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Rebuilding the theory of isotope fractionation for evaporation of silicate melts under vacuum condition
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作者 Jie Wang Yun Liu 《Acta Geochimica》 EI CAS CSCD 2024年第4期661-676,共16页
Isotope eff ects are pivotal in understanding silicate melt evaporation and planetary accretion processes.Based on the Hertz-Knudsen equation,the current theory often fails to predict observed isotope fractionations o... Isotope eff ects are pivotal in understanding silicate melt evaporation and planetary accretion processes.Based on the Hertz-Knudsen equation,the current theory often fails to predict observed isotope fractionations of laboratory experiments due to its oversimplified assumptions.Here,we point out that the Hertz-Knudsen-equation-based theory is incomplete for silicate melt evaporation cases and can only be used for situations where the vaporized species is identical to the one in the melt.We propose a new model designed for silicate melt evaporation under vacuum.Our model considers multiple steps including mass transfer,chemical reaction,and nucleation.Our derivations reveal a kinetic isotopic fractionation factor(KIFF orα)αour model=[m(^(1)species)/m(^(2)species)]^(0.5),where m(species)is the mass of the reactant of reaction/nucleation-limiting step or species of diffusion-limiting step and superscript 1 and 2 represent light and heavy isotopes,respectively.This model can eff ectively reproduce most reported KIFFs of laboratory experiments for various elements,i.e.,Mg,Si,K,Rb,Fe,Ca,and Ti.And,the KIFF-mixing model referring that an overall rate of evaporation can be determined by two steps jointly can account for the eff ects of low P_(H2)pressure,composition,and temperature.In addition,we find that chemical reactions,diffusion,and nucleation can control the overall rate of evaporation of silicate melts by using the fitting slope in ln(−ln f)versus ln(t).Notably,our model allows for the theoretical calculations of parameters like activation energy(E_(a)),providing a novel approach to studying compositional and environmental eff ects on evaporation processes,and shedding light on the formation and evolution of the proto-solar and Earth-Moon systems. 展开更多
关键词 EVAPORATION Kinetic isotopic fractionation Chemical kinetics Hertz-Knudsen equation CAIS
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Theoretical study of kinetic isotope effects for vacancy diffusion of impurity in solids
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作者 Yuxi Jing Xuefang Li Yun Liu 《Acta Geochimica》 EI CAS CSCD 2024年第5期959-970,共12页
Theoretical studies of the diffusionalisotope effect in solids are still stuck in the 1960s and 1970s.With the development of high spatial resolution mass spectrometers,isotopic data of mineral grains are rapidly accu... Theoretical studies of the diffusionalisotope effect in solids are still stuck in the 1960s and 1970s.With the development of high spatial resolution mass spectrometers,isotopic data of mineral grains are rapidly accumulated.To dig up information from these data,molecularlevel theoretical models are urgently needed.Based on the microscopic definition of the diffusion coe fficient(D),a new theoretical framework for calculating the diffusional isotope effect(DIE(v))(intermsofD*/D)forvacancy-mediated impurity diffusion in solids is provided based on statistical mechanics formalism.The newly derived equation shows that theDIE(v)can be easily calculated as long as the vibration frequencies of isotope-substituted solids are obtained.The calculatedDIE(v)values of^(199)Au/^(195)Au and^(60)Co/^(57)Co during diffusion in Cu and Au metals are all within 1%of errors compared to the experimental data,which shows that this theoretical model is reasonable and precise. 展开更多
关键词 Vacancy diffusion Diffusional isotope effect Statistical mechanics
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Experimental constraints on the formation of oxychlorine species by UV irradiation and mechanical pulverization on the lunar surface
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作者 Jiamei Li Yu-Yan Sara Zhao +4 位作者 He Cui Shuai-Yi Qu Yanhua Peng Yuhong Yang Xiongyao Li 《Acta Geochimica》 EI CAS CSCD 2024年第4期625-637,共13页
Perchlorate and chlorate are present in various extraterrestrial celestial bodies throughout the solar system,such as Mars,the moon,and asteroids.To date,the origin mechanisms of perchlorate and chlorate on the Martia... Perchlorate and chlorate are present in various extraterrestrial celestial bodies throughout the solar system,such as Mars,the moon,and asteroids.To date,the origin mechanisms of perchlorate and chlorate on the Martian surface have been well-established;however,relatively little attention has been cast to airless bodies.Here,we experimentally investigated the potential oxidation mechanisms of chloride to chlorate and perchlorate,such as ultraviolet irradiation under H_(2)O-and O_(2)-free conditions and mechanical pulverization processes.Individual minerals,olivine,pyroxene,ilmenite,magnetite,TiO_(2)and anhydrous ferric sulfate,and lunar regolith simulants(low Ti,CLRS-1;high-Ti,CLRS-2)and their metallic iron(Fe^( 0))bearing counterparts were examined.We found that pulverization of dry matrix material-halite mixtures,even in the presence of O_(2),does not necessarily lead to perchlorate and chlorate formation without involving water.Under photocatalytic and H_(2)O and O_(2)-free conditions,olivine and pyroxene can produce oxychlorine(ClO_(x)^(−))species,although the yields were orders of magnitude lower than those under Martian-relevant conditions.Nanophase-Fe^(0)particles in the lunar regolith and the common photocatalyst TiO_(2)can facilitate the ClO_(x)^(−)formation,but their yields were lower than those with olivine.The oxides ilmenite and magnetite did not efficiently contribute to ClO_(x)^(−)production.Our results highlight the critical role of H_(2)O in the oxidation chloride to chlorate and perchlorate,and provide essential insights into the environmental influence on the formation of oxychlorine species on different celestial bodies. 展开更多
关键词 PERCHLORATE CHLORATE Lunar regolith Metallic Fe Airless bodies
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Formation and growth of nanophase iron particles on the surface of Mercury revealed by experimental study
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作者 Ronghua Pang Yang Li +11 位作者 Chen Li Pengfei Zhang Zhuang Guo Sizhe Zhao Han Yu Li Wang Chenxi Zhu Shuangyu Wang Kairui Tai Qinwei Zhang Yuanyun Wen Rui Li 《Acta Geochimica》 EI CAS CSCD 2024年第4期774-784,共11页
Space weathering is a primary factor in altering the composition and spectral characteristics of surface materials on airless planets.However,current research on space weathering focuses mainly on the Moon and certain... Space weathering is a primary factor in altering the composition and spectral characteristics of surface materials on airless planets.However,current research on space weathering focuses mainly on the Moon and certain types of asteroids.In particular,the impacts of meteoroids and micrometeoroids,radiation from solar wind/solar flares/cosmic rays,and thermal fatigue due to temperature variations are being studied.Space weathering produces various transformation products such as melted glass,amorphous layers,iron particles,vesicles,and solar wind water.These in turn lead to soil maturation,changes in visible and near-infrared reflectance spectra(weakening of characteristic absorption peaks,decreased reflectance,increased near-infrared slope),and alterations in magnetism(related to small iron particles),collectively termed the“lunar model”of space weathering transformation.Compared to the Moon and asteroids,Mercury has unique spatial environmental characteristics,including more intense meteoroid impacts and solar thermal radiation,as well as a weaker particle radiation environment due to the global distribution of its magnetic field.Therefore,the lunar model of space weathering may not apply to Mercury.Previous studies have extensively explored the eff ects of micrometeoroid impacts.Hence,this work focuses on the eff ects of solar-wind particle radiation in global magnetic-field distribution and on the weathering transformation of surface materials on Mercury under prolonged intense solar irradiation.Through the utilization of highvalence state,heavy ion implantation,and vacuum heating simulation experiments,this paper primarily investigates the weathering transformation characteristics of the major mineral components such as anorthite,pyroxene,and olivine on Mercury’s surface and compares them to the weathering transformation model of the Moon.The experimental results indicate that ion implantation at room temperature is insufficient to generate np-Fe^(0)directly but can facilitate its formation,while prolonged exposure to solar thermal radiation on Mercury’s surface can lead directly to the formation of np-Fe^(0).Therefore,intense solar thermal radiation is a crucial component of the unique space weathering transformation process on Mercury’s surface. 展开更多
关键词 MERCURY Space weathering Np-Fe^(0) Solar thermal radiation Solar wind
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Nuclear volume effects in kinetic isotope fractionation:A case study of mercury oxidation by chlorine species
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作者 Chenlu Yang Yining Zhang Yun Liu 《Acta Geochimica》 EI CAS CSCD 2024年第3期411-423,共13页
It is well-known that the equilibrium isotope fractionation of mercury(Hg)includes classical massdependent fractionations(MDFs)and nuclear volume effect(NVE)induced mass-independent fractionations(MIFs).However,the ef... It is well-known that the equilibrium isotope fractionation of mercury(Hg)includes classical massdependent fractionations(MDFs)and nuclear volume effect(NVE)induced mass-independent fractionations(MIFs).However,the effect of the NVE on these kinetic processes is not known.The total fractionations(MDFs+NVEinduced MIFs)of several representative Hg-incorporated substances were selected and calculated with ab initio calculations in this work for both equilibrium and kinetic processes.NVE-induced MIFs were calculated with scaled contact electron densities at the nucleus through systematic evaluations of their accuracy and errors using the Gaussian09 and DIRAC19 packages(named the electron density scaling method).Additionally,the NVE-induced kinetic isotope effect(KIE)of Hg isotopes are also calculated with this method for several representative Hg oxidation reactions by chlorine species.Total KIEs for 202 Hg/^(198)Hg ranging from−2.27‰to 0.96‰are obtained.Three anomalous^(202)Hg-enriched KIEs(δ^(202)Hg/^(198)Hg=0.83‰,0.94‰,and 0.96‰,)caused by the NVE are observed,which are quite different from the classical view(i.e.,light isotopes react faster than the heavy ones).The electron density scaling method we developed in this study can provide an easier way to calculate the NVE-induced KIEs for heavy isotopes and serve to better understand the fractionation mechanisms of mercury isotope systems. 展开更多
关键词 Nuclear volume effect Kinetic fractionation Hg isotopes Ab initio calculations
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Correction:The escape mechanisms of the proto-atmosphere on terrestrial planets:“boil-off”escape,hydrodynamic escape and impact erosion
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作者 Ziqi Wang You Zhou Yun Liu 《Acta Geochimica》 EI CAS CSCD 2024年第3期623-623,共1页
In the original publication of the article,the affiliation“College of Earth and Planetary Sciences,University of Chinese Academy of Sciences,Beijing,People’s Republic of China”for author Ziqi Wang was missing and i... In the original publication of the article,the affiliation“College of Earth and Planetary Sciences,University of Chinese Academy of Sciences,Beijing,People’s Republic of China”for author Ziqi Wang was missing and included in this correction article. 展开更多
关键词 ESCAPE PLANET COLLEGE
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Early Silurian Wuchuan–Sihui–Shaoguan exhalative sedimentary pyrite belt, South China: constraints from zircon dating for K-bentonite of the giant Dajiangping deposit 被引量:3
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作者 Yingying Zhang Taiyi Luo +2 位作者 Tian Gan Mingzhong Zhou Xinqiao Han 《Acta Geochimica》 EI CAS CSCD 2021年第1期1-12,共12页
The Wuchuan-Sihui-Shaoguan(WSS)exhalative sedimentary pyrite belt in the southwestern part of the Qinzhou-Hangzhou(Qin-Hang)belt is the most important sulfur industry base in China.However,a wide range of metallogenet... The Wuchuan-Sihui-Shaoguan(WSS)exhalative sedimentary pyrite belt in the southwestern part of the Qinzhou-Hangzhou(Qin-Hang)belt is the most important sulfur industry base in China.However,a wide range of metallogenetic ages spanning from Ediacaran to Devonian has been reported in the literature.This age range does not support the idea that the typical character of"coeval mineralization"in an exhalative sedimentary mineralization belt in China and worldwide.Therefore,the precise determination of mineralization ages of representative deposits is necessary to provide guides for exploration and metallogenetic models.The Dajiangping pyrite deposit is a typical example of this kind of deposits and is also the largest deposit with a proven reserve of 210 Mt.This deposit was thought to have formed in Ediacaran or Devonian.In this study,2-3 layers of 10-25 cm thick 2M1-type microcrystalline muscovite slate abruptly embedded in the No.Ⅳmassive orebody of the deposit has been identified to be low-grade metamorphic K-bentonite.A Concordia zircon LA-ICP-MS U-Pb age of 432.5±1.3 Ma(mean standard weighted deviation of concordance and equivalence=1.2;N=11)has been yielded for the low-grade metamorphic K-bentonite.This age is distinctly different from the Rb-Sr isochron age of630.1±7.3 Ma for siliceous rock at the top of the No.Ⅲbanded orebody and the Re-Os isochron age of 389±62 Ma for pyrites from a laminated orebody.Instead,it is close to the intercept age(429 Ma)of the youngest detrital zircons from sandstone interlayers of the No.Ⅲbanded orebody.The Concordia age is also coincident with those of the Late Caledonian(400-460 Ma)magmatism-metamorphism events which are widely distributed in Cathaysia Block.Particularly,it agrees well with that of the Early Silurian extensional volcanism(434-444 Ma)which have been revealed in the Dabaoshan,Siqian-Hekou,and Nanjing volcanic basins in northern Guangdong Province and southern Jiangxi Province.Hence,the dating result in this study confirms that the sedimentary time of the ore-host Daganshan Formation is Early Silurian,and implies that the mineralization age of the Dajiangping pyrite deposit should also be Early Silurian.In combination with the Early Silurian age of Shezui pyrite deposit and the Dabaoshan volcanic basin along the WSS pyrite belt,it could be inferred that the WSS pyrite belt provides a record of the northern expanding of Qinzhou-Fangcheng trough in Early Silurian and that the exhalative pyrite mineralization was triggered by the postcollisional extension of the margin of Cathaysia Block after the intracontinental collision between Cathaysia Block and Yangtze Block during Late Caledonian stage. 展开更多
关键词 Wuchuan–Sihui–Shaoguan exhalative sedimentary pyrite belt Dajiangping pyrite deposit Lowgrade metamorphic K-bentonite Zircon U–Pb dating
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A model of crust-mantle differentiation for the early Earth
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作者 Qingwen Zhang Dan Zhu +1 位作者 Wei Du Yun Liu 《Acta Geochimica》 EI CAS CSCD 2022年第4期689-703,共15页
The Archean continents,primarily composed of the felsic tonalite-trondhjemite-granodiorite(TTG)suite,were formed or conserved since~3.8 Ga,with significant growth of the continental crust since~2.7 Ga.The difficulty i... The Archean continents,primarily composed of the felsic tonalite-trondhjemite-granodiorite(TTG)suite,were formed or conserved since~3.8 Ga,with significant growth of the continental crust since~2.7 Ga.The difficulty in direct differentiation of the felsic crustal components from Earth’s mantle peridotite leads to a requirement for the presence of a large amount of hydrated mafic precursor of TTG in Earth’s proto-crust,the origin of which,however,remains elusive.The mafic proto-crust may have formed as early as~4.4 Ga ago as reflected by the Hf and Nd isotopic signals from Earth’s oldest geological records.Such a significant time lag between the formation of the mafic proto-crust and the occurrence of felsic continental crust is not reconciled with a single-stage scenario of Earth’s early differentiation.Here,inspired by the volcanism-dominated heat-pipe tectonics witnessed on Jupiter’s moon Io and the resemblances of the intensive internal heating and active magmatism between the early Earth and the present-day Io,we present a conceptual model of Earth’s early crust-mantle differentiation,which involves an Io-like scenario of efficient extraction of a mafic proto-crust from the early mantle,followed by an intrusion-dominating regime that could account for the subsequent formation of the felsic continents as Earth cools.The model thus allows an early formation of the preTTG proto-crust and the generation of TTG in the continent by providing the favorable conditions for its subsequent melting.This model is consistent with the observed early fractionation of the Earth and the late but rapid formation and/or accumulation of the felsic components in the Archean continents,thus sheds new light on the early Earth’s differentiation and tectonic evolution. 展开更多
关键词 Crust-mantle differentiation Heat-pipe tectonics Plutonic squishy lid tectonics Proto-crust TTG Io
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The cooling models of Earth’s early mantle
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作者 Ting He Qingwen Zhang Yun Liu 《Acta Geochimica》 EI CAS CSCD 2023年第5期803-816,共14页
The thermal state of the early Earth’s interior and its way of cooling are crucial for its subsequent evo-lution.Earth is initially hot as it acquired enormous heat in response to violent processes during its formati... The thermal state of the early Earth’s interior and its way of cooling are crucial for its subsequent evo-lution.Earth is initially hot as it acquired enormous heat in response to violent processes during its formation,e.g.,the Moon-forming giant impact,the segregation and formation of its metallic core,the tidal interaction with the early Moon,and the decay of radioactive elements,etc.In the meantime,the cooling mechanisms of early Earth’s mantle remain elusive despite their importance,and the previously proposed cooling models of the mantle are controversial.In this paper,we first reviewed several prevalent parameter-ized thermal evolution models of the early mantle.The models give unrealistic predictions since they were estab-lished solely based on a single tectonic regime,such as the stagnant-lid regime,or relied on the disputable existence of the plate tectonics prior to-3.5 Ga.Then we argue that the mantle should have started to cool down from a very hot state after the solidification of the ferocious magma ocean.Instead of using one single scaling law to describe a single-stage model,we suggest that an episodic multi-stage cooling model(EMCM)of the early mantle could be more plausible to account for the mantle’s early cooling process.The model reconciles with the fact that the mantle cools down from a hot state prior to*3.5 Ga and can also explain the well-constrained post-3.5 Ga thermal history of the mantle. 展开更多
关键词 Thermal evolution MANTLE Parameterized model Episodic cooling Early mantle
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How to estimate isotope fractionations of a Rayleigh-like but diffusion-limited disequilibrium process?
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作者 Zi Xuan Guan Yun Liu 《Acta Geochimica》 EI CAS CSCD 2023年第1期24-37,共14页
The Rayleigh distillation isotope fractionation(RDIF) model is one of the most popular methods used in isotope geochemistry. Numerous isotope signals observed in geologic processes have been interpreted with this mode... The Rayleigh distillation isotope fractionation(RDIF) model is one of the most popular methods used in isotope geochemistry. Numerous isotope signals observed in geologic processes have been interpreted with this model. The RDIF model provides a simple mathematic solution for the reservoir-limited equilibrium isotope fractionation effect. Due to the reservoir effect, tremendously large isotope fractionations will always be produced if the reservoir is close to being depleted. However, in real situations, many prerequisites assumed in the RDIF model are often difficult to meet. For instance, it requires the relocated materials, which are removed step by step from one reservoir to another with different isotope compositions(i.e., with isotope fractionation), to be isotopically equilibrated with materials in the first reservoir simultaneously. This ‘‘quick equilibrium requirement’’ is indeed hard to meet if the first reservoir is sufficiently large or the removal step is fast. The whole first reservoir will often fail to re-attain equilibrium in time before the next removal starts.This problem led the RDIF model to fail to interpret isotope signals of many real situations. Here a diffusion-coupled and Rayleigh-like(i.e., reservoir-effect included) separation process is chosen to investigate this problem. We find that the final isotope fractionations are controlled by both the diffusion process and the reservoir effects via the disequilibrium separation process. Due to its complexity, we choose to use a numerical simulation method to solve this problem by developing specific computing codes for the working model.According to our simulation results, the classical RDIF model only governs isotope fractionations correctly at the final stages of separation when the reservoir scale(or thickness of the system) is reduced to the order of magnitude of the quotient of the diffusivity and the separation rate. The RDIF model fails in other situations and the isotope fractionations will be diffusion-limited when the reservoir is relatively large, or the separation rate is fast. We find that the effect of internal isotope distribution inhomogeneity caused by diffusion on the Rayleigh-like separation process is significant and cannot be ignored. This method can be applied to study numerous geologic and planetary processes involving diffusion-limited disequilibrium separation processes including partial melting,evaporation, mineral precipitation, core segregation, etc.Importantly, we find that far more information can be extracted through analyzing isotopic signals of such ‘‘disequilibrium’’processes than those of fully equilibrated ones, e.g., reservoir size and the separation rate. Such information may provide a key to correctly interpreting many isotope signals observed from geochemical and cosmochemical processes. 展开更多
关键词 Isotope fractionation Reservoir isotope effect Rayleigh-like distillation process Diffusional isotope effect Numerical modeling Disequilibrium process
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Isotopic analysis based on terahertz spectrum
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作者 Qijun Chen Yun Liu 《Acta Geochimica》 EI CAS CSCD 2023年第5期859-869,共11页
As a new promising detection technology in the terahertz research field,the terahertz time-domain spec-troscopy(THz-TDS)has very broad application potential in many fields because its advantage on the characteristic s... As a new promising detection technology in the terahertz research field,the terahertz time-domain spec-troscopy(THz-TDS)has very broad application potential in many fields because its advantage on the characteristic spectrum,wide spectrum and non-destructive analysis of interested substances.In this paper,the terahertz absorption spectra of gases mixed with 12 CO and 13 CO in the spec-trum range of 0.5–2.5 THz are measured by terahertz time-domain spectroscopy for the first time.Several isotopo-logues can be clearly distinguished based on the difference in their rotational energies and the consequent terahertz spectrum.The experimental results show that 12 CO and 13 CO have obvious characteristic absorption peaks in the spectrum range of 0.5–2.5 THz due to the difference in rotational energy,and the rotational constant B can be calculated according to the experimental values to distin-guish the two gaseous isotopologues.The frequency posi-tions of the characteristic absorption peak measured by this experiment and the rotation constant B calculated accord-ing to the experimental values are compared with those previous theoretical calculations and experimental results,and they are in good agreement.This result lays a foun-dation for developing more sophisticated terahertz instru-ments to the detection of different isotopologues. 展开更多
关键词 Isotope analysis CO isotopologue Terahertz time-domain spectroscopy(THz-TDS) Rotational spectrum
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A review of GEMC method and its improved algorithms
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作者 Liwen Zhang Yuhong Yang +1 位作者 Kun Yin Yun Liu 《Acta Geochimica》 EI CAS CSCD 2023年第3期409-434,共26页
Gibbs Ensemble Monte Carlo(GEMC)is a molecular simulation method commonly used for simulating phase equilibrium.This method has been proposed since 1987 and applied in many fields,such as geology,planetary science,che... Gibbs Ensemble Monte Carlo(GEMC)is a molecular simulation method commonly used for simulating phase equilibrium.This method has been proposed since 1987 and applied in many fields,such as geology,planetary science,chemical engineering,material science,etc.GEMC method combines canonical(NVT),isobaricisothermal(NPT),and grand canonical(μVT)Monte Carlo techniques in a single simulation.The GEMC method was developed on the fundamental law of phase equilibrium that chemical potentials of each phase all equal.Two key factors affect the rationality and reliability of GEMC simulations:1.particles can be efficiently moved in/out from certain phase during simulation;2.samplings can represent the whole system well,in other words,samplings hold good ergodicity.In addition,various parallel methods have been developed to improve the simulation efficiency.In this review,an introduction to the theoretical fundamentals,improvements on particle movement and sampling protocols,acceleration techniques and some applications of the GEMC method will be presented.This is the first integrated review introducing the fundamentals,improvements and applications of the GEMC simulation method. 展开更多
关键词 Gibbs Ensemble Monte Carlo Molecular simulation Phase equilibrium
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Microbially-mediated formation of Ca-Fe carbonates during dissimilatory ferrihydrite reduction:Implications for the origin of sedimentary ankerite
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作者 Deng LIU Jinpeng CAO +8 位作者 Shanshan YANG Yating YIN Pengcong WANG Dominic PAPINEAU Hongmei WANG Xuan QIU Genming LUO Zongmin ZHU Fengping WANG 《Science China Earth Sciences》 SCIE EI CAS CSCD 2024年第1期208-221,共14页
The origin of sedimentary dolomite has become a long-standing problem in the Earth Sciences.Some carbonate minerals like ankerite have the same crystal structure as dolomite,hence their genesis may provide clues to he... The origin of sedimentary dolomite has become a long-standing problem in the Earth Sciences.Some carbonate minerals like ankerite have the same crystal structure as dolomite,hence their genesis may provide clues to help solving the dolomite problem.The purpose of this study was to probe whether microbial activity can be involved in the formation of ankerite.Bio-carbonation experiments associated with microbial iron reduction were performed in batch systems with various concentrations of Ca^(2+)(0–20 mmol/L),with a marine iron-reducing bacterium Shewanella piezotolerans WP3 as the reaction mediator,and with lactate and ferrihydrite as the respective electron donor and acceptor.Our biomineralization data showed that Ca-amendments expedited microbially-mediated ferrihydrite reduction by enhancing the adhesion between WP3 cells and ferrihydrite particles.After bioreduction,siderite occurred as the principal secondary mineral in the Ca-free systems.Instead,Ca-Fe carbonates were formed when Ca^(2+)ions were present.The CaCO_(3) content of microbially-induced Ca-Fe carbonates was positively correlated with the initial Ca2+concentration.The Ca-Fe carbonate phase produced in the 20 mmol/L Ca-amended biosystems had a chemical formula of Ca_(0.8)Fe_(1.2)(CO_(3))_(2),which is close to the theoretical composition of ankerite.This ankeritelike phase was nanometric in size and spherical,Ca-Fe disordered,and structurally defective.Our simulated diagenesis experiments further demonstrated that the resulting ankerite-like phase could be converted into ordered ankerite under hydrothermal conditions.We introduced the term“proto-ankerite”to define the Ca-Fe phases that possess near-ankerite stoichiometry but disordered cation arrangement.On the basis of the present study,we proposed herein that microbial activity is an important contributor to the genesis of sedimentary ankerite by providing the metastable Ca-Fe carbonate precursors. 展开更多
关键词 ANKERITE Proto-ankerite Microbial iron reduction Dolomite problem Mineral transformation
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Late veneer and the origins of volatiles of Earth 被引量:1
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作者 Chun-Hui Li 《Acta Geochimica》 EI CAS CSCD 2022年第4期650-664,共15页
