This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in sit...This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in situ and ex situ X-ray diffraction,Raman spectroscopy,X-ray photoelectron spectroscopy,and transmission electron microscopy,the research unravels the complex structural and chemical evolution of MoS_(2) throughout its cycling.A key discovery is the identification of a unique Li intercalation mechanism in MoS_(2),leading to the formation of reversible Li_(2)MoS_(2) phases that contribute to the extra capacity of the MoS_(2) electrode.Density function theory calculations suggest the potential for overlithiation in MoS_(2),predicting Li5MoS_(2) as the most energetically favorable phase within the lithiation–delithiation process.Additionally,the formation of a Li-rich phase on the surface of Li_(4)MoS_(2) is considered energetically advantageous.After the first discharge,the battery system engages in two main reactions.One involves operation as a Li-sulfur battery within the carbonate electrolyte,and the other is the reversible intercalation and deintercalation of Li in Li_(2)MoS_(2).The latter reaction contributes to the extra capacity of the battery.The incorporation of reduced graphene oxide as a conductive additive in MoS_(2) electrodes notably improves their rate capability and cycling stability.展开更多
Inspired by the concept of "polymer-in-ceramic",a composite poly(ε-caprolactone)(PCL)/ceramic containing LiTFSI is prepared and investigated as a solid electrolyte for all-solid-state batteries.The composit...Inspired by the concept of "polymer-in-ceramic",a composite poly(ε-caprolactone)(PCL)/ceramic containing LiTFSI is prepared and investigated as a solid electrolyte for all-solid-state batteries.The composite with the optimum concentration of 45 wt% LiTFSI and 75 wt% Li1.5Al0.5Ge1.5(PO4)3(LAGP,NASICON-type structure) exhibits a high ionic conductivity(σi=0.17 mS cm-1) at 30℃,a transference number of 0.30,and is stable up to 5.0 V.The composite electrolyte is a flexible and self-standing membrane.Solid-state LiFePO4//Li batteries with this composite electrolyte demonstrate excellent cycling stability with high discharge capacity of 157 mA h g-1,high capacity retention of 96% and coulombic efficiency of 98.5% after 130 cycles at 30℃ and 0.1 C rate.These electrochemical properties are better than other PCL-based allsolid-lithium batteries,and validate the concept of "polymer-in-ceramic" by avoiding the drawback of lower conductivity in prior "polymer-in-ceramic" electrolyte at high concentration of the ceramic.展开更多
At peak granulite-facies metamorphic conditions, lower continental crust is arguably fluxed by large amounts of two key low water activity fluids： （i） high-density CO2 and/or （ii） concentrated saline so- lutions....At peak granulite-facies metamorphic conditions, lower continental crust is arguably fluxed by large amounts of two key low water activity fluids： （i） high-density CO2 and/or （ii） concentrated saline so- lutions. These fluids are either internally-derived, generated by mineral reactions or dehydration melting or, notably for CO2, externally-derived, issued from the underlying mantle. Postmetamorphic evolution results in complete disappearance of these fluids, except for minute remnants preserved in minerals as fluid inclusions. Two major processes are involved： （i） at peak conditions, granitoid magmas form, migrate upward, and crystallize as shallow intrusions in the upper crust （mineralized porphyry types or reduced intrusions）; （ii） during the rapid decompression which almost systematically follows a period of post-peak isobaric cooling, especially for ultrahigh-temperature granulites （anticlockwise P-T paths）, quartz-carbonate megashear zones are formed by repeated periods of seismic activity. Seismic activity may continue until all free fluids have disappeared, resulting in the ultramylonites and pseudotachylites that are found in many granulite domes. A great majority of vein-type Au deposits worldwide occur in the above-mentioned settings or nearby. We suggest that the Au has been scavenged by the granulite fluids, then redistributed and concentrated during the formation of veins and related phenomena.展开更多
