High energy synchrotron diffraction offers great potential to study the recrystallization kinetics of metallic materials. To study the formation of Goss texture （{ [10}（001）） of grain oriented （GO） silicon steel...High energy synchrotron diffraction offers great potential to study the recrystallization kinetics of metallic materials. To study the formation of Goss texture （{ [10}（001）） of grain oriented （GO） silicon steel during secondary recrystallization process, an in situ experiment using hi gh energy X-ray diffraction was designed. The results showed that the secondary recrystallization began when the heating temperature was 1,494 K, and the grains grew rapidly above this temperature. With an increase in annealing temperature, the large grains with 7 orientation [〈111〉//normal direction] formed and gradually occupied the dominant position. As the annealing temperature increased even further, the grains with Goss orientation to a very large size by devouring the 7 orientation grains that formed in the early annealing stage. A single crystal with a Goss orientation was observed in the GO silicon steel when the annealing temperature was 1,540 K.展开更多
The phase evolution and thermal expansion behavior in superalloy during heating play an essential role in controlling the size and distribution of precipitates,as well as optimizing thermomechanical properties.Synchro...The phase evolution and thermal expansion behavior in superalloy during heating play an essential role in controlling the size and distribution of precipitates,as well as optimizing thermomechanical properties.Synchrotron X-ray diffraction is able to go through the interior of sample and can be carried out with in situ environment,and thus,it can obtain more statistics information in real time comparing with traditional methods,such as electron and optical microscopies.In this study,in situ heating synchrotron X-ray diffraction was carried out to study the phase evolution in a typicalγ′phase precipitation strengthened Ni-based superalloy,Waspaloy,from 29 to 1050°C.Theγ′,γ,M_(23)C_(6)and M C phases,including their lattice parameters,misfits,dissolution behavior and thermal expansion coefficients,were mainly investigated.Theγ′phase and M_(23)C_(6)carbides appeared obvious dissolution during heating and re-precipitated when the temperature dropped to room temperature.Combining with the microscopy results,we can indicate that the dissolution of M_(23)C_(6)leads to the growth of grain andγ′phase cannot be completely dissolved for the short holding time above the solution temperature.Besides,the coefficients of thermal expansions of all the phases are calculated and fitted as polynomials.展开更多
High-energy synchrotron diffraction offers great potential for experimental study of recrystallization kinetics. An experimental design to study the recrystallization mechanism of interstitial-free （IF） steel was im...High-energy synchrotron diffraction offers great potential for experimental study of recrystallization kinetics. An experimental design to study the recrystallization mechanism of interstitial-free （IF） steel was implemented. The whole annealing process of cold-rolled IF steel with 80% reduction was observed in situ using high-energy X-ray diffraction （HEXRD）. The results show how the main texture component of IF steel change, i.e. the α [∥rolling direction （RD）] fiber texture decreases and the γ [∥normal direction （ND）] fiber texture increases. The important part of the α fiber texture is that both the {100} and {112} texture decrease at the beginning of recrystallization. The γ fiber texture increases at the early stage of recrystallization which stems from the increase of {111}. Nevertheless, the {111} does not change after recrystallization. The dynamic evolution of the main texture components {100}, {112}, {111} and {111} is given by in-situ HEXRD.展开更多
The lower mantle makes up more than a half of our planet’s volume. Mineralogical and petrological experiments on realistic bulk compositions under high pressure–temperature (P–T) conditions are essential for unders...The lower mantle makes up more than a half of our planet’s volume. Mineralogical and petrological experiments on realistic bulk compositions under high pressure–temperature (P–T) conditions are essential for understanding deep mantle processes. Such high P–T experiments are commonly conducted in a laser-heated diamond anvil cell, producing a multiphase assemblage consisting of 100 nm to submicron crystallite grains. The structures of these lower mantle phases often cannot be preserved upon pressure quenching;thus, in situ characterization is needed. The X-ray diffraction (XRD) pattern of such a multiphase assemblage usually displays a mixture of diffraction spots and rings as a result of the coarse grain size relative to the small X-ray beam size (3–5 lm) available at the synchrotron facilities. Severe peak overlapping from multiple phases renders the powder XRD method inadequate for indexing new phases and minor phases. Consequently, structure determination of new phases in a high P–T multiphase assemblage has been extremely difficult using conventional XRD techniques. Our recent development of multigrain XRD in high-pressure research has enabled the indexation of hundreds of individual crystallite grains simultaneously through the determination of crystallographic orientations for these individual grains. Once indexation is achieved, each grain can be treated as a single crystal. The combined crystallographic information from individual grains can be used to determine the crystal structures of new phases and minor phases simultaneously in a multiphase system. With this new development, we have opened up a new area of crystallography under the high P–T conditions of the deep lower mantle. This paper explains key challenges in studying multiphase systems and demonstrates the unique capabilities of high-pressure multigrain XRD through successful examples of its applications.展开更多
