,and bacteria,accompanied by some reworked material derived from higher plants.Due to the predominance of anoxic conditions and the actions of sulfate-reducing bacteria,the bitumen present is enriched with sulfur compounds.The percentages of saturates,aromatics,and nitrogen-sulfuroxygen(NSO)fractions in the bitumen samples classify them as naphthenic oils.Isotope analysis reveals that biodegradation and water-washing have reduced the concentrations of some volatile saturates and low molecular weight aromatics in the bitumen samples.These actions have resulted in distinctiveδ^(13)C values for the formation's kerogen and bitumen fractions.The formation's organic matter has been subjected to high-temperature thermal regimes and has entered the oil-generation window at the sampled localities,with vitrinite reflectance(%R_(C))varying between 0.7%and 0.75%.展开更多
Coal power plants annually generate quantities of byproducts that release environmentally hazardous heavy metals like Cd and Pb.Understanding the behavior and spatiotemporal impacts on soils of these releases is cruci...Coal power plants annually generate quantities of byproducts that release environmentally hazardous heavy metals like Cd and Pb.Understanding the behavior and spatiotemporal impacts on soils of these releases is crucial for pollution control.This study investigated the concentrations and isotope ratios of Cd/Pb in combustion byproducts,depositions and soils collected froma coal-fired power plant or its surrounding area.The pulverized fuel ash(PFA)and desulfurized gypsum(DG)exhibited heavier Cd isotopes withΔ^(114)Cd values of 0.304‰and 0.269‰,respectively,while bottom ash(BA)showed lighter Cd isotopes(Δ^(114)CdBA-coal=–0.078‰),compared to feed coal.We proposed a two-stage condensation process that governs the distribution of Cd/Pb,including accumulation on PFA and DG within electrostatic precipitators and desulfurization unit,as well as condensation onto fine particles upon release from the stack.Emissions from combustion and large-scale transport make a significant contribution to deposition,while the dispersion of Cd/Pb in deposition is primarily influenced by the prevailing wind patterns.However,the distribution of Cd/Pb in soils not only exhibit predominant wind control but is also potentially influenced by the resuspension of long-term storage byproducts.The power plant significantly contributes to soil in the NW–N–NE directions,even at a considerable distance(66%–79%),demonstrating its pervasive impact on remote regions along these orientations.Additionally,based on the vertical behavior in the profile,we have identified that Cd tends to migrate downward through leaching,while variations in Pb respond to the historical progression of dust removal.展开更多
Prediction of production decline and evaluation of the adsorbed/free gas ratio are critical for determining the lifespan and production status of shale gas wells.Traditional production prediction methods have some sho...Prediction of production decline and evaluation of the adsorbed/free gas ratio are critical for determining the lifespan and production status of shale gas wells.Traditional production prediction methods have some shortcomings because of the low permeability and tightness of shale,complex gas flow behavior of multi-scale gas transport regions and multiple gas transport mechanism superpositions,and complex and variable production regimes of shale gas wells.Recent research has demonstrated the existence of a multi-stage isotope fractionation phenomenon during shale gas production,with the fractionation characteristics of each stage associated with the pore structure,gas in place(GIP),adsorption/desorption,and gas production process.This study presents a new approach for estimating shale gas well production and evaluating the adsorbed/free gas ratio throughout production using isotope fractionation techniques.A reservoir-scale carbon isotope fractionation(CIF)model applicable to the production process of shale gas wells was developed for the first time in this research.In contrast to the traditional model,this model improves production prediction accuracy by simultaneously fitting the gas production rate and δ^(13)C_(1) data and provides a new evaluation method of the adsorbed/free gas ratio during shale gas production.The results indicate that the diffusion and adsorption/desorption properties of rock,bottom-hole flowing pressure(BHP)of gas well,and multi-scale gas transport regions of the reservoir all affect isotope fractionation,with the diffusion and adsorption/desorption parameters of rock having the greatest effect on isotope fractionation being D∗/D,PL,VL,α,and others in that order.We effectively tested the universality of the four-stage isotope fractionation feature and revealed a unique isotope fractionation mechanism caused by the superimposed coupling of multi-scale gas transport regions during shale gas well production.Finally,we applied the established CIF model to a shale gas well in the Sichuan Basin,China,and calculated the estimated ultimate recovery(EUR)of the well to be 3.33×10^(8) m^(3);the adsorbed gas ratio during shale gas production was 1.65%,10.03%,and 23.44%in the first,fifth,and tenth years,respectively.The findings are significant for understanding the isotope fractionation mechanism during natural gas transport in complex systems and for formulating and optimizing unconventional natural gas development strategies.展开更多