The formation of continents involves a combination of magmatic and metamorphic processes. These processes become indistinguishable at the crust-mantle interface, where the pressure-temperature（P-T）conditions of（ul...The formation of continents involves a combination of magmatic and metamorphic processes. These processes become indistinguishable at the crust-mantle interface, where the pressure-temperature（P-T）conditions of（ultra） high-temperature granulites and magmatic rocks are similar. Continents grow laterally, by magmatic activity above oceanic subduction zones（high-pressure metamorphic setting）, and vertically by accumulation of mantle-derived magmas at the base of the crust（high-temperature metamorphic setting）. Both events are separated from each other in time; the vertical accretion postdating lateral growth by several tens of millions of years. Fluid inclusion data indicate that during the high-temperature metamorphic episode the granulite lower crust is invaded by large amounts of low H2O-activity fluids including high-density CO2 and concentrated saline solutions（brines）. These fluids are expelled from the lower crust to higher crustal levels at the end of the high-grade metamorphic event. The final amalgamation of supercontinents corresponds to episodes of ultra-high temperature metamorphism involving large-scale accumulation of these low-water activity fluids in the lower crust.This accumulation causes tectonic instability, which together with the heat input from the subcontinental lithospheric mantle, leads to the disruption of supercontinents. Thus, the fragmentation of a supercontinent is already programmed at the time of its amalgamation.展开更多
Recalling some of the most important events and persons during his education and career, the author sketches his growth from a young engineer, educated in the sanctuary of solid state reactions, to an involved fully d...Recalling some of the most important events and persons during his education and career, the author sketches his growth from a young engineer, educated in the sanctuary of solid state reactions, to an involved fully devoted scientific career for the study of fluids in the deep Earth. Most important in this respect was the discovery of C02 inclusions in granulites, which triggered years of discussion on fluid- absent or fluid-assisted granulite metamorphism. To some extent, this debate is a continuation of the former granite controversy, but it shows also how the famous battle of ＂soaks against pontiffs＂ could have been easily avoided.展开更多
Fluid （and melt） inclusion studies have shown a marked devel- opment in the last decades, as indicated by the increasing number of papers and as covered under major themes in specialized meetings （e.g. ECROFI in Eu...Fluid （and melt） inclusion studies have shown a marked devel- opment in the last decades, as indicated by the increasing number of papers and as covered under major themes in specialized meetings （e.g. ECROFI in Europe, PACROFI in America, ACROFI in Asia）. However, a basic text book is lacking in current literature, available information being either somewhat outdated （e,g. Roedder, 1984） or scattered in multi-author ＂short course＂, mainly organized by the Mineralogical Societies of Canada, America or Europe. A result is that basic features of fluid inclusion studies, notably its key technique, microthermometry, and recently supplemented by micro Raman of infrared spectroscopy, is rarely taught in most universities, leaving the student alone to discover a field of study which has grown to the dimensions of a major science.展开更多
The long-term redistribution of Zn in a naturally Zn-enriched soil during pedogenesis was quantified based on mass balance calculations. According to their fate, parent limestones comprised three Zn pools: bound to ca...The long-term redistribution of Zn in a naturally Zn-enriched soil during pedogenesis was quantified based on mass balance calculations. According to their fate, parent limestones comprised three Zn pools: bound to calcite and pyritesphalerite grains, bound to phyllosilicates and bound to goethite in the inherited phosphate nodules. Four pedological processes, i.e., carbonate dissolution, two stages of redox processes and eluviation, redistributed Zn during pedogenesis. The carbonate dissolution of limestones released Zn bound to calcite into soil solution. Due to residual enrichment, Zn concentrations in the soil are higher than those in parent limestones. Birnessite, ferrihydrite and goethite dispersed in soil horizon trapped high quantities of Zn during their formation. Afterwards, primary redox conditions induced the release of Zn and Fe into soil solution, and the subsequent individualization of Fe and Mn into Zn-rich concretions. Both processes and subsequent aging of the concretions formed induced significant exportation of Zn through the bottom water table. Secondary redox conditions promoted the weathering of Fe and Mn oxides in cements and concretions. This process caused other losses of Zn through lateral exportation in an upper water table. Concomitantly, eluviation occurred at the top of the solum. The lateral exportation of eluviated minerals through the upper water table limited illuviation. Eluviation was also responsible for Zn loss, but this Zn bound to phyllosilicates was not bioavailable.展开更多
Fluid infiltration into retrograde granulites of the Southern Marginal Zone （Limpopo high grade terrain） is exemplified by hydration reactions, shear zone hosted metasomatism, and lode gold mineralisation. Hydration...Fluid infiltration into retrograde granulites of the Southern Marginal Zone （Limpopo high grade terrain） is exemplified by hydration reactions, shear zone hosted metasomatism, and lode gold mineralisation. Hydration reactions include the breakdown of cordierite and orthopyroxene to gedrite ＋ kyanite, and anthophyllite, respectively. Metamorphic petrology, fluid inclusions, and field data indicate that a low H2O-activity carbon-saturated CO2-rich and a saline aqueous fluid infiltrated the Southern Marginal Zone during exhumation. The formation of anthophyllite after orthopyroxene established a regional retrograde anthophyllite-in isograd and occurred at P-Tconditions of -6 kbar and 610 ℃, which fixes the minimum mole fraction of H20 in the CO2-rich fluid phase at ~ 0.1. The maximum H20 mole fraction is fixed by the lower temperature limit （~800 ℃） for partial melting at -0.3. C-O-H fluid calculations show that the CO2-rich fluid had an oxygen fugacity that was 0.6 log10 units higher than that of the fayalite-magnetite- quartz buffer and that the CO2/（CO2＋CH4） mole ratio of this fluid was 1. The presence of dominantly relatively low density CO2-rich fluid inclusions in the hydrated granulites indicates that the fluid pressure was less than the lithostatic pressure. This can be explained by strike slip faulting and/or an increase of the rock permeability caused by hydration reactions.展开更多
The cumulative effects of periodic redox cycling on the mobility of As,Fe,and S from alluvial sediment to groundwater were investigated in bioreactor experiments.Two particular sediments from the alluvial floodplain o...The cumulative effects of periodic redox cycling on the mobility of As,Fe,and S from alluvial sediment to groundwater were investigated in bioreactor experiments.Two particular sediments from the alluvial floodplain of the Mekong Delta River were investigated: Matrix A (14 m deep) had a higher pyrite concentration than matrix B (7 m deep) sediments.Gypsumwas present in matrix B but absent in matrix A.In the reactors,the sediment suspensions were supplemented with As(III) and SO4^2-,and were subjected to three full-redox cycles entailing phases of nitrogen/CO2,compressed air sparging,and cellobiose addition.Major differences in As concentration and speciation were observed upon redox cycling.Evidences support the fact that initial sediment composition is the main factor controlling arsenic release and its speciation during the redox cycles.Indeed,a high pyrite content associated with a low SO4^2- content resulted in an increase in dissolved As concentrations,mainly in the form of As(III),after anoxic half-cycles;whereas a decrease in As concentrations mainly in the form of As(V),was instead observed after oxic half-cycles.In addition,oxic conditions were found to be responsible for pyrite and arsenian pyrite oxidation,increasing the As pool available for mobilization.The same processes seem to occur in sediment with the presence of gypsum,but,in this case,dissolved As were sequestered by biotic or abiotic redox reactions occurring in the FeeS system,and by specific physico-chemical condition (e.g.pH).The contrasting results obtained for two sediments sampled from the same core show that many complexes and entangled factors are at work,and further refinement is needed to explain the spatial and temporal variability of As release to groundwater of the Mekong River Delta (Vietnam).展开更多
Laser-driven ramp compression was used to investigate iron characteristics along the isentropic path. The iterative Lagrangian analysis method was employed to analyze the free surface velocity profiles in iron stepped...Laser-driven ramp compression was used to investigate iron characteristics along the isentropic path. The iterative Lagrangian analysis method was employed to analyze the free surface velocity profiles in iron stepped target measured with two VISARs. The onset stress for the α to ε phase transformation was determined from the sudden change in the sound velocity and was found over-pressurized compared to the static and shock results. The derived stress（26 GPa） and strain rate（up to 10-8 s^-1） are consistent with our previous experimental results. The stress-density relations were compared with those from previous ramp experiments and good agreements were found, which experimentally confirms the simulations,showing that iterative Lagrangian analysis can be applied to the ramp-compression data with weak shock.展开更多