Rechargeable battery cycling performance and related safety have been persistent concerns.It is crucial to decipher the capacity fading induced by electrode material failure via a range of techniques.Among these,synch...Rechargeable battery cycling performance and related safety have been persistent concerns.It is crucial to decipher the capacity fading induced by electrode material failure via a range of techniques.Among these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation mechanisms.In this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray methodologies.Subsequently,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,respectively.At last,we envision the future of exploring material failure mechanism.展开更多
We present a fast synchrotron X-ray tomography study of the packing structures of rods with different aspect ratios. Utilizing the high flux of the X-rays generated from the third-generation synchrotron source, we can...We present a fast synchrotron X-ray tomography study of the packing structures of rods with different aspect ratios. Utilizing the high flux of the X-rays generated from the third-generation synchrotron source, we can complete a high- resolution tomography scan within a short period of time, after which the three-dimensional （3D） packing structure can be obtained for the subsequent structural analysis. The image phase-retrieval procedure has been implemented to enhance the image contrast. We systematically investigated the effects of particle shape and aspect ratio on the structural properties including packing density and contact number. It turns out that large aspect ratio rod packings will have wider distributions of free volume fraction and larger mean contact numbers.展开更多
Fluorine-free electrolytes have attracted great attention because of its low-cost and environmental friendliness. However, so far, little is known about the solution structures of these electrolytes. Here,we compare t...Fluorine-free electrolytes have attracted great attention because of its low-cost and environmental friendliness. However, so far, little is known about the solution structures of these electrolytes. Here,we compare the solvation phenomenon of sodium tetraphenylborate(NaBPh_(4)) salt dissolved in organic solvents of propylene carbonate(PC), 1,2-dimethoxyethane(DME), acetonitrile(ACN) and tetrahydrofuran(THF). Small-angle X-ray scattering(SAXS) reveals a unique two-peak structural feature in this saltconcentrated PC electrolyte, while solutions using other solvents only have one scattering peak.Molecular dynamics(MD) simulations further reveal that there are anion-based clusters in addition to the short-range charge ordering in the concentrated NaBPh4/PC electrolyte. Raman spectroscopy confirms the existence of considerable contact ion pairs(CIPs). This work emphasizes the importance of global and local structural analysis, which will provide valuable clues for understanding the structureperformance relationship of electrolytes.展开更多
A multiscale crystal plasticity model accounting for temperature-dependent mechanical behaviors without introducing a larger number of unknown parameters was developed.The model was implemented in elastic-plastic self...A multiscale crystal plasticity model accounting for temperature-dependent mechanical behaviors without introducing a larger number of unknown parameters was developed.The model was implemented in elastic-plastic self-consistent(EPSC)and crystal plasticity finite element(CPFE)frameworks for grain-scale simulations.A computationally efficient EPSC model was first employed to estimate the critical resolved shear stress and hardening parameters of the slip and twin systems available in a hexagonal close-packed magnesium alloy,ZEK100.The constitutive parameters were thereafter refined using the CPFE.The crystal plasticity frameworks incorporated with the temperature-dependent constitutive model were used to predict stress–strain curves in macroscale and lattice strains in microscale at different testing temperatures up to 200℃.In particular,the predictions by the crystal plasticity models were compared with the measured lattice strain data at the elevated temperatures by in situ high-energy X-ray diffraction,for the first time.The comparison in the multiscale improved the fidelity of the developed temperature-dependent constitutive model and validated the assumption with regard to the temperature dependency of available slip and twin systems in the magnesium alloy.Finally,this work provides a time-efficient and precise modeling scheme for magnesium alloys at elevated temperatures.展开更多
High-pressure β-Sn germanium may transform into diverse metastable allotropes with distinctive nanostructures and unique physical properties via multiple pathways under decompression.However,the mechanism and transit...High-pressure β-Sn germanium may transform into diverse metastable allotropes with distinctive nanostructures and unique physical properties via multiple pathways under decompression.However,the mechanism and transition kinetics remain poorly understood.Here,we investigate the formation of metastable phases and nanostructures in germanium via controllable transition pathways of β-Sn Ge under rapid decompression at different rates.High-resolution transmission electron microscopy reveals three distinct metastable phases with the distinctive nanostructures:an almost perfect st12 Ge crystal,nanosized bc8/r8 structures with amorphous boundaries,and amorphous Ge with nanosized clusters (0.8–2.5 nm).Fast in situ x-ray diffraction and x-ray absorption measurements indicate that these nanostructured products form in certain pressure regions via distinct kinetic pathways and are strongly correlated with nucleation rates and electronic transitions mediated by compression rate,temperature,and stress.This work provides deep insight into the controllable synthesis of metastable materials with unique crystal symmetries and nanostructures for potential applications.展开更多