Late veneer is an important paradigm in early Earth and planetary studies.It refers to the late addition of extraterrestrial materials to the Earth’s mantle after the core formation,which leads to the overabundances ... Late veneer is an important paradigm in early Earth and planetary studies.It refers to the late addition of extraterrestrial materials to the Earth’s mantle after the core formation,which leads to the overabundances of highly siderophile elements in the primitive upper mantle.In this review,the origin,evolution,and expansion of the late veneer hypothesis are summarized,including some unresolved problems.I hope this review would be helpful for the new entrants to this field. 展开更多
关键词 Highly siderophile elements Late veneer CHONDRITES Primitive mantle Core formation Volatile elements
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Equilibrium mercury and lead isotope fractionation caused by nuclear volume effects in crystals 被引量:1
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作者 Sha Yang Yun Liu 《Acta Geochimica》 EI CAS CSCD 2021年第2期150-162,共13页
To investigate equilibrium mercury(Hg)and lead(Pb)isotope fractionation caused by the nuclear volume effect(NVE)in crystals,the electron densities at nuclei(i.e.,|Ψ(0)|2)for Hg-or Pb-bearing crystalline compounds wer... To investigate equilibrium mercury(Hg)and lead(Pb)isotope fractionation caused by the nuclear volume effect(NVE)in crystals,the electron densities at nuclei(i.e.,|Ψ(0)|2)for Hg-or Pb-bearing crystalline compounds were investigated by using the relativistic spin orbit zeroth-order regular approximation(ZORA)method with a three-dimensional periodic boundary condition based on the density functional theory(DFT).Many isotope fractionation factors of crystalline compounds are provided for the first time.Our results show,even at1000℃,NVE-driven Hg and Pb isotope fractionation are meaningfully large,i.e.,range from 0.12‰to 0.49‰(202Hg/^(198)Hg),from-0.20‰to 0.17‰(208Pb/^(206)Pb)and from-0.08‰to 0.06‰(207Pb/^(206) Pb)relative to Hg0 vapor and Pb0 vapor,respectively.Specifically,the fractionations range from-0.06‰to-0.20‰(208Pb/^(206)Pb)and from-0.02‰to-0.08‰(207Pb/^(206)Pb)for Pb2+-bearing species,from 0.10‰to 0.17‰(208Pb/^(206)Pb)and from 0.04‰to 0.06‰(207Pb/^(206)Pb)for Pb4+-bearing species in crystals.All calculated Hg-bearing species in crystals will enrich heavier isotope(202Hg)relative to Hg0 vapor.Meanwhile,Pb4+-bearing species enrich heavier Pb isotopes(208Pb and 207Pb)than Pb^(2+)-bearing species in crystals,which the enrichment can be up to 0.37‰(208-Pb/^(206)Pb)and 0.14‰(207Pb/^(206)Pb)at 1000℃,due to their NVEs are in opposite directions.The NVE-driven MIFs of Hg isotopes,which are compared to the Hg202-Hg198baseline,are up to-0.158‰(ΔNV199Hg),-0.024‰(ΔNV200Hg)and-0.094‰(ΔNV201Hg)relative to Hg0 vapor at5000 C.For all studied Hg-bearing species in crystals,the MIFs of two odd-mass isotopes(i.e.,ΔNV199Hg andΔNV201Hg)will be changed proportionally and their ratio(i.e.,ΔNV199Hg/ΔNV201Hg)will be a constant 1.67.The NVE can also cause mass-independent fractionations for 207Pb and 204 Pb compared to the baseline of 208Pb and 206Pb.The largest NVEdriven MIFs are 0.043‰(ΔNV207Pb)and-0.040‰(ΔNV204Pb)among all the studied species relative to Pb0 vapor at 5000 C.The magnitudes of odd-mass isotope MIF(ΔNV207Pb)and even-mass isotope MIF(ΔNV204Pb)are almost the same but with opposite signs,leading to the MIF ratio of them(i.e.,ΔNV207Pb/ΔNV204Pb)is-1.08. 展开更多
关键词 Mercury and lead isotopes CRYSTALS Nuclear volume effect DFT relativistic effect calculations
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Origin of ULVZs near the African LLSVP: Implications from their distribution and characteristics 被引量:1
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作者 An Fan Xinlei Sun 《Earthquake Science》 2021年第4期299-309,共11页
Ultra-low velocity zones(ULVZs)provide important information on the composition and dynamics of the core-mantle boundary(CMB).However,their global distribution and characteristics are not well constrained,especially n... Ultra-low velocity zones(ULVZs)provide important information on the composition and dynamics of the core-mantle boundary(CMB).However,their global distribution and characteristics are not well constrained,especially near African large low-shear velocity provinces(LLSVPs).Here,we used ScS precursor(SdS)and postcursor(ScscS)phases recorded by various seismic networks in Africa and South America to investigate the ULVZ characteristics underlying the South Atlantic Ocean.We found no evidence of ULVZs near the SE boundary of South America,but an ULVZ was found within the SW boundary of the African LLSVP,with thicknesses ranging from 11–18 km and reductions in S-wave velocities of 18%–34%.Our results,combined with the global distribution of ULVZs,suggest that thermal activity may be essential to ULVZ formation.Moreover,subducted slab and mantle flow may also play a key role,depending on the location of the ULVZs. 展开更多
关键词 ultra-low velocity zone slab subduction mantle flow thermal effect African large low-shear velocity province.
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The escape mechanisms of the proto-atmosphere on terrestrial planets:"boil-off" escape,hydrodynamic escape and impact erosion
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作者 Ziqi Wang You Zhou Yun Liu 《Acta Geochimica》 EI CAS CSCD 2022年第4期592-606,共15页
Atmospheric escape is an essential process that affects the evolution of the proto-atmosphere.The atmospheric escape of early terrestrial planets was extremely rapid compared with the current scenarios,and the main at... Atmospheric escape is an essential process that affects the evolution of the proto-atmosphere.The atmospheric escape of early terrestrial planets was extremely rapid compared with the current scenarios,and the main atmospheric escape modes were also quite different.During the dissipation of the nebula disk,the primordial atmosphere experienced a brief but violent"boiling"escape,in which most of the primordial atmosphere was lost.After the nebula disk dissipates,hydrodynamic escape and impact erosion are the two most important mass-loss mechanisms for the proto-atmosphere.Hydrodynamic escape is a rapid atmospheric escape process caused by strong solar radiation,while impact erosion refers to the process in which small-large or giant impacts erode the proto-atmosphere.In the early solar system,there were other escape mechanisms,such as non-thermodynamic escape and Jeans escape,but it is generally believed that these mechanisms have relatively little impact.Here we systematically introduce the above-mentioned atmospheric escape mechanisms and then make some suggestions for the existing problems and future research for atmospheric escape models. 展开更多
关键词 Proto-atmosphere Primordial atmosphere "Boil-off" Hydrodynamic escape Impact erosion
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^(182)W anomalies in mantle:a brief review
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作者 Yining Zhang Yun Liu 《Acta Geochimica》 EI CAS CSCD 2022年第4期704-716,共13页
With significant advances in mass spectrometry for isotope analysis in the last decade,e.g.,negative thermal ionization mass spectrometry and multi-collector inductively coupled plasma mass spectrometry,high-precision... With significant advances in mass spectrometry for isotope analysis in the last decade,e.g.,negative thermal ionization mass spectrometry and multi-collector inductively coupled plasma mass spectrometry,high-precision(ppm-level)measurements of tungsten(W)isotopes have been widely used for early earth differentiation processes,such as metal-silicate segregation,melting and crystallization processes during the magma ocean,and putative core-mantle exchange and dynamics.Here,we give a brief review of works on ^(182)W anomalies in terrestrial samples,including methods,results,explanations,implications,and prospects.The review will be presented by including the following parts:the introduction of W isotopes and the short-lived radioactive ^(182)Hf-^(182)W system;data notations and W isotope measurement methods;^(182)W anomalies observed in terrestrial samples;a summary of models developed for interpreting origins of positive and negative ^(182)W anomalies;future prospects. 展开更多
关键词 ^(182)W anomalies Mantle samples MC-ICPMS N-TIMS NORMALIZATION
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Electrical and thermal conductivity of Earth's core and its thermal evolution——A review
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作者 Yuan Yin Qingwen Zhang +2 位作者 Youjun Zhang Shuangmeng Zhai Yun Liu 《Acta Geochimica》 EI CAS CSCD 2022年第4期665-688,共24页
The Earth’s core is composed of iron,nickel,and a small amount of light elements(e.g.,Si,S,O,C,N,H and P).The thermal conductivities of these components dominate the adiabatic heat flow in the core,which is highly co... The Earth’s core is composed of iron,nickel,and a small amount of light elements(e.g.,Si,S,O,C,N,H and P).The thermal conductivities of these components dominate the adiabatic heat flow in the core,which is highly correlated to geodynamo.Here we review a large number of studies on the electrical and thermal conductivity of iron and iron alloys and discuss their implications on the thermal evolution of the Earth’s core.In summary,we suggest that the Wiedemann-Franz law,commonly used to convert the electrical resistivity to thermal conductivity for metals and alloys,should be cautiously applied under extremely high pressure-temperature(P-T)conditions(e.g.,Earth’s core)because the Lorentz number may be P-T dependent.To date,the discrepancy in the thermal conductivity of iron and iron alloys remains between those from the resistivity measurements and the thermal diffusivity modeling,where the former is systematically larger.Recent studies reconcile the electrical resistivity by first-principles calculation and direct measurements,and this is a good start in resolving this discrepancy.Due to an overall higher thermal conductivity than previously thought,the inner core age is presently constrained at~1.0 Ga.However,light elements in the core would likely lower the thermal conductivity and prolong the crystallization of the inner core.Meanwhile,whether thermal convection can power the dynamo before the inner core formation depends on the amounts of the proper light elements in the core.More works are needed to establish the thermal evolution model of the core. 展开更多
关键词 Earth’s core Electrical and thermal conductivity Iron and its alloys Thermal evolution GEODYNAMO
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Preface:the early stage of the early Earth study in China
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作者 Yun Liu 《Acta Geochimica》 EI CAS CSCD 2022年第4期551-552,共2页
This special issue is originated from two successive failures of our application of the major project of the National Natural Science Foundation of China(NSFC)under the discipline category of“Early Earth Evolution”.... This special issue is originated from two successive failures of our application of the major project of the National Natural Science Foundation of China(NSFC)under the discipline category of“Early Earth Evolution”.In the end,this major project was awarded to a research proposal titled“Early shale oil evolution”,and by that the NSFC closed the funding category“Early Earth Evolution”. 展开更多
关键词 NSFC EARTH CATEGORY
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