In-plane heteroatom substitution of graphene is a promising strategy to modify its properties. The ability to dope graphene with electron-donor nitrogen heteroatoms is highly important for modulating electrical proper...In-plane heteroatom substitution of graphene is a promising strategy to modify its properties. The ability to dope graphene with electron-donor nitrogen heteroatoms is highly important for modulating electrical properties of graphene. Here we demonstrate a transfer-free method to directly grow large area quasi free-standing N-doped graphene bilayers on an insulating substrate （Si3N4）. Electron-bombardment heating under nitrogen flux results in simultaneous growth of N-doped graphene and a Si3N4 layer on the SiC surface. The decoupling of N-doped graphene from the substrate and the presence of Si3N4 are identified by X-ray photoemission spectroscopy and low-energy electron diffraction. The substitution of nitrogen atoms in the graphene planes was confirmed using high resolution X-ray photoemission spectroscopy which reveals several atomic configurations for the nitrogen atoms： Graphitic-like, pyridine-like, and pyrrolic- like. Furthermore, we demonstrated for the first time that N-doped graphene could be used to efficiently probe oxygen molecules via nitrogen atom defects.展开更多
In this study,the flocculation and the subsequent decantation step of mixed suspensions of 10 nm-sizedγ-Fe_(2)O_(3) magnetic nanoparticles and 500 nm-sized beidellite clay platelets was investigated.This work may fin...In this study,the flocculation and the subsequent decantation step of mixed suspensions of 10 nm-sizedγ-Fe_(2)O_(3) magnetic nanoparticles and 500 nm-sized beidellite clay platelets was investigated.This work may find application in the field of water treatment,specifically the flocculation processes with magnetically assisted sedimentation.After a short description of the preparation and characterization of the raw materials(nanoparticles and clays),the influence of several parameters(pH,concentrations of nanoparticles and clays etc.)on the amount of flocculated materials was examined,which gave information on the concentration ranges allowing a complete flocculation,together with a better understanding on the interactions between nanoparticles and clays responsible for flocculation.The optimal conditions for magnetically assisted settling were then determined by comparing for each sample sedimentation velocities under gravity and in the presence of a Nd-Fe-B magnet.Finally,the complex multiscale structure of the flocs in water was explored,through the measurement of several bulk properties(zeta-potential and volume measurements,laser granulometry),while the organization of the materials at a microscopic scale was investigated by cryo-transmission electron microscopy(cryo-TEM)and small-angle X-ray scattering(SAXS).展开更多
Fe3O4(magnetite), a-Fe2O3(hematite), and Fe O(wu¨ stite) are the three major iron oxides and some of the most fundamental solids in nature. Interest in these systems is due to their abundance as minerals in the E...Fe3O4(magnetite), a-Fe2O3(hematite), and Fe O(wu¨ stite) are the three major iron oxides and some of the most fundamental solids in nature. Interest in these systems is due to their abundance as minerals in the Earth and other telluric planets as well as their interesting electronic and magnetic properties which have been studied for decades. In this article, we review high-pressure studies on these three systems using neutron powder diffraction in the0–14 GPa range with a particular focus on the behavior of magnetism under pressure. Unpublished data on the pressure dependence of the Ne′el temperature in Fe O are presented. This review will give at the same time an introduction into technical aspects and illustrate the potential of high-pressure neutron scattering in the future.展开更多
The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC（0001） substrate and d...The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC（0001） substrate and demonstrate the formation of periodic arrangement of monolayer graphene on planar （0001） terraces and Bernal bilayer graphene on （1120） nanofacets of SiC. We investigate these lateral superlattices using Raman spectroscopy, atomic force microscopy/ electrostatic force microscopy （AFM/EFM） and X-ray and angle resolved photoemission spectroscopy （XPS/ARPES）. The correlation of EFM and ARPES reveals the appearance of permanent electronic band gaps in AB-stacked bilayer graphene on （1120） SiC nanofacets of 150 meV. This feature is confirmed by density functional theory （DFT） calculations. The charge transfer between the substrate and graphene bilayer results in an asymmetric charge distribution between the top and the bottom graphene layers opening an energy gap. This surface organization can be thus defined as self-organized metal-semiconductor graphene.展开更多
基金the financial support from the Science, Technology, and Innovation Funding Authority (STIFA, STDF previously) through project number 42691 entitled “Microstructure-Based, Multi-Physics Simulation and Optimization to Improve Battery Performance”supported by the U.S. DOE (Department of Energy), Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357supported by the U.S. DOE Vehicle Technologies office, under contract number DE-AC02-06CH11357
文摘This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in situ and ex situ X-ray diffraction,Raman spectroscopy,X-ray photoelectron spectroscopy,and transmission electron microscopy,the research unravels the complex structural and chemical evolution of MoS_(2) throughout its cycling.A key discovery is the identification of a unique Li intercalation mechanism in MoS_(2),leading to the formation of reversible Li_(2)MoS_(2) phases that contribute to the extra capacity of the MoS_(2) electrode.Density function theory calculations suggest the potential for overlithiation in MoS_(2),predicting Li5MoS_(2) as the most energetically favorable phase within the lithiation–delithiation process.Additionally,the formation of a Li-rich phase on the surface of Li_(4)MoS_(2) is considered energetically advantageous.After the first discharge,the battery system engages in two main reactions.One involves operation as a Li-sulfur battery within the carbonate electrolyte,and the other is the reversible intercalation and deintercalation of Li in Li_(2)MoS_(2).The latter reaction contributes to the extra capacity of the battery.The incorporation of reduced graphene oxide as a conductive additive in MoS_(2) electrodes notably improves their rate capability and cycling stability.
基金supported by the National Key R&D Program of China (2016YFB0100500)Special fund of key technology research and development projects (20180201097GX) (20180201099GX) (20180201096GX) (20190302130GX)+1 种基金Jilin province science and technology department. The R&D Program of power batteries with low temperature and high energy, Science and Technology Bureau of Changchun (19SS013)Key Subject Construction of Physical Chemistry of Northeast Normal University。
文摘Inspired by the concept of "polymer-in-ceramic",a composite poly(ε-caprolactone)(PCL)/ceramic containing LiTFSI is prepared and investigated as a solid electrolyte for all-solid-state batteries.The composite with the optimum concentration of 45 wt% LiTFSI and 75 wt% Li1.5Al0.5Ge1.5(PO4)3(LAGP,NASICON-type structure) exhibits a high ionic conductivity(σi=0.17 mS cm-1) at 30℃,a transference number of 0.30,and is stable up to 5.0 V.The composite electrolyte is a flexible and self-standing membrane.Solid-state LiFePO4//Li batteries with this composite electrolyte demonstrate excellent cycling stability with high discharge capacity of 157 mA h g-1,high capacity retention of 96% and coulombic efficiency of 98.5% after 130 cycles at 30℃ and 0.1 C rate.These electrochemical properties are better than other PCL-based allsolid-lithium batteries,and validate the concept of "polymer-in-ceramic" by avoiding the drawback of lower conductivity in prior "polymer-in-ceramic" electrolyte at high concentration of the ceramic.
文摘At peak granulite-facies metamorphic conditions, lower continental crust is arguably fluxed by large amounts of two key low water activity fluids： （i） high-density CO2 and/or （ii） concentrated saline so- lutions. These fluids are either internally-derived, generated by mineral reactions or dehydration melting or, notably for CO2, externally-derived, issued from the underlying mantle. Postmetamorphic evolution results in complete disappearance of these fluids, except for minute remnants preserved in minerals as fluid inclusions. Two major processes are involved： （i） at peak conditions, granitoid magmas form, migrate upward, and crystallize as shallow intrusions in the upper crust （mineralized porphyry types or reduced intrusions）; （ii） during the rapid decompression which almost systematically follows a period of post-peak isobaric cooling, especially for ultrahigh-temperature granulites （anticlockwise P-T paths）, quartz-carbonate megashear zones are formed by repeated periods of seismic activity. Seismic activity may continue until all free fluids have disappeared, resulting in the ultramylonites and pseudotachylites that are found in many granulite domes. A great majority of vein-type Au deposits worldwide occur in the above-mentioned settings or nearby. We suggest that the Au has been scavenged by the granulite fluids, then redistributed and concentrated during the formation of veins and related phenomena.