Precipitation isotopes(δ^(18)O and δ^(2)H)are closely related to meteorological conditions for precipitation generation and the initial state of water vapor source areas,and are essential to the study of the regiona...Precipitation isotopes(δ^(18)O and δ^(2)H)are closely related to meteorological conditions for precipitation generation and the initial state of water vapor source areas,and are essential to the study of the regional hydrological cycle.The deuterium excess(d-excess)indicates deviation in isotope fractionation during evaporation and can trace water vapor sources.This study analyzed 443 precipitation samples collected from the Gannan Plateau,China in 2022 to assess precipitation isotope variations and their driving factors.Water vapor sources were evaluated using the Hybrid Single-Particle Lagrangian Integrated Trajectory(HYSPLIT),Concentration Weighted Trajectory(CWT),and Potential Source Contribution Factor(PSCF)models.Results showed that precipitation isotope values showed significant spatial and temporal variations on the Gannan Plateau.Temporally,precipitation isotope values peaked in June(when evaporation dominated)and minimized in March(depletion effect of air masses in the westerly wind belt).Spatially,the isotope values showed a distribution pattern of"high in the east and low in the west",which was mainly regulated by the differences in altitude and local meteorological conditions.Compared with the global meteoric water line(GMWL)with equation of δ^(2)H=8.00δ^(18)O+10.00,the slope and intercept of local meteoric water line(LMWL)for precipitation on the Gannan Plateau were smaller(7.49 and 7.63,respectively),reflecting the existence of a stronger secondary evaporation effect under the clouds in the region.The sources of water vapor on the Gannan Plateau showed significant seasonality and spatial heterogeneity.Specifically,the westerly belt and monsoon were the main water vapor transport paths at each sampling point,with Central Asian continental water vapor dominating in spring(53.49%),Indian Ocean water vapor dominating in summer(52.53%),Atlantic Ocean water vapor dominating in autumn(46.74%),and Atlantic Ocean and Mediterranean Sea water vapor dominating in winter(42.30%and 33.68%,respectively).Changes in the intensity of convective activity and Outgoing Longwave Radiation(OLR)affected the enrichment of isotopic values,which exhibited the same change trends as δ^(18)O.During the precipitation process,the δ^(18)O value first decreased and then increased.During the initial and final stages of precipitation process,precipitation was mainly influenced by continental air masses,while during the middle stage,it was controlled by marine air masses.The systematic research on precipitation isotopes and water vapor sources is important for climate change research and extreme precipitation prediction on the Gannan Plateau and other similar areas.展开更多
Sulfur isotopes of S-bearing materials are powerful tools to trace various geological processes and sulfur sources in earth sciences,especially in ore deposits where sulfide-sulfate pair coprecipitates widely.However,...Sulfur isotopes of S-bearing materials are powerful tools to trace various geological processes and sulfur sources in earth sciences,especially in ore deposits where sulfide-sulfate pair coprecipitates widely.However,in-situ S isotope determination of barite is challenging without natural matrix-matched reference material.In this study,we present two natural barite reference materials(1-YS and 294-YS)for in-situ sulfur isotopic analysis.Independent LA-MC-ICP-MS laboratories were utilized to test theδ34S micron-scale homogeneity of 1-YS and 294-YS barites that have 2s repeatabilities of better than±0.45‰and±0.41‰,respectively.Meanwhile,the in-situ analysis results are consistent with the results of the bulk analysis by GS-IRMS within uncertainty.The grand meanδ~(34)S values of 1-YS(13.37‰±0.42‰,2s)and 294-YS(14.38‰±0.44‰,2s)are the final recommended values obtained from four independent laboratories.All the results confirm the suitability of 1-YS and 294-YS barite used as calibration materials with respect to in-situ S isotopic analysis.Moreover,the new developed barite reference materials were used as matrix-matched standard to calibrate the barite samples from the Huayangchuan carbonatite-hosted U-polymetallic deposit(Qinling orogenic belt,western China)to obtainδ34S values.Utilizing the temperaturedependentδ34S fractionation of barite-pyrite pair,we calculate the formation temperature of barite(i.e.,506 to 537°C)and theδ34S value of mineralizing fluid(i.e.,-7.11‰to-7.59‰)in the Huayangchuan deposit.The results indicate an involvement of sedimentary sulfur,presumably acting as a potential uranium source(e.g.,upper crustal materials)for the giant Huayangchuan deposit.展开更多
The Cretaceous Koum Basin is a rift-related half-graben in northern Cameroon,which constitutes a portion of the Yola Arm of the Upper Benue Trough.This study presents the first comprehensive dataset combining mineral-...The Cretaceous Koum Basin is a rift-related half-graben in northern Cameroon,which constitutes a portion of the Yola Arm of the Upper Benue Trough.This study presents the first comprehensive dataset combining mineral-ogical,bulk-rock geochemical,and stable C-H-O isotopic data for dark-gray,finegrained mudstones from the basin,providing new insights into its sediment source,paleoenvironment,and geodynamic setting.The mudstones primarily consist of phyllosilicates(~8.6%),feldspars(~30.5%),carbonates(~13.7%),and minor iron oxides(~2.7%),with vermiculite,illite,and kaolinite as the main clay minerals.The presence of analcime,ankerite,and dolomite suggests low-grade metamorphism and/or hydrothermal alteration.Fe_(2)O_(3)/K_(2)O(1.52-6.40)and SiO_(2)/Al_(2)O_(3)(2.97-4.68)ratios classify the mudstones as compositionally immature shales(ICV~1.64)with low-moderate chemical weathering(CIA~56.35;PIA~59.74;R^(3+)/R^(3+)+R^(2+)+M^(+)~0.51).Trace