The structure transitions in cluster-cluster aggregation (CCA) and diffusion-limited aggregation (DLA) under external electric fields have been investigated by computer simulations. With the increase of external elect...The structure transitions in cluster-cluster aggregation (CCA) and diffusion-limited aggregation (DLA) under external electric fields have been investigated by computer simulations. With the increase of external electric field, there exists a structure transition from disorder to order, i. e., the aggregates change from fractals of diffusion-limited CCA and DLA to the electrorheological chains parallel to electric field. Pair distribution shows, the system changes from local order to long-range order gradually with the external field rising.展开更多
The atomic pair distribution function（PDF） reveals the interatomic distance in a material directly in real-space. It is a very powerful method to characterize the local structure of materials. With the help of the t...The atomic pair distribution function（PDF） reveals the interatomic distance in a material directly in real-space. It is a very powerful method to characterize the local structure of materials. With the help of the third generation synchrotron facility and spallation neutron source worldwide, the PDF method has developed quickly both experimentally and theoretically in recent years. Recently this method was successfully implemented at the Shanghai Synchrotron Radiation Facility（SSRF）. The data quality is very high and this ensures the applicability of the method to study the subtle structural changes in complex materials. In this article, we introduce in detail this new method and show some experimental data we collected.展开更多
Metal-organic frameworks(MOFs),a family of highly porous materials possessing huge surface areas and feasible chemical tunability,are emerging as critical functional materials to solve the growing challenges associate...Metal-organic frameworks(MOFs),a family of highly porous materials possessing huge surface areas and feasible chemical tunability,are emerging as critical functional materials to solve the growing challenges associated with energy-water systems,such as water scarcity issues.In this contribution,the roles of MOFs are highlighted in electrochemical-based water applications(i.e.,reactions,sensing,and separations),where MOF-based functional materials exhibit outstanding performances in detecting/removing pollutants,recovering resources,and harvesting energies from different water sources.Compared with the pristine MOFs,the efficiency and/or selectivity can be further enhanced via rational structural modulation of MOFs(e.g.,partial metal substitution)or integration of MOFs with other functional materials(e.g.,metal clusters and reduced graphene oxide).Several key factors/properties that affect the performances of MOF-based materials are also reviewed,including electronic structures,nanoconfined effects,stability,conductivity,and atomic structures.The advancement in the fundamental understanding of these key factors is expected to shed light on the functioning mechanisms of MOFs(e.g.,charge transfer pathways and guest-host interactions),which will subsequently accelerate the integration of precisely designed MOFs into electrochemical architectures to achieve highly effective water remediation with optimized selectivity and long-term stability.展开更多
The increased use of rechargeable batteries in portable electronic devices and the continuous develop-ment of novel applications （e.g. transportation and large scale energy storage）, have raised a strong de-mand for...The increased use of rechargeable batteries in portable electronic devices and the continuous develop-ment of novel applications （e.g. transportation and large scale energy storage）, have raised a strong de-mand for high performance batteries with increased energy density, cycle and calendar life, safety andlower costs. This triggers significant efforts to reveal the fundamental mechanism determining batteryperformance with the use of advanced analytical techniques. However, the inherently complex character-istics of battery systems make the mechanism analysis sophisticated and difficult. Synchrotron radiationis an advanced collimated light source with high intensity and tunable energies. It has particular ad-vantages in electronic structure and geometric structure （both the short-range and long-range structure）analysis of materials on different length and time scales. In the past decades, synchrotron X-ray tech-niques have been widely used to understand the fundamental mechanism and guide the technologicaloptimization of batteries. In particular, in situ and operando techniques with high spatial and temporalresolution, enable the nondestructive, real time dynamic investigation of the electrochemical reaction,and lead to significant deep insights into the battery operation mechanism. This review gives a brief introduction of the application of synchrotron X-ray techniques to the inves-tigation of battery systems. The five widely implicated techniques, including X-ray diffraction （XRD）, PairDistribution Function （PDF）, Hard and Soft X-ray absorption spectroscopy （XAS） and X-ray photoelectronspectroscopy （XPS） will be reviewed, with the emphasis on their in situ studies of battery systems during cycling.展开更多