文摘The formation of continents involves a combination of magmatic and metamorphic processes. These processes become indistinguishable at the crust-mantle interface, where the pressure-temperature（P-T）conditions of（ultra） high-temperature granulites and magmatic rocks are similar. Continents grow laterally, by magmatic activity above oceanic subduction zones（high-pressure metamorphic setting）, and vertically by accumulation of mantle-derived magmas at the base of the crust（high-temperature metamorphic setting）. Both events are separated from each other in time; the vertical accretion postdating lateral growth by several tens of millions of years. Fluid inclusion data indicate that during the high-temperature metamorphic episode the granulite lower crust is invaded by large amounts of low H2O-activity fluids including high-density CO2 and concentrated saline solutions（brines）. These fluids are expelled from the lower crust to higher crustal levels at the end of the high-grade metamorphic event. The final amalgamation of supercontinents corresponds to episodes of ultra-high temperature metamorphism involving large-scale accumulation of these low-water activity fluids in the lower crust.This accumulation causes tectonic instability, which together with the heat input from the subcontinental lithospheric mantle, leads to the disruption of supercontinents. Thus, the fragmentation of a supercontinent is already programmed at the time of its amalgamation.
文摘Recalling some of the most important events and persons during his education and career, the author sketches his growth from a young engineer, educated in the sanctuary of solid state reactions, to an involved fully devoted scientific career for the study of fluids in the deep Earth. Most important in this respect was the discovery of C02 inclusions in granulites, which triggered years of discussion on fluid- absent or fluid-assisted granulite metamorphism. To some extent, this debate is a continuation of the former granite controversy, but it shows also how the famous battle of ＂soaks against pontiffs＂ could have been easily avoided.
文摘Fluid （and melt） inclusion studies have shown a marked devel- opment in the last decades, as indicated by the increasing number of papers and as covered under major themes in specialized meetings （e.g. ECROFI in Europe, PACROFI in America, ACROFI in Asia）. However, a basic text book is lacking in current literature, available information being either somewhat outdated （e,g. Roedder, 1984） or scattered in multi-author ＂short course＂, mainly organized by the Mineralogical Societies of Canada, America or Europe. A result is that basic features of fluid inclusion studies, notably its key technique, microthermometry, and recently supplemented by micro Raman of infrared spectroscopy, is rarely taught in most universities, leaving the student alone to discover a field of study which has grown to the dimensions of a major science.
基金Project supported by the "GDR TRANSMET" Program of the Centre National de la Recherche Scientifique (CNRS),France.
文摘The long-term redistribution of Zn in a naturally Zn-enriched soil during pedogenesis was quantified based on mass balance calculations. According to their fate, parent limestones comprised three Zn pools: bound to calcite and pyritesphalerite grains, bound to phyllosilicates and bound to goethite in the inherited phosphate nodules. Four pedological processes, i.e., carbonate dissolution, two stages of redox processes and eluviation, redistributed Zn during pedogenesis. The carbonate dissolution of limestones released Zn bound to calcite into soil solution. Due to residual enrichment, Zn concentrations in the soil are higher than those in parent limestones. Birnessite, ferrihydrite and goethite dispersed in soil horizon trapped high quantities of Zn during their formation. Afterwards, primary redox conditions induced the release of Zn and Fe into soil solution, and the subsequent individualization of Fe and Mn into Zn-rich concretions. Both processes and subsequent aging of the concretions formed induced significant exportation of Zn through the bottom water table. Secondary redox conditions promoted the weathering of Fe and Mn oxides in cements and concretions. This process caused other losses of Zn through lateral exportation in an upper water table. Concomitantly, eluviation occurred at the top of the solum. The lateral exportation of eluviated minerals through the upper water table limited illuviation. Eluviation was also responsible for Zn loss, but this Zn bound to phyllosilicates was not bioavailable.
基金DDvR would like to thank the NRF(Grant No. IFR1202190048)the University of Johannesburg for financial support
文摘Fluid infiltration into retrograde granulites of the Southern Marginal Zone （Limpopo high grade terrain） is exemplified by hydration reactions, shear zone hosted metasomatism, and lode gold mineralisation. Hydration reactions include the breakdown of cordierite and orthopyroxene to gedrite ＋ kyanite, and anthophyllite, respectively. Metamorphic petrology, fluid inclusions, and field data indicate that a low H2O-activity carbon-saturated CO2-rich and a saline aqueous fluid infiltrated the Southern Marginal Zone during exhumation. The formation of anthophyllite after orthopyroxene established a regional retrograde anthophyllite-in isograd and occurred at P-Tconditions of -6 kbar and 610 ℃, which fixes the minimum mole fraction of H20 in the CO2-rich fluid phase at ~ 0.1. The maximum H20 mole fraction is fixed by the lower temperature limit （~800 ℃） for partial melting at -0.3. C-O-H fluid calculations show that the CO2-rich fluid had an oxygen fugacity that was 0.6 log10 units higher than that of the fayalite-magnetite- quartz buffer and that the CO2/（CO2＋CH4） mole ratio of this fluid was 1. The presence of dominantly relatively low density CO2-rich fluid inclusions in the hydrated granulites indicates that the fluid pressure was less than the lithostatic pressure. This can be explained by strike slip faulting and/or an increase of the rock permeability caused by hydration reactions.
基金the financial support of the doctoral scholarship from University Grenoble Alpes and Geochemistry group (ISTerre), which is part of Labex OSUG@2020 (ANR10 LAB56)
文摘The cumulative effects of periodic redox cycling on the mobility of As,Fe,and S from alluvial sediment to groundwater were investigated in bioreactor experiments.Two particular sediments from the alluvial floodplain of the Mekong Delta River were investigated: Matrix A (14 m deep) had a higher pyrite concentration than matrix B (7 m deep) sediments.Gypsumwas present in matrix B but absent in matrix A.In the reactors,the sediment suspensions were supplemented with As(III) and SO4^2-,and were subjected to three full-redox cycles entailing phases of nitrogen/CO2,compressed air sparging,and cellobiose addition.Major differences in As concentration and speciation were observed upon redox cycling.Evidences support the fact that initial sediment composition is the main factor controlling arsenic release and its speciation during the redox cycles.Indeed,a high pyrite content associated with a low SO4^2- content resulted in an increase in dissolved As concentrations,mainly in the form of As(III),after anoxic half-cycles;whereas a decrease in As concentrations mainly in the form of As(V),was instead observed after oxic half-cycles.In addition,oxic conditions were found to be responsible for pyrite and arsenian pyrite oxidation,increasing the As pool available for mobilization.The same processes seem to occur in sediment with the presence of gypsum,but,in this case,dissolved As were sequestered by biotic or abiotic redox reactions occurring in the FeeS system,and by specific physico-chemical condition (e.g.pH).The contrasting results obtained for two sediments sampled from the same core show that many complexes and entangled factors are at work,and further refinement is needed to explain the spatial and temporal variability of As release to groundwater of the Mekong River Delta (Vietnam).
基金Project supported by the National Basic Research Program of China(Grant No.2013CBA01503)the National Natural Science Foundation of China(Grant No.11103040)
文摘Laser-driven ramp compression was used to investigate iron characteristics along the isentropic path. The iterative Lagrangian analysis method was employed to analyze the free surface velocity profiles in iron stepped target measured with two VISARs. The onset stress for the α to ε phase transformation was determined from the sudden change in the sound velocity and was found over-pressurized compared to the static and shock results. The derived stress（26 GPa） and strain rate（up to 10-8 s^-1） are consistent with our previous experimental results. The stress-density relations were compared with those from previous ramp experiments and good agreements were found, which experimentally confirms the simulations,showing that iterative Lagrangian analysis can be applied to the ramp-compression data with weak shock.
文摘In-plane heteroatom substitution of graphene is a promising strategy to modify its properties. The ability to dope graphene with electron-donor nitrogen heteroatoms is highly important for modulating electrical properties of graphene. Here we demonstrate a transfer-free method to directly grow large area quasi free-standing N-doped graphene bilayers on an insulating substrate （Si3N4）. Electron-bombardment heating under nitrogen flux results in simultaneous growth of N-doped graphene and a Si3N4 layer on the SiC surface. The decoupling of N-doped graphene from the substrate and the presence of Si3N4 are identified by X-ray photoemission spectroscopy and low-energy electron diffraction. The substitution of nitrogen atoms in the graphene planes was confirmed using high resolution X-ray photoemission spectroscopy which reveals several atomic configurations for the nitrogen atoms： Graphitic-like, pyridine-like, and pyrrolic- like. Furthermore, we demonstrated for the first time that N-doped graphene could be used to efficiently probe oxygen molecules via nitrogen atom defects.
基金We wish to kindly thank Delphine Talbot and Aude Michel for their technical support,and Cedric Boissiere for the fruitful discussions.We equally acknowledge the local staffs of the ID02 and BM26 lines of the European Scientific Radiation Facility(ESRF)in Grenoble.
文摘In this study,the flocculation and the subsequent decantation step of mixed suspensions of 10 nm-sizedγ-Fe_(2)O_(3) magnetic nanoparticles and 500 nm-sized beidellite clay platelets was investigated.This work may find application in the field of water treatment,specifically the flocculation processes with magnetically assisted sedimentation.After a short description of the preparation and characterization of the raw materials(nanoparticles and clays),the influence of several parameters(pH,concentrations of nanoparticles and clays etc.)on the amount of flocculated materials was examined,which gave information on the concentration ranges allowing a complete flocculation,together with a better understanding on the interactions between nanoparticles and clays responsible for flocculation.The optimal conditions for magnetically assisted settling were then determined by comparing for each sample sedimentation velocities under gravity and in the presence of a Nd-Fe-B magnet.Finally,the complex multiscale structure of the flocs in water was explored,through the measurement of several bulk properties(zeta-potential and volume measurements,laser granulometry),while the organization of the materials at a microscopic scale was investigated by cryo-transmission electron microscopy(cryo-TEM)and small-angle X-ray scattering(SAXS).
文摘Fe3O4(magnetite), a-Fe2O3(hematite), and Fe O(wu¨ stite) are the three major iron oxides and some of the most fundamental solids in nature. Interest in these systems is due to their abundance as minerals in the Earth and other telluric planets as well as their interesting electronic and magnetic properties which have been studied for decades. In this article, we review high-pressure studies on these three systems using neutron powder diffraction in the0–14 GPa range with a particular focus on the behavior of magnetism under pressure. Unpublished data on the pressure dependence of the Ne′el temperature in Fe O are presented. This review will give at the same time an introduction into technical aspects and illustrate the potential of high-pressure neutron scattering in the future.
文摘The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC（0001） substrate and demonstrate the formation of periodic arrangement of monolayer graphene on planar （0001） terraces and Bernal bilayer graphene on （1120） nanofacets of SiC. We investigate these lateral superlattices using Raman spectroscopy, atomic force microscopy/ electrostatic force microscopy （AFM/EFM） and X-ray and angle resolved photoemission spectroscopy （XPS/ARPES）. The correlation of EFM and ARPES reveals the appearance of permanent electronic band gaps in AB-stacked bilayer graphene on （1120） SiC nanofacets of 150 meV. This feature is confirmed by density functional theory （DFT） calculations. The charge transfer between the substrate and graphene bilayer results in an asymmetric charge distribution between the top and the bottom graphene layers opening an energy gap. This surface organization can be thus defined as self-organized metal-semiconductor graphene.