element ratios(Th/Sc~1.70,Zr/Sc~1.33,La/Sc~6.30,La/Th~4.14)indicate an intermediate igneous provenance from a continental crustal source.Paleoenviron-mental proxies suggest deposition in a dynamic basin environment marked by fluctuating redox(C org/P:0.21-178.34)and salinity(Sr/Ba:0.34-3.25;N-values:48-35.92)conditions,ranging from oxic to anoxic and brackish to saline.Major element data(SiO_(2) vs.Al_(2)O_(3)+K_(2)O+Na_(2)O)indicate a semi-arid regime,while Paleoclimatic indicators such as Sr/Cu(1.88-37.47)and C-values(0.12-0.93)suggests alter-nating humid and arid conditions.Notably,stable isotope data,reported here for the first time in the Koum Basin,reveal a predominantly terrestrial,fluvial-deltaic C_(3) plant source for organic carbon(δ^(13)C-25.2‰ to -35.2‰)and complex fluid-rock interactions involving meteoric and magmatic-metamorphic fluids under a warm,equatorial climate(δ^(18)O+3.6‰to +24.9‰,δ^(2)H-104‰ to-50‰).The combined mineralogical,geochemical,and isotopic data point to deposition in a tectonically active continental arc setting,with contributions from ocean island arc and passive margin sources.展开更多
文摘In recent years,terbium radioisotopes have been investigated for their potential therapeutic and diagnostic applications in nuclear medicine.This study aimed to investigate the production of ^(152) Tb and ^(155) Tb by alpha-induced reactions in detail,with a specific focus on determining the optimum production parameters and testing existing nuclear models.Given the limited number of experiments conducted on reactions related to terbium isotope production,it is necessary to perform theoretical calculations of cross sections over a wide energy range to gain a detailed understanding of terbium isotope production.To achieve this objective,the cross sections of the ^(151)Eu(α,n)^(154) Tb reactions were calculated up to 60 MeV using the TALYS computer code with 432 different combinations of optical model parameters,level density,and strength function models.The theoretical reaction cross-section results were compared with the experimental results in the literature.The best input parameters were determined using the Threshold Logic Unit method,and these parameters were used in all isotope production calculations.Once the optimal model combination was determined,the total activity production and isotopic fraction of ^(152) Tb and ^(155) Tb isotopes were calculated in detail for beam energies of 17–50 MeV,different irradiation times,and varying ^(151) Eu and ^(153) Eu target thicknesses.
基金supported by the National Science Foundation of China(Nos.42225202 and 41827802)。
文摘CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and secondary sulfides within the Aguas Zarcas(CM2)chondrite,investigating their formation mechanisms based on their morphology,textures,and compositions.Moreover,we infer the formation temperatures of the sulfides from 230 to 500℃ for primary and from 100 to 135℃ for secondary.We select representative grains and conduct Fe isotope measurements on them.The primary sulfides with δ^(56/54)Fe ranging from -2.44‰ to +0.69‰are associated with sulfidesilicate melt segregation,while secondary sulfides with δ^(56/54)Fe values between -1.83‰ and -0.14‰ are linked to aqueous alteration.Overall,the Ni content of the grains is positively correlated with δ^(56/54)Fe.It might be related to the changes in crystal structure and chemical bond lengths due to the increase in nickel content.Fe isotopes provide a new perspective on sulfide formation and the evolution of a carbonaceous chondrite parent body.
基金supported by the Helium Enrichment and Detection in Natural Gas Reservoirs Related to Oil and Gas Fields project(Grant No.2025ZD1010500)the Deep Earth Probe and Mineral Resources Exploration―National Science and Technology Major Project.-。
文摘Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural gases.We used the GC-Py-GC-IRMS method to study TSR and obtained a novel finding related to intramolecular carbon isotope fractionation in natural propane.The results show that theΔC-T(δ^(13)C_(central)-13 C_(terminal))andδ^(13)C_(central)values significantly increased to 44.7‰and 11.9‰,respectively,with increasing TSR alteration.In contrast,the 13 C_(terminal)values of propane remained largely unaltered by the TSR reaction.This difference in position-specific isotope fractionation can be attributed to the central carbon’s reactivity being higher than that of terminal carbon during TSR.In sum,the results indicate that theδ^(13)C_(terminal)values of propane can serve as robust indicators for source rock identification of natural gas altered by post-generation reactions such as TSR and anaerobic microbial oxidation.
基金supported in part by the National Key R&D Program of China (Contract Nos.2023YFA1606500,2024YFE0109800,and 2024YFE0110400)Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB34010000)+5 种基金the Gansu Key Project of Science and Technology (Grant No.23ZDGA014)the Guangdong Major Project of Basic and Applied Basic Research (Grant No.2021B0301030006)the National Natural Science Foundation of China (Grant Nos.12105328,W2412040,12475126,12422507,12035011,12375118,12435008,and W2412043)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-002)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant Nos.2020409 and 2023439)the Russian Science Foundation (Grant No.25-42-00003)。
文摘We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.
基金Supported by PetroChina Science and Technology Research and Technology Development Project(2021DJ0502)Open Research Project of Key Laboratory of Shale Gas Resources Exploration,Ministry of Natural Resources(Chongqing Institute of Geology and Mineral Resources)(KLSGE-2023).