Grain-twin interactions are significant in texture modification under thermodynamic driving force.In this study,annealing-driven twinning/detwinning behavior,grain growth,and corresponding texture evolution in a pre-d...Grain-twin interactions are significant in texture modification under thermodynamic driving force.In this study,annealing-driven twinning/detwinning behavior,grain growth,and corresponding texture evolution in a pre-deformed AZ31 magnesium alloy were systematically tracked and investigated via in-situ heating synchrotron X-ray diffraction and quasi in-situ electron backscattered diffraction techniques.A twinning texture is generated in the pre-deformed sample due to the activation of{1012}tensile twinning.During annealing,dislocation annihilation occurs between 100 and 280℃,and recrystallization occurs above 280℃,manifesting as the initial residual matrix and twins being competitively swallowed by each other,forming a bimodal texture.The recrystallization process is completed by boundary movement,which depends on the energy difference across the boundary.In addition,it is found that the grain boundaries favor movement towards the side with higher stored energy,regardless of the boundary type or the boundary energy.展开更多
The advancement of efficient,cheap,and durable catalysts for oxygen reduction reaction(ORR)to substitute Pt/C in metal-air batteries is of paramount importance.However,traditional solvent-based methods fall short in t...The advancement of efficient,cheap,and durable catalysts for oxygen reduction reaction(ORR)to substitute Pt/C in metal-air batteries is of paramount importance.However,traditional solvent-based methods fall short in terms of environmental benign and scalability.Herein,a solvent-free organic-inorganic selfassembly approach is explored to construct cobalt single atom and cobalt nanocluster decorated nitrogendoped porous carbon spheres(Co-SA/NC@NCS).The solvent-free synthesis demonstrates an impressively high yield(282 g/L)and the resultant Co-SA/NC@NCS possesses a high N content(6.9 wt%).Density functional theory calculations disclose that the Co-SAs and Co-NCs are able to optimize the surface oxygen adsorption capability and enhance the conductivity of the NCS,thereby facilitating the ORR performance.The sol vent-free synthesis is also feasible for the synthesis of other non-noble metal element(Fe,Ni,and Zn)decorated nitrogen-doped porous carbon spheres.展开更多
Maraging steels are known for their exceptional strength but suffer from limited work hardening and ductility.Here,we report an intermittent printing strategy to tailor the microstructure and mechanical properties of ...Maraging steels are known for their exceptional strength but suffer from limited work hardening and ductility.Here,we report an intermittent printing strategy to tailor the microstructure and mechanical properties of maraging 250 steel via tuning the thermal history during wire-arc directed energy deposition.By introducing a dwell time between adjacent layers,the maraging 250 steel is cooled below the martensite start temperature,triggering thermally-driven martensitic transformation during the printing process.Thermal cycling during subsequent layer deposition results in the formation of reverted austenite which shows a refined microstructure and induces elemental segregation between martensite and reverted austenite.The Ni enrichment in the austenite promotes stabilization of the reverted austenite upon cooling to room temperature.The reverted austenite is metastable during deformation,leading to strain-induced martensitic transformation under loading.Specifically,a 3 min interlayer dwell time produces a maraging 250 steel with approximately 8% reverted austenite,resulting in improved work hardening via martensitic transformation induced plasticity during deformation.Meanwhile,the higher cooling rate and refined prior austenite grains lead to substantially refined martensitic grains(by approximately fivefold)together with an increased dislocation density.With 3 min interlayer dwell time,the yield strength of the printed maraging 250 steel increases from 836 MPa to 990 MPa,and the uniform elongation is doubled from 3.2% to 6.5%.This intermittent deposition strategy demonstrates the potential to tune the microstructure of maraging steels for achieving strength-ductility synergy by engineering the thermal history during additive manufacturing.展开更多
Iron-and manganese-based layered metal oxides,as cathodes for sodium ion batteries,have received widespread attention because of the low cost and high specific capacity.However,the Jahn-teller effect of Mn^(3+)ions an...Iron-and manganese-based layered metal oxides,as cathodes for sodium ion batteries,have received widespread attention because of the low cost and high specific capacity.However,the Jahn-teller effect of Mn^(3+)ions and the resulted unstable structure usually lead to continuously capacity decay.Herein,Titanium(Ti)has been successfully doped into Na_(2/3)Fe_(2/3)Mn_(2/3)O_(2)to suppress the Jahn-Teller distortion and improve both cycling and rate performance of sodium ion batteries.In situ high-energy synchrotron X-ray diffraction study shows that Ti-doped compound(Na_(2/3)Fe_(1/3)Mn_(0.57)Ti_(0.1)O_(2))can maintain the single P2 phase without any phase transition during the whole charging/discharging process.Various electrochemical characterizations are also applied to explore the better kinetics of sodium ions transfer in the Na_(2/3)Fe_(1/3)Mn_(0.5)7 Ti_(0.1)O_(2).This work provides a comprehensive insight into the Ti-doping effects on the performance from both structural and electro kinetic perspectives.展开更多
Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a b...Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a big challenge.Herein,a spray-drying strategy is adopted to construct graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene microsphere network.The unique structural and compositional advantages endow these electrodes to exhibit outstanding electrochemical properties with remarkable rate performance and long cycle life.Mechanism analyses further explain the outstanding electrochemical properties from the structural aspect.展开更多
The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicati...The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicating the occurrence of a liquid-state phase transition driven by entropy.However,the underlying mechanism of the polyamorphous phase transition remains unsettled.In the paper,in situ scattering techniques were employed to reveal multiscale structure evidence in a Mg65Cu15Ag10Gd10metallic glass with an anomalous exothermic peak upon heating.Resistivity measurements indicate a reentrant behavior for the Mg-Cu-Ag-Gd metallic glass in the anomalous exothermic peak temperature region during heating.In situ synchrotron diffraction results revealed that the local atomic structure tends to be ordered and loosely packed first,followed by reentering into the initial state upon heating.Moreover,time-resolved small-angle synchrotron X-ray scattering(SAXS) results show an increase in nanoscale heterogeneity first followed by a reentrant supercooled liquid behavior.A core-shell structure model has been used to fit the SAXS profiles when polyamorphous phase transition occurs.In contrast,there is no structure anomaly for the reference Mg-Cu-Gd alloy system.The detailed multiscale structural evidence suggests the occurrence of a liquid-liquid phase transition followed by a reentrant behavior in the MgCu-Ag-Gd metallic glass.Our results deepen the understanding of the structural origin of the glass-forming ability and shed light on the possibility of tuning the physical and mechanical properties by heat-treatment in the supercooled liquid region of Mg-based metallic glasses.展开更多
High-voltage LiCoO_(2)(LCO) is an attractive cathode for ultra-high energy density lithium-ion batteries(LIBs) in the 3 C markets.However,the sluggish lithium-ion diffusion at high voltage significantly hampers its ra...High-voltage LiCoO_(2)(LCO) is an attractive cathode for ultra-high energy density lithium-ion batteries(LIBs) in the 3 C markets.However,the sluggish lithium-ion diffusion at high voltage significantly hampers its rate capability.Herein,combining experiments with density functional theory(DFT) calculations,we demonstrate that the kinetic limitations can be mitigated by a facial Mg^(2+)+Gd^(3+)co-doping method.The as-prepared LCO shows significantly enhanced Li-ion diffusion mobility at high voltage,making more homogenous Li-ion de/intercalation at a high-rate charge/discharge process.The homogeneity enables the structural stability of LCO at a high-rate current density,inhibiting stress accumulation and irreversible phase transition.When used in combination with a Li metal anode,the doped LCO shows an extreme fast charging(XFC) capability,with a superior high capacity of 193.1 mAh g^(-1)even at the current density of 20 C and high-rate capacity retention of 91.3% after 100 cycles at 5 C.This work provides a new insight to prepare XFC high-voltage LCO cathode materials.展开更多
For electrochemical CO_(2) reduction to HCOOH,an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density(JHCOOH)at a low overpotential.Indium oxide is good HCOOH ...For electrochemical CO_(2) reduction to HCOOH,an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density(JHCOOH)at a low overpotential.Indium oxide is good HCOOH production catalyst but with low con-ductivity.In this work,we report a unique corn design of In_(2)O_(3-x)@C nanocatalyst,wherein In_(2)O_(3-x)nanocube as the fine grains dispersed uniformly on the carbon nanorod cob,resulting in the enhanced conductivity.Excellent performance is achieved with 84%Faradaic efficiency(FE)and 11 mA cm^(−2)JHCOOH at a low potential of−0.4 V versus RHE.At the current density of 100 mA cm^(−2),the applied potential remained stable for more than 120 h with the FE above 90%.Density functional theory calculations reveal that the abundant oxygen vacancy in In_(2)O_(3-x) has exposed more In^(3+) sites with activated electroactivity,which facilitates the formation of HCOO*intermediate.Operando X-ray absorp-tion spectroscopy also confirms In^(3+) as the active site and the key intermediate of HCOO*during the process of CO_(2) reduction to HCOOH.展开更多
基金supported by the Key Projects of the National Science & Technology Pillar Program (No. 2011BAE13B03)the Fundamental Research Funds for the Central Universities (No. N110502001)
文摘High energy synchrotron diffraction offers great potential to study the recrystallization kinetics of metallic materials. To study the formation of Goss texture （{ [10}（001）） of grain oriented （GO） silicon steel during secondary recrystallization process, an in situ experiment using hi gh energy X-ray diffraction was designed. The results showed that the secondary recrystallization began when the heating temperature was 1,494 K, and the grains grew rapidly above this temperature. With an increase in annealing temperature, the large grains with 7 orientation [〈111〉//normal direction] formed and gradually occupied the dominant position. As the annealing temperature increased even further, the grains with Goss orientation to a very large size by devouring the 7 orientation grains that formed in the early annealing stage. A single crystal with a Goss orientation was observed in the GO silicon steel when the annealing temperature was 1,540 K.
基金supported by the National Natural Science Foundation of China(NSFC)(Grant Nos.11805009 and 51921001)the Fundamental Research Funds for the Central Universities(Grant No.06111020)。
文摘The phase evolution and thermal expansion behavior in superalloy during heating play an essential role in controlling the size and distribution of precipitates,as well as optimizing thermomechanical properties.Synchrotron X-ray diffraction is able to go through the interior of sample and can be carried out with in situ environment,and thus,it can obtain more statistics information in real time comparing with traditional methods,such as electron and optical microscopies.In this study,in situ heating synchrotron X-ray diffraction was carried out to study the phase evolution in a typicalγ′phase precipitation strengthened Ni-based superalloy,Waspaloy,from 29 to 1050°C.Theγ′,γ,M_(23)C_(6)and M C phases,including their lattice parameters,misfits,dissolution behavior and thermal expansion coefficients,were mainly investigated.Theγ′phase and M_(23)C_(6)carbides appeared obvious dissolution during heating and re-precipitated when the temperature dropped to room temperature.Combining with the microscopy results,we can indicate that the dissolution of M_(23)C_(6)leads to the growth of grain andγ′phase cannot be completely dissolved for the short holding time above the solution temperature.Besides,the coefficients of thermal expansions of all the phases are calculated and fitted as polynomials.
基金Sponsored by Key Projects in National Science and Technology Pillar Program of China(2011BAE13B03)Fundamental Research Funds for Central Universities of China(N110502001)
文摘High-energy synchrotron diffraction offers great potential for experimental study of recrystallization kinetics. An experimental design to study the recrystallization mechanism of interstitial-free （IF） steel was implemented. The whole annealing process of cold-rolled IF steel with 80% reduction was observed in situ using high-energy X-ray diffraction （HEXRD）. The results show how the main texture component of IF steel change, i.e. the α [∥rolling direction （RD）] fiber texture decreases and the γ [∥normal direction （ND）] fiber texture increases. The important part of the α fiber texture is that both the {100} and {112} texture decrease at the beginning of recrystallization. The γ fiber texture increases at the early stage of recrystallization which stems from the increase of {111}. Nevertheless, the {111} does not change after recrystallization. The dynamic evolution of the main texture components {100}, {112}, {111} and {111} is given by in-situ HEXRD.
基金This work was supported by the National Natural Science Foundation of China (41574080 and U1530402).
文摘The lower mantle makes up more than a half of our planet’s volume. Mineralogical and petrological experiments on realistic bulk compositions under high pressure–temperature (P–T) conditions are essential for understanding deep mantle processes. Such high P–T experiments are commonly conducted in a laser-heated diamond anvil cell, producing a multiphase assemblage consisting of 100 nm to submicron crystallite grains. The structures of these lower mantle phases often cannot be preserved upon pressure quenching;thus, in situ characterization is needed. The X-ray diffraction (XRD) pattern of such a multiphase assemblage usually displays a mixture of diffraction spots and rings as a result of the coarse grain size relative to the small X-ray beam size (3–5 lm) available at the synchrotron facilities. Severe peak overlapping from multiple phases renders the powder XRD method inadequate for indexing new phases and minor phases. Consequently, structure determination of new phases in a high P–T multiphase assemblage has been extremely difficult using conventional XRD techniques. Our recent development of multigrain XRD in high-pressure research has enabled the indexation of hundreds of individual crystallite grains simultaneously through the determination of crystallographic orientations for these individual grains. Once indexation is achieved, each grain can be treated as a single crystal. The combined crystallographic information from individual grains can be used to determine the crystal structures of new phases and minor phases simultaneously in a multiphase system. With this new development, we have opened up a new area of crystallography under the high P–T conditions of the deep lower mantle. This paper explains key challenges in studying multiphase systems and demonstrates the unique capabilities of high-pressure multigrain XRD through successful examples of its applications.
基金supported by the U.S.National Science Foundation(2208972,2120559,and 2323117)
文摘Rechargeable battery cycling performance and related safety have been persistent concerns.It is crucial to decipher the capacity fading induced by electrode material failure via a range of techniques.Among these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation mechanisms.In this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray methodologies.Subsequently,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,respectively.At last,we envision the future of exploring material failure mechanism.
基金Project supported by the National Natural Science Foundation of China(Grant No.11175121)the National Basic Research Program of China(GrantNo.2010CB834301)supported by the U.S.DOE(Grant No.DE-AC02-06CH11357)
文摘We present a fast synchrotron X-ray tomography study of the packing structures of rods with different aspect ratios. Utilizing the high flux of the X-rays generated from the third-generation synchrotron source, we can complete a high- resolution tomography scan within a short period of time, after which the three-dimensional （3D） packing structure can be obtained for the subsequent structural analysis. The image phase-retrieval procedure has been implemented to enhance the image contrast. We systematically investigated the effects of particle shape and aspect ratio on the structural properties including packing density and contact number. It turns out that large aspect ratio rod packings will have wider distributions of free volume fraction and larger mean contact numbers.
基金supported as part of the Joint Center for Energy Storage Research,an Energy Innovation Hub funded by the U.S.Department of Energy,Office of Science,Basic Energy Sciencesthe supported by U.S.National Science Foundation(Grant No.2120559)。
文摘Fluorine-free electrolytes have attracted great attention because of its low-cost and environmental friendliness. However, so far, little is known about the solution structures of these electrolytes. Here,we compare the solvation phenomenon of sodium tetraphenylborate(NaBPh_(4)) salt dissolved in organic solvents of propylene carbonate(PC), 1,2-dimethoxyethane(DME), acetonitrile(ACN) and tetrahydrofuran(THF). Small-angle X-ray scattering(SAXS) reveals a unique two-peak structural feature in this saltconcentrated PC electrolyte, while solutions using other solvents only have one scattering peak.Molecular dynamics(MD) simulations further reveal that there are anion-based clusters in addition to the short-range charge ordering in the concentrated NaBPh4/PC electrolyte. Raman spectroscopy confirms the existence of considerable contact ion pairs(CIPs). This work emphasizes the importance of global and local structural analysis, which will provide valuable clues for understanding the structureperformance relationship of electrolytes.
基金the supports by the Fundamental Research Program of the Korea Institute of Materials Science(KIMS,PNK7760)。
文摘A multiscale crystal plasticity model accounting for temperature-dependent mechanical behaviors without introducing a larger number of unknown parameters was developed.The model was implemented in elastic-plastic self-consistent(EPSC)and crystal plasticity finite element(CPFE)frameworks for grain-scale simulations.A computationally efficient EPSC model was first employed to estimate the critical resolved shear stress and hardening parameters of the slip and twin systems available in a hexagonal close-packed magnesium alloy,ZEK100.The constitutive parameters were thereafter refined using the CPFE.The crystal plasticity frameworks incorporated with the temperature-dependent constitutive model were used to predict stress–strain curves in macroscale and lattice strains in microscale at different testing temperatures up to 200℃.In particular,the predictions by the crystal plasticity models were compared with the measured lattice strain data at the elevated temperatures by in situ high-energy X-ray diffraction,for the first time.The comparison in the multiscale improved the fidelity of the developed temperature-dependent constitutive model and validated the assumption with regard to the temperature dependency of available slip and twin systems in the magnesium alloy.Finally,this work provides a time-efficient and precise modeling scheme for magnesium alloys at elevated temperatures.
基金supported by the National Nature Science Foundation of China(NSFC)(Grant No.11974033)Xuqiang Liu acknowledges support from the National Postdoctoral Foundation Project of China under Grant No.GZC20230215+2 种基金the National Nature Science Foundation of China under Grants No.12404001The XRD measurements at room and high temperatures were performed at the 4W2 HPStation of the Beijing Synchrotron Radiation Facility(BSRF)and beamline 15U1 of the Shanghai Synchrotron Radiation Facility(SSRF)In situ high-pressure,low-temperature XRD measurements were conducted at sector 16 ID-B,HPCAT of the Advanced Photon Source,and were supported by DOE-NNSA under Award No.DE-NA0001974.
文摘High-pressure β-Sn germanium may transform into diverse metastable allotropes with distinctive nanostructures and unique physical properties via multiple pathways under decompression.However,the mechanism and transition kinetics remain poorly understood.Here,we investigate the formation of metastable phases and nanostructures in germanium via controllable transition pathways of β-Sn Ge under rapid decompression at different rates.High-resolution transmission electron microscopy reveals three distinct metastable phases with the distinctive nanostructures:an almost perfect st12 Ge crystal,nanosized bc8/r8 structures with amorphous boundaries,and amorphous Ge with nanosized clusters (0.8–2.5 nm).Fast in situ x-ray diffraction and x-ray absorption measurements indicate that these nanostructured products form in certain pressure regions via distinct kinetic pathways and are strongly correlated with nucleation rates and electronic transitions mediated by compression rate,temperature,and stress.This work provides deep insight into the controllable synthesis of metastable materials with unique crystal symmetries and nanostructures for potential applications.
基金the financial support from the Beijing Municipal Natural Science Foundation(No.2244096)the Fundamental Research Funds for the Central Universities(No.FRF-TP-24-007A)Use of the Advanced Photon Source and the Center for Nanoscale Materials,both Office of Science user facilities at Argonne National Laboratory,was supported by the US DOE,Office of Science and Office of Basic Energy Sciences,under contract number DE-AC02-06CH11357.
文摘Grain-twin interactions are significant in texture modification under thermodynamic driving force.In this study,annealing-driven twinning/detwinning behavior,grain growth,and corresponding texture evolution in a pre-deformed AZ31 magnesium alloy were systematically tracked and investigated via in-situ heating synchrotron X-ray diffraction and quasi in-situ electron backscattered diffraction techniques.A twinning texture is generated in the pre-deformed sample due to the activation of{1012}tensile twinning.During annealing,dislocation annihilation occurs between 100 and 280℃,and recrystallization occurs above 280℃,manifesting as the initial residual matrix and twins being competitively swallowed by each other,forming a bimodal texture.The recrystallization process is completed by boundary movement,which depends on the energy difference across the boundary.In addition,it is found that the grain boundaries favor movement towards the side with higher stored energy,regardless of the boundary type or the boundary energy.
基金supported by the National Natural Science Foundation of China(No.52072283)the program of China Scholarship Council(No.202306950008)。
文摘The advancement of efficient,cheap,and durable catalysts for oxygen reduction reaction(ORR)to substitute Pt/C in metal-air batteries is of paramount importance.However,traditional solvent-based methods fall short in terms of environmental benign and scalability.Herein,a solvent-free organic-inorganic selfassembly approach is explored to construct cobalt single atom and cobalt nanocluster decorated nitrogendoped porous carbon spheres(Co-SA/NC@NCS).The solvent-free synthesis demonstrates an impressively high yield(282 g/L)and the resultant Co-SA/NC@NCS possesses a high N content(6.9 wt%).Density functional theory calculations disclose that the Co-SAs and Co-NCs are able to optimize the surface oxygen adsorption capability and enhance the conductivity of the NCS,thereby facilitating the ORR performance.The sol vent-free synthesis is also feasible for the synthesis of other non-noble metal element(Fe,Ni,and Zn)decorated nitrogen-doped porous carbon spheres.
基金the U.S.Army Research Laboratory under Cooperative Agreement Award No.HQ0034-15-2-0007the U.S.National Science Foundation(DMR-2207965).
文摘Maraging steels are known for their exceptional strength but suffer from limited work hardening and ductility.Here,we report an intermittent printing strategy to tailor the microstructure and mechanical properties of maraging 250 steel via tuning the thermal history during wire-arc directed energy deposition.By introducing a dwell time between adjacent layers,the maraging 250 steel is cooled below the martensite start temperature,triggering thermally-driven martensitic transformation during the printing process.Thermal cycling during subsequent layer deposition results in the formation of reverted austenite which shows a refined microstructure and induces elemental segregation between martensite and reverted austenite.The Ni enrichment in the austenite promotes stabilization of the reverted austenite upon cooling to room temperature.The reverted austenite is metastable during deformation,leading to strain-induced martensitic transformation under loading.Specifically,a 3 min interlayer dwell time produces a maraging 250 steel with approximately 8% reverted austenite,resulting in improved work hardening via martensitic transformation induced plasticity during deformation.Meanwhile,the higher cooling rate and refined prior austenite grains lead to substantially refined martensitic grains(by approximately fivefold)together with an increased dislocation density.With 3 min interlayer dwell time,the yield strength of the printed maraging 250 steel increases from 836 MPa to 990 MPa,and the uniform elongation is doubled from 3.2% to 6.5%.This intermittent deposition strategy demonstrates the potential to tune the microstructure of maraging steels for achieving strength-ductility synergy by engineering the thermal history during additive manufacturing.
基金supported by the National Key R&D Program of China(2020YFA0406203)the Shenzhen Science and Technology Innovation Commission(SGDX2019081623240948,JCYJ20200109105618137)+1 种基金the ECS scheme(City U 21307019)the Shenzhen Research Institute,City University of Hong Kong。
文摘Iron-and manganese-based layered metal oxides,as cathodes for sodium ion batteries,have received widespread attention because of the low cost and high specific capacity.However,the Jahn-teller effect of Mn^(3+)ions and the resulted unstable structure usually lead to continuously capacity decay.Herein,Titanium(Ti)has been successfully doped into Na_(2/3)Fe_(2/3)Mn_(2/3)O_(2)to suppress the Jahn-Teller distortion and improve both cycling and rate performance of sodium ion batteries.In situ high-energy synchrotron X-ray diffraction study shows that Ti-doped compound(Na_(2/3)Fe_(1/3)Mn_(0.57)Ti_(0.1)O_(2))can maintain the single P2 phase without any phase transition during the whole charging/discharging process.Various electrochemical characterizations are also applied to explore the better kinetics of sodium ions transfer in the Na_(2/3)Fe_(1/3)Mn_(0.5)7 Ti_(0.1)O_(2).This work provides a comprehensive insight into the Ti-doping effects on the performance from both structural and electro kinetic perspectives.
基金financial support by the National Natural Science Foundation of China(Nos.21673165 and 21972108)National Key Research Program of China(No.2016YFB0901500)the supercomputing system in the Supercomputing Center of Wuhan University。
文摘Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a big challenge.Herein,a spray-drying strategy is adopted to construct graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene microsphere network.The unique structural and compositional advantages endow these electrodes to exhibit outstanding electrochemical properties with remarkable rate performance and long cycle life.Mechanism analyses further explain the outstanding electrochemical properties from the structural aspect.
基金financially supported by the National Natural Science Foundation of China(No.51871120)the Natural Science Foundation of Jiangsu Province(No.BK20200019)+4 种基金the Fundamental Research Funds for the Central Universities(Nos.30919011107 and 30919011404)support by Shenzhen Science and Technology Innovation Committee(No.JCYJ20170413140446951)the supports by Shenzhen Science and Technology Innovation Commission(No.JCYJ20180507181806316)the supports by Shenzhen Science and Technology Innovation Commission(No.JCYJ202000109105618137)the Ministry of Science and Technology of China(No.2016YFA0401501)。
文摘The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicating the occurrence of a liquid-state phase transition driven by entropy.However,the underlying mechanism of the polyamorphous phase transition remains unsettled.In the paper,in situ scattering techniques were employed to reveal multiscale structure evidence in a Mg65Cu15Ag10Gd10metallic glass with an anomalous exothermic peak upon heating.Resistivity measurements indicate a reentrant behavior for the Mg-Cu-Ag-Gd metallic glass in the anomalous exothermic peak temperature region during heating.In situ synchrotron diffraction results revealed that the local atomic structure tends to be ordered and loosely packed first,followed by reentering into the initial state upon heating.Moreover,time-resolved small-angle synchrotron X-ray scattering(SAXS) results show an increase in nanoscale heterogeneity first followed by a reentrant supercooled liquid behavior.A core-shell structure model has been used to fit the SAXS profiles when polyamorphous phase transition occurs.In contrast,there is no structure anomaly for the reference Mg-Cu-Gd alloy system.The detailed multiscale structural evidence suggests the occurrence of a liquid-liquid phase transition followed by a reentrant behavior in the MgCu-Ag-Gd metallic glass.Our results deepen the understanding of the structural origin of the glass-forming ability and shed light on the possibility of tuning the physical and mechanical properties by heat-treatment in the supercooled liquid region of Mg-based metallic glasses.
基金supported by the National Key R&D Program of China(2020YFA0406203)the Shenzhen Science and Technology Innovation Commission(JCYJ20180507181806316,JCYJ20200109105618137)+1 种基金the ECS Scheme(City U 21307019,City U7020043,City U7005500,City U7005612)the Shenzhen Research Institute,City University of Hong Kong。
文摘High-voltage LiCoO_(2)(LCO) is an attractive cathode for ultra-high energy density lithium-ion batteries(LIBs) in the 3 C markets.However,the sluggish lithium-ion diffusion at high voltage significantly hampers its rate capability.Herein,combining experiments with density functional theory(DFT) calculations,we demonstrate that the kinetic limitations can be mitigated by a facial Mg^(2+)+Gd^(3+)co-doping method.The as-prepared LCO shows significantly enhanced Li-ion diffusion mobility at high voltage,making more homogenous Li-ion de/intercalation at a high-rate charge/discharge process.The homogeneity enables the structural stability of LCO at a high-rate current density,inhibiting stress accumulation and irreversible phase transition.When used in combination with a Li metal anode,the doped LCO shows an extreme fast charging(XFC) capability,with a superior high capacity of 193.1 mAh g^(-1)even at the current density of 20 C and high-rate capacity retention of 91.3% after 100 cycles at 5 C.This work provides a new insight to prepare XFC high-voltage LCO cathode materials.
基金supported by Natural Science Foundation of China(21972006,U2001217,21771156)Shenzhen Science and Technology Innovation Commission(KCXFZ20201221173604012)+2 种基金Shenzhen Peacock Plan(KQTD2016053015544057)Shenzhen-Hong Kong Innovation Circle United Research Project(SGLH20180622092406130)supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under Contract No.DE-AC02-06CH11357.
文摘For electrochemical CO_(2) reduction to HCOOH,an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density(JHCOOH)at a low overpotential.Indium oxide is good HCOOH production catalyst but with low con-ductivity.In this work,we report a unique corn design of In_(2)O_(3-x)@C nanocatalyst,wherein In_(2)O_(3-x)nanocube as the fine grains dispersed uniformly on the carbon nanorod cob,resulting in the enhanced conductivity.Excellent performance is achieved with 84%Faradaic efficiency(FE)and 11 mA cm^(−2)JHCOOH at a low potential of−0.4 V versus RHE.At the current density of 100 mA cm^(−2),the applied potential remained stable for more than 120 h with the FE above 90%.Density functional theory calculations reveal that the abundant oxygen vacancy in In_(2)O_(3-x) has exposed more In^(3+) sites with activated electroactivity,which facilitates the formation of HCOO*intermediate.Operando X-ray absorp-tion spectroscopy also confirms In^(3+) as the active site and the key intermediate of HCOO*during the process of CO_(2) reduction to HCOOH.