The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Underst...The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Understanding the mechanism of the structure transition and atom rearrangement via synthesis or processing is key to expediting the exploration of excellent energy materials. In this work, in situ neutron scattering is employed to reveal the real-time structure evolution, including the TM-O bonds, lattice,TM valence and the migration of the high-voltage spinel cathode LiNi_(0.5)Mn_(1.5)O_(4). The transition-metalmediated spinel destabilization under the annealing at the oxygen-deficient atmosphere is pinpointed.The formation of Mn^(3+) is correlated to the TM migration activation, TM disordered rearrangement in the spinel, and the transition to a layered-rocksalt phase. The further TM interdiffusion and Mn^(3+) reduction are also revealed with multi-stage thermodynamics and kinetics. The mechanisms of phase transition and atom migrations as functions of temperature, time and atmosphere present important guidance on the synthesis in various-valence element containing oxides.展开更多
A well-established pseodopotential is used to study the structure of some 4f rare earth liquid metals （Ce, Pr, Eu, Gd, Tb, and Yb）. The structure factor S（q）, pair distribution function g（r）, interatomic distanc...A well-established pseodopotential is used to study the structure of some 4f rare earth liquid metals （Ce, Pr, Eu, Gd, Tb, and Yb）. The structure factor S（q）, pair distribution function g（r）, interatomic distance r1, and coordination number n1 are calculated using Charged Hard Sphere （CHS） reference system. To introduce the exchange and correlation effects, the local field correction due to Sarkar et al. （S） is applied. The present investigation is successful in generating the structural information of Ce, Pr, Eu, Gd, Tb, and Yb 4f rare earth liquid metals.展开更多
It has been a challenge to fully understand the structural characteristics of laser-irradiation induced amorphous(L-a) Ge2Sb2Te5(GST) alloy due to the difficulties of collecting diffraction data from high purity speci...It has been a challenge to fully understand the structural characteristics of laser-irradiation induced amorphous(L-a) Ge2Sb2Te5(GST) alloy due to the difficulties of collecting diffraction data from high purity specimens. In this paper,by fabricating GST thin films on different substrates,we exhibit an effective way of preparing L-a GST dots in submicron scale on various types of specially designed transmission electron microscope(TEM) grids. The structural characteristics of L-a GST in the form of pair distribution functions(PDF) can be achieved on single dots of L-a GST via selected area electron diffraction(SAED) . This general approach would be convenient for precisely producing laser-irradiation induced materials in submicron scale for structural investigation.展开更多
文摘The structure transitions in cluster-cluster aggregation (CCA) and diffusion-limited aggregation (DLA) under external electric fields have been investigated by computer simulations. With the increase of external electric field, there exists a structure transition from disorder to order, i. e., the aggregates change from fractals of diffusion-limited CCA and DLA to the electrorheological chains parallel to electric field. Pair distribution shows, the system changes from local order to long-range order gradually with the external field rising.
基金Project supported by the National Natural Science Foundation of China(Grant No.U1232112)the National Key Basic Research Program of China(Grant No.2012CB825700)
文摘The atomic pair distribution function（PDF） reveals the interatomic distance in a material directly in real-space. It is a very powerful method to characterize the local structure of materials. With the help of the third generation synchrotron facility and spallation neutron source worldwide, the PDF method has developed quickly both experimentally and theoretically in recent years. Recently this method was successfully implemented at the Shanghai Synchrotron Radiation Facility（SSRF）. The data quality is very high and this ensures the applicability of the method to study the subtle structural changes in complex materials. In this article, we introduce in detail this new method and show some experimental data we collected.
基金supported by the start-up package and COES Institutional Research Incentive Program at the Florida Institute of Technology.