文摘Based on geochemical data from natural gas samples across spring water systems and sedimentary basins,including Songliao,Bohai Bay,Sanshui,Sichuan,Ordos,Tarim and Ying-Qiong,this paper systematically compares the geochemical compositions of abiogenic versus biogenic gases.Emphasis is placed on the diagnostic signatures of abiogenic gases in terms of gas composition,and carbon,hydrogen and helium isotopes.The main findings are as follows.(1)In hydrothermal spring systems,abiogenic alkane gases are extremely scarce.Methane concentrations are typically less than 1%,with almost no detectable C^(2+)hydrocarbons.The gas is dominantly composed of CO_(2),while N_(2)is the major component in a few samples.(2)Abiogenic alkane gases display distinct isotopic signatures,including enriched methane carbon isotopic compositions(δ^(13)C_(1)>-25‰generally),complete carbon isotopic reversal(δ^(13)C_(1)>δ^(13)C_(2)>δ^(13)C_(3)>δ^(13)C_(4)),and enriched helium isotope(R/Ra>0.5,CH_(4)/^(3)He≤10^(6)generally).(3)The hydrogen isotopic composition of abiogenic alkane gases may be characterized by a positive sequence(δD_(1)<δD_(2)<δD_(3)),or a complete reversal(δD_(1)>δD_(2)>δD_(3)),or a V-shaped distribution(δD_(1)>δD_(2),δD_(2)<δD_(3)).The hydrogen isotopic compositions of methane generally show limited variation(about 9‰),possibly due to hydrogen isotopic exchange with connate water.(4)In terms of identifying gas origin,CH_(4)/^(3)He-R/Ra andδ^(13)CCO_(2)-R/Ra charts are more effective than CO_(2)/^(3)He-R/Ra chart.These new geological insights provide theoretical clues and diagnostic charts for the genetic identification of natural gas and further research on abiogenic gases.
基金sponsored by the National Natural Science Foundation of China(No.12305190)Lingchuang Research Project of China National Nuclear Corporation(CNNC).
文摘Medical isotopes are the foundation material for nuclear medicine and are primarily produced through in-reactor irradia-tion.Neutron spectrum regulation is the main technical approach for enhancing the production of medical isotopes,and it requires determining the optimal neutron spectrum and quantifying the values of neutrons in different energy regions.We calculated the neutron energy region values for 20 medical isotopes(^(14)C,^(32)P,^(47)Sc,^(60)Co,^(64)Cu,^(67)Cu,^(89)Sr,^(90)Y,^(99)Mo,^(125)I,^(131)I,^(153)Sm,^(161)Tb,^(166)Ho,^(177)Lu,^(186)Re,^(188)Re,^(92)Ir,^(225)Ac,and ^(252)Cf).The entire energy range was divided into 238 energy regions to improve the energy spectrum resolution,and both fast and thermal reactors were simulated to enhance universal applicability.A dataset of neutron energy region values across the entire energy range was built,which identifies the positive and negative-energy regions and guides the neutron spectrum regulation process during in-reactor medical isotope produc-tion.We conducted neutron spectrum regulation based on this dataset,which effectively improved the production efficiency of medical isotopes and demonstrated the correctness and feasibility of the dataset.
基金financially supported by the National Natural Science Foundation of China(Grant No.42102202)U.S.Department of Energy Geosciences program(DE-SC0016271)。
文摘Hydrocarbons are one of the important fluids within the Earth's crust,and different biotic and abitoic processes can generate hydrocarbon during geological periods.Tracing the sources and sinks of hydrocarbons can help us better understand the carbon cycle of the earth.In this study,an improved approach of adsorbed hydrocarbons extraction from sediments was established.The improved thermal desorption approach,compound-specific isotope analysis and position-specific isotope analysis were integrated to investigate the molecular and intramolecular isotope fractionation between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The isotopic compositions of the terminal position carbon of propane(δ^(13)C_(terminal))serves as a correlation indicator between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The tight sandstone gas from the Turpan-Hami Basin is a first case study for the application of this novel method to trace hydrocarbon origins.The results showed that the hydrocarbons in the tight sandstone gases in the study area most likely originated from humic organic matter(typeⅢkerogen)at an early mature stage.δ^(13)C_(terminal)values of the thermally desorbed propane gases from different source rocks were distinguishable and the values of the tight sandstone gases significantly overlap with those of the Lower Jurassic Sangonghe source rocks,suggesting their genetic relationship.Overall,the results provided novel position-specific carbon isotopic constraints on origins of hydrocarbons.
基金the National Science Foundation of China(Nos.42273007 and 42473008)the Distinguished Young Scholars of Anhui,China(No.2408085J021)。
文摘The Metal Stable Isotope Geochemistry Laboratory(MSIGL)at the University of Science and Technology of China has developed state-of-the-art analytical methods for twelve stable isotope systems,including Mg,Si,V,Fe,Cu,Zn,Rb,Sr,Ag,Cd,Ba,and U.Geological and biological samples were first digested by acid dissolution or alkali dissolution.The target element was subsequently purified by the column chromatography method.A Neptune Plus MC-ICP-MS was used to measure isotope compositions and the isotope bias caused during measurements was calibrated by standard bracketing and/or the double spike method.The analytical procedure was carefully checked to ensure the high precision and accuracy of the data.Here,we summarized the protocol of these established methods and compiled the standard data measured at our lab as well as those reported in literature.This comprehensive dataset can serve as a reliable benchmark for calibration,method validation,and quality assurance in metal stable isotope analyses.
基金supported by National Natural Science Foundation of China(42473009).
文摘Stable Sr isotopic composition(δ^(88/86)Sr)can be used to study magmatic processes,but their fractionation mechanism during magmatic evolution remains unclear.To understand the fractionation behaviors of the stable Sr isotopes during magmatism,we report theδ^(88/86)Sr values of the Huili granitic pluton,which was subjected to intensive crystal-melt separation.The Huili pluton consists of K-feldspar granite and more evolved albite granite,and the albite granite exhibits significantly higherδ^(88/86)Sr values(+0.36‰to+0.52‰)than that of K-feldspar granite(+0.11‰to+0.25‰).K-feldspar,which contributes most of the Sr budget of the K-feldspar granite,has slightly lowerδ^(88/86)Sr values(−0.01‰to+0.17‰)than the whole rock.Theδ^(88/86)Sr variation of the Huili granites can be explained by separation of melt from K-feldspar-dominated crystals,because crystallization of K-feldspar can result in heavy Sr isotopic composition of the extracted interstitial melt.Stable Sr and Ba isotopic ratios in the Huili granites are highly coupled toward the heavy direction,refl ecting their similar element partitioning and isotope fractionation behaviors between the crystalline K-feldspar and melt.This study indicates that melt extraction plays a key role in granitic magma evolution.
基金supported by the Hubei Provincial Natural Science Foundation of China(Grant No.2022CFB490,2024AFD381)Science and Technology Project of Hubei Geological Bureau(Grant No.KJ2024-2,KJ2025-14)Open Fund of Technology Innovation Center for Shale oil and Gas Accumulation Theory and Engineering in Southern Complex Structural Area,China Geological Survey(Grant No.SOG-202410).
文摘Significant progress has been made in exploring shale gas resources in the middle-upper Permian strata of western Hubei.However,the unclear geochemical characteristics and origins of the gas have hindered a comprehensive understanding of reservoir evolution and have constrained integrated resource development.This study involved a 28-h desorption experiment in which gases released from shales of the Dalong and Gufeng Formations were systematically collected for compositional and carbon—hydrogen isotope analyses.Comparing the compositional and geochemical characteristics of the desorbed gases and investigating their genetic origins resulted in four main findings:(1)Gas composition during the middle stage of desorption,excluding H_(2)S,best represents the original reservoir fluid,with component variations linked to adsorption and diffusion capacities.(2)Both shales display similar gas compositions with trace H_(2)S;the Dalong shale contains lower CH_(4),CO_(2),and H_(2)S but higher C_(2)H_(6)and N_(2).(3)Carbon and hydrogen isotopes indicate oil-type thermogenic gases,with carbon isotope reversal reflecting tectonic uplift,depressurization,and the mixing of primary kerogen-derived and secondary oil-/condensate-derived gases.(4)N_(2)likely originates from ammonium-bearing silicate decomposition,CO_(2)is mainly inorganic,from thermal carbonate decomposition with minor organic contribution,and H_(2)S may result from oil cracking or thermochemical sulfate reduction.This study provides a comprehensive record of the fluid characteristics of middle-upper Permian shale gas reservoirs and enhances the understanding of their formation and evolution.
基金Under the auspices of the National Science Foundation for Distinguished Young Scholars(No.42425107)the Science and Technology Project of Gansu Province(No.24JRRA168,23ZDKA017)+1 种基金the Key Talent Project in Gansu Province(No.2025RCXM057)National Nature Science Foundation of China(No.42107063)。
文摘In this study,we systematically explored the environmental significance of stable isotope characteristics and the controlling factors of precipitation stable isotopes in the source region of the Three Rivers(SRTR),the transitional zone of the Qinghai-Tibet Plateau in China.A total of 862 precipitation samples were collected from six fixed-point sampling locations between 2019 and 2021 in the SRTR.In June,the values of hydrogen(δD)and oxygen(δ^(18)O)stable isotopes were most enriched.The deuterium-excess(d-excess)in atmospheric precipitation was>0 in the SRTR;however,the maximum value of d-excess occurred in October.Moreover,the slopes of the local meteoric water line(LMWL)for Dari,Zaduo,Maduo,Qumalai,and Tuotuohe sites were lower than those of the global met-eoric water line(GMWL).In contrast,the slope of the LMWL for Zhimenda was higher than that of the GMWL.The altitude effects of oxygen(δ^(18)O)and hydrogen(δD)isotopes of precipitation were 0.70‰/100 m and 5.22‰/100 m,respectively.When the temperature was≤5℃,there was a significant temperature effect on stable oxygen isotope of precipitation(0.24‰/℃,P<0.05).Furthermore,even a minor increase(1%)in the weight of raindrops after falling results in a 0.82%rise in the evaporation enrichment rate ofδ^(18)O.Success-ive precipitation events also had a substantial influence on precipitation in the transitional region of the Qinghai-Tibet Plateau.The res-ults of this study provide a theoretical basis for revealing the impact mechanism of precipitation in the transitional zone of the Qinghai-Tibet Plateau under a warming climate.
基金supported by the National Natural Science Foundation of China(Nos.22108181,22178233)the Fund of Science and Technology on Reactor Fuel and Materials Laboratory(No.6142A06190601)+6 种基金the National Excellent Young Scientists Fund(No.00308054A1045)the National Key R&D Program of China(No.2022YFA0912800)the Talents Program of Sichuan ProvinceDouble First Class University Plan of Sichuan Universitythe State Key Laboratory of Polymer Materials Engineering(No.sklpme 2020–03–01)the Tianfu Emei Program of Sichuan Province(No.2022EC02–00073-CG)Ministry of Education Key Laboratory of Leather Chemistry and Engineering(Sichuan University)。
文摘Although the demand of ^(10)B separation has arisen in the 1930s,^(10)B/^(11)B are among the most difficult isotopes to separate due to the extremely similar relative atomic mass.Herein,we report an efficient separation of ^(10)B isotopologue by engineering amino-galloyl synergistic materials via a selective adsorption and isotope exchange reaction,achieving a record-high single-stage separation factor of 1.048 with ^(10)B abundance up to 21.42%.^(11)B MAS NMR results and DFT calculations reveal that the galloyl groups exhibit inherent high affinity for B(OH)4-,forming tetrahedral sp^(3) B-galloyl complexes.The relatively higher ^(10)B–O bond energy of ^(10)B-galloyl complexes facilitates the isotope exchange between11B in B-galloyl complexes and ^(10)B in B(OH)_(3).Flowthrough dynamic separation in fixed-bed demonstrates the feasibility and potential of large-scale deployment of this method in real-world,suggesting a promising avenue for the exploitation of more efficient enrichment of ^(10)B for the sustainable nuclear energy and biomedical research.
文摘Nitrogen-15 isotope-modified compounds are widely used in medicine, pharmacology, agriculture and various fields of science and their nomenclature is gradually increasing. Their widespread use depends on the availability of inexpensive and simple isotope analysis methods. The present article is an attempt to determine the nitrogen-15 isotope content directly in organic compounds without their conversion. The general principle of possibility of determination of the isotopes of nitrogen directly in organic compounds is proposed. Based on the study of mass-spectra of Carbamide Carbonyldiamide, isocyanic acid and nitrobenzene the mass peaks are selected, by which it is possible to determine the atomic fraction of the isotopes of nitrogen. The respective formulas are proposed.
基金supported by the National Natural Science Foundation of China(Grant No.42030607)the Beijing Municipal Science and Technology Commission(Grant No.Z251100004525005)the National Science Foundation/National Center for Atmospheric Research,and NASA(Grant No.80NSSC22M0129)。
文摘The growth trajectory of hailstones within clouds has remained elusive due to the inability to trace them directly,impeding the comprehension of their underlying growth mechanisms.This study investigated hailstone vertical growth trajectories by detecting the stable isotope signatures(2H and 18O compositions)of different shells in 27 hailstones from 9hailstorms,which allowed us to capture the ambient temperature during hailstone growth.The vertical growth trajectories were obtained by comparing the isotopic compositions of water condensate in clouds,derived from the Adiabatic Model,with those measured in hailstones.Although hailstone growth was primarily observed in the–10°C to–30°C temperature layer,the embryo formation height and subsequent growth trajectories significantly varied among hailstones.Embryos formed over a wide range of temperatures(–8.7°C to–33.4°C);four originated at temperatures above–15°C and 16originated at temperatures below–20°C,suggesting ice nuclei composed of bioproteins and mineral dust,respectively.Among the 27 measured hailstones,3 exhibited minimal vertical movement,16 exhibited a monotonic rise or fall,and the remaining 8 exhibited alternating up-down trajectories;only one experienced“recycling”during up-down drifting.Trajectory analysis revealed that similar-sized hailstones from a single storm tended to form at similar heights,whereas those larger than 25 mm in diameter exhibited at least one period of upward growth.Vertical trajectories derived from isotopic analysis were corroborated by radar hydrometeor observations.
文摘Biomarker and stable carbon isotope analyses are presented for the Garau Formation of the Cretaceous Age,an important source rock in western Iran,to reveal its potential as an oilprone source rock.The C_(28)/C_(29)sterane ratio value range(0.72 to 0.83)of bitumen samples from the formation suggests that they were likely formed during phytoplankton blooms.Sterane,hopane,and isoprenoid/n-alkane ratios indicate that the formation's organic matter predominantly consists of algae,and bacteria,accompanied by some reworked material derived from higher plants.Due to the predominance of anoxic conditions and the actions of sulfate-reducing bacteria,the bitumen present is enriched with sulfur compounds.The percentages of saturates,aromatics,and nitrogen-sulfuroxygen(NSO)fractions in the bitumen samples classify them as naphthenic oils.Isotope analysis reveals that biodegradation and water-washing have reduced the concentrations of some volatile saturates and low molecular weight aromatics in the bitumen samples.These actions have resulted in distinctiveδ^(13)C values for the formation's kerogen and bitumen fractions.The formation's organic matter has been subjected to high-temperature thermal regimes and has entered the oil-generation window at the sampled localities,with vitrinite reflectance(%R_(C))varying between 0.7%and 0.75%.
基金supported by the National Natural Science Foundation of China(No.42025705)the Construction Project of Modern Agricultural Science and Technology Innovation Alliance of Guangdong Province,China(No.2023KJ112)+1 种基金the National Natural Science Foundation of China(Nos.41977291 and 42177242)the GDAS’Project of Science and Technology Development,China(No.2019GDASYL-0103048).
文摘Coal power plants annually generate quantities of byproducts that release environmentally hazardous heavy metals like Cd and Pb.Understanding the behavior and spatiotemporal impacts on soils of these releases is crucial for pollution control.This study investigated the concentrations and isotope ratios of Cd/Pb in combustion byproducts,depositions and soils collected froma coal-fired power plant or its surrounding area.The pulverized fuel ash(PFA)and desulfurized gypsum(DG)exhibited heavier Cd isotopes withΔ^(114)Cd values of 0.304‰and 0.269‰,respectively,while bottom ash(BA)showed lighter Cd isotopes(Δ^(114)CdBA-coal=–0.078‰),compared to feed coal.We proposed a two-stage condensation process that governs the distribution of Cd/Pb,including accumulation on PFA and DG within electrostatic precipitators and desulfurization unit,as well as condensation onto fine particles upon release from the stack.Emissions from combustion and large-scale transport make a significant contribution to deposition,while the dispersion of Cd/Pb in deposition is primarily influenced by the prevailing wind patterns.However,the distribution of Cd/Pb in soils not only exhibit predominant wind control but is also potentially influenced by the resuspension of long-term storage byproducts.The power plant significantly contributes to soil in the NW–N–NE directions,even at a considerable distance(66%–79%),demonstrating its pervasive impact on remote regions along these orientations.Additionally,based on the vertical behavior in the profile,we have identified that Cd tends to migrate downward through leaching,while variations in Pb respond to the historical progression of dust removal.
基金supported by the Natural Science Foundation of China(Grant No.42302170)National Postdoctoral Innovative Talent Support Program(Grant No.BX20220062)+3 种基金CNPC Innovation Found(Grant No.2022DQ02-0104)National Science Foundation of Heilongjiang Province of China(Grant No.YQ2023D001)Postdoctoral Science Foundation of Heilongjiang Province of China(Grant No.LBH-Z22091)the Natural Science Foundation of Shandong Province(Grant No.ZR2022YQ30).
文摘Prediction of production decline and evaluation of the adsorbed/free gas ratio are critical for determining the lifespan and production status of shale gas wells.Traditional production prediction methods have some shortcomings because of the low permeability and tightness of shale,complex gas flow behavior of multi-scale gas transport regions and multiple gas transport mechanism superpositions,and complex and variable production regimes of shale gas wells.Recent research has demonstrated the existence of a multi-stage isotope fractionation phenomenon during shale gas production,with the fractionation characteristics of each stage associated with the pore structure,gas in place(GIP),adsorption/desorption,and gas production process.This study presents a new approach for estimating shale gas well production and evaluating the adsorbed/free gas ratio throughout production using isotope fractionation techniques.A reservoir-scale carbon isotope fractionation(CIF)model applicable to the production process of shale gas wells was developed for the first time in this research.In contrast to the traditional model,this model improves production prediction accuracy by simultaneously fitting the gas production rate and δ^(13)C_(1) data and provides a new evaluation method of the adsorbed/free gas ratio during shale gas production.The results indicate that the diffusion and adsorption/desorption properties of rock,bottom-hole flowing pressure(BHP)of gas well,and multi-scale gas transport regions of the reservoir all affect isotope fractionation,with the diffusion and adsorption/desorption parameters of rock having the greatest effect on isotope fractionation being D∗/D,PL,VL,α,and others in that order.We effectively tested the universality of the four-stage isotope fractionation feature and revealed a unique isotope fractionation mechanism caused by the superimposed coupling of multi-scale gas transport regions during shale gas well production.Finally,we applied the established CIF model to a shale gas well in the Sichuan Basin,China,and calculated the estimated ultimate recovery(EUR)of the well to be 3.33×10^(8) m^(3);the adsorbed gas ratio during shale gas production was 1.65%,10.03%,and 23.44%in the first,fifth,and tenth years,respectively.The findings are significant for understanding the isotope fractionation mechanism during natural gas transport in complex systems and for formulating and optimizing unconventional natural gas development strategies.
基金supported by the National Natural Science Foundation of China(42161007)the Innovation Foundation of Higher Education Institutions of Gansu Province(2021B-081)the Foundation for Distinguished Young Scholars of Gansu Province(20JR10RA112).
文摘Precipitation isotopes(δ^(18)O and δ^(2)H)are closely related to meteorological conditions for precipitation generation and the initial state of water vapor source areas,and are essential to the study of the regional hydrological cycle.The deuterium excess(d-excess)indicates deviation in isotope fractionation during evaporation and can trace water vapor sources.This study analyzed 443 precipitation samples collected from the Gannan Plateau,China in 2022 to assess precipitation isotope variations and their driving factors.Water vapor sources were evaluated using the Hybrid Single-Particle Lagrangian Integrated Trajectory(HYSPLIT),Concentration Weighted Trajectory(CWT),and Potential Source Contribution Factor(PSCF)models.Results showed that precipitation isotope values showed significant spatial and temporal variations on the Gannan Plateau.Temporally,precipitation isotope values peaked in June(when evaporation dominated)and minimized in March(depletion effect of air masses in the westerly wind belt).Spatially,the isotope values showed a distribution pattern of"high in the east and low in the west",which was mainly regulated by the differences in altitude and local meteorological conditions.Compared with the global meteoric water line(GMWL)with equation of δ^(2)H=8.00δ^(18)O+10.00,the slope and intercept of local meteoric water line(LMWL)for precipitation on the Gannan Plateau were smaller(7.49 and 7.63,respectively),reflecting the existence of a stronger secondary evaporation effect under the clouds in the region.The sources of water vapor on the Gannan Plateau showed significant seasonality and spatial heterogeneity.Specifically,the westerly belt and monsoon were the main water vapor transport paths at each sampling point,with Central Asian continental water vapor dominating in spring(53.49%),Indian Ocean water vapor dominating in summer(52.53%),Atlantic Ocean water vapor dominating in autumn(46.74%),and Atlantic Ocean and Mediterranean Sea water vapor dominating in winter(42.30%and 33.68%,respectively).Changes in the intensity of convective activity and Outgoing Longwave Radiation(OLR)affected the enrichment of isotopic values,which exhibited the same change trends as δ^(18)O.During the precipitation process,the δ^(18)O value first decreased and then increased.During the initial and final stages of precipitation process,precipitation was mainly influenced by continental air masses,while during the middle stage,it was controlled by marine air masses.The systematic research on precipitation isotopes and water vapor sources is important for climate change research and extreme precipitation prediction on the Gannan Plateau and other similar areas.
基金supported by the National Natural Science Foundation of China(Nos.42003014,42363004,42073051,42303023)Jiangxi Provincial Natural Science Foundation(No.20232BAB213070)the Natural Science Foundation of Shandong Province(No.ZR2022QD050)。
文摘Sulfur isotopes of S-bearing materials are powerful tools to trace various geological processes and sulfur sources in earth sciences,especially in ore deposits where sulfide-sulfate pair coprecipitates widely.However,in-situ S isotope determination of barite is challenging without natural matrix-matched reference material.In this study,we present two natural barite reference materials(1-YS and 294-YS)for in-situ sulfur isotopic analysis.Independent LA-MC-ICP-MS laboratories were utilized to test theδ34S micron-scale homogeneity of 1-YS and 294-YS barites that have 2s repeatabilities of better than±0.45‰and±0.41‰,respectively.Meanwhile,the in-situ analysis results are consistent with the results of the bulk analysis by GS-IRMS within uncertainty.The grand meanδ~(34)S values of 1-YS(13.37‰±0.42‰,2s)and 294-YS(14.38‰±0.44‰,2s)are the final recommended values obtained from four independent laboratories.All the results confirm the suitability of 1-YS and 294-YS barite used as calibration materials with respect to in-situ S isotopic analysis.Moreover,the new developed barite reference materials were used as matrix-matched standard to calibrate the barite samples from the Huayangchuan carbonatite-hosted U-polymetallic deposit(Qinling orogenic belt,western China)to obtainδ34S values.Utilizing the temperaturedependentδ34S fractionation of barite-pyrite pair,we calculate the formation temperature of barite(i.e.,506 to 537°C)and theδ34S value of mineralizing fluid(i.e.,-7.11‰to-7.59‰)in the Huayangchuan deposit.The results indicate an involvement of sedimentary sulfur,presumably acting as a potential uranium source(e.g.,upper crustal materials)for the giant Huayangchuan deposit.
文摘The Cretaceous Koum Basin is a rift-related half-graben in northern Cameroon,which constitutes a portion of the Yola Arm of the Upper Benue Trough.This study presents the first comprehensive dataset combining mineral-ogical,bulk-rock geochemical,and stable C-H-O isotopic data for dark-gray,finegrained mudstones from the basin,providing new insights into its sediment source,paleoenvironment,and geodynamic setting.The mudstones primarily consist of phyllosilicates(~8.6%),feldspars(~30.5%),carbonates(~13.7%),and minor iron oxides(~2.7%),with vermiculite,illite,and kaolinite as the main clay minerals.The presence of analcime,ankerite,and dolomite suggests low-grade metamorphism and/or hydrothermal alteration.Fe_(2)O_(3)/K_(2)O(1.52-6.40)and SiO_(2)/Al_(2)O_(3)(2.97-4.68)ratios classify the mudstones as compositionally immature shales(ICV~1.64)with low-moderate chemical weathering(CIA~56.35;PIA~59.74;R^(3+)/R^(3+)+R^(2+)+M^(+)~0.51).Trace element ratios(Th/Sc~1.70,Zr/Sc~1.33,La/Sc~6.30,La/Th~4.14)indicate an intermediate igneous provenance from a continental crustal source.Paleoenviron-mental proxies suggest deposition in a dynamic basin environment marked by fluctuating redox(C org/P:0.21-178.34)and salinity(Sr/Ba:0.34-3.25;N-values:48-35.92)conditions,ranging from oxic to anoxic and brackish to saline.Major element data(SiO_(2) vs.Al_(2)O_(3)+K_(2)O+Na_(2)O)indicate a semi-arid regime,while Paleoclimatic indicators such as Sr/Cu(1.88-37.47)and C-values(0.12-0.93)suggests alter-nating humid and arid conditions.Notably,stable isotope data,reported here for the first time in the Koum Basin,reveal a predominantly terrestrial,fluvial-deltaic C_(3) plant source for organic carbon(δ^(13)C-25.2‰ to -35.2‰)and complex fluid-rock interactions involving meteoric and magmatic-metamorphic fluids under a warm,equatorial climate(δ^(18)O+3.6‰to +24.9‰,δ^(2)H-104‰ to-50‰).The combined mineralogical,geochemical,and isotopic data point to deposition in a tectonically active continental arc setting,with contributions from ocean island arc and passive margin sources.