文摘Metal-organic frameworks(MOFs),a family of highly porous materials possessing huge surface areas and feasible chemical tunability,are emerging as critical functional materials to solve the growing challenges associated with energy-water systems,such as water scarcity issues.In this contribution,the roles of MOFs are highlighted in electrochemical-based water applications(i.e.,reactions,sensing,and separations),where MOF-based functional materials exhibit outstanding performances in detecting/removing pollutants,recovering resources,and harvesting energies from different water sources.Compared with the pristine MOFs,the efficiency and/or selectivity can be further enhanced via rational structural modulation of MOFs(e.g.,partial metal substitution)or integration of MOFs with other functional materials(e.g.,metal clusters and reduced graphene oxide).Several key factors/properties that affect the performances of MOF-based materials are also reviewed,including electronic structures,nanoconfined effects,stability,conductivity,and atomic structures.The advancement in the fundamental understanding of these key factors is expected to shed light on the functioning mechanisms of MOFs(e.g.,charge transfer pathways and guest-host interactions),which will subsequently accelerate the integration of precisely designed MOFs into electrochemical architectures to achieve highly effective water remediation with optimized selectivity and long-term stability.
基金the National Natural Science Foundation of China (Grant nos.21233004,21303147 and 21473148,etc.)the National Key Research and Development Program (Grant no.2016YFB0901500)
文摘The increased use of rechargeable batteries in portable electronic devices and the continuous develop-ment of novel applications （e.g. transportation and large scale energy storage）, have raised a strong de-mand for high performance batteries with increased energy density, cycle and calendar life, safety andlower costs. This triggers significant efforts to reveal the fundamental mechanism determining batteryperformance with the use of advanced analytical techniques. However, the inherently complex character-istics of battery systems make the mechanism analysis sophisticated and difficult. Synchrotron radiationis an advanced collimated light source with high intensity and tunable energies. It has particular ad-vantages in electronic structure and geometric structure （both the short-range and long-range structure）analysis of materials on different length and time scales. In the past decades, synchrotron X-ray tech-niques have been widely used to understand the fundamental mechanism and guide the technologicaloptimization of batteries. In particular, in situ and operando techniques with high spatial and temporalresolution, enable the nondestructive, real time dynamic investigation of the electrochemical reaction,and lead to significant deep insights into the battery operation mechanism. This review gives a brief introduction of the application of synchrotron X-ray techniques to the inves-tigation of battery systems. The five widely implicated techniques, including X-ray diffraction （XRD）, PairDistribution Function （PDF）, Hard and Soft X-ray absorption spectroscopy （XAS） and X-ray photoelectronspectroscopy （XPS） will be reviewed, with the emphasis on their in situ studies of battery systems during cycling.
基金supported by the Division of Materials Science and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy (DOE)。
文摘The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Understanding the mechanism of the structure transition and atom rearrangement via synthesis or processing is key to expediting the exploration of excellent energy materials. In this work, in situ neutron scattering is employed to reveal the real-time structure evolution, including the TM-O bonds, lattice,TM valence and the migration of the high-voltage spinel cathode LiNi_(0.5)Mn_(1.5)O_(4). The transition-metalmediated spinel destabilization under the annealing at the oxygen-deficient atmosphere is pinpointed.The formation of Mn^(3+) is correlated to the TM migration activation, TM disordered rearrangement in the spinel, and the transition to a layered-rocksalt phase. The further TM interdiffusion and Mn^(3+) reduction are also revealed with multi-stage thermodynamics and kinetics. The mechanisms of phase transition and atom migrations as functions of temperature, time and atmosphere present important guidance on the synthesis in various-valence element containing oxides.
基金The project supported by University Grants Commission, New Delhi, India
文摘A well-established pseodopotential is used to study the structure of some 4f rare earth liquid metals （Ce, Pr, Eu, Gd, Tb, and Yb）. The structure factor S（q）, pair distribution function g（r）, interatomic distance r1, and coordination number n1 are calculated using Charged Hard Sphere （CHS） reference system. To introduce the exchange and correlation effects, the local field correction due to Sarkar et al. （S） is applied. The present investigation is successful in generating the structural information of Ce, Pr, Eu, Gd, Tb, and Yb 4f rare earth liquid metals.
基金supported by the National Basic Research Program of China (Grant Nos.2007CB935400 and 2009CB623700)
文摘It has been a challenge to fully understand the structural characteristics of laser-irradiation induced amorphous(L-a) Ge2Sb2Te5(GST) alloy due to the difficulties of collecting diffraction data from high purity specimens. In this paper,by fabricating GST thin films on different substrates,we exhibit an effective way of preparing L-a GST dots in submicron scale on various types of specially designed transmission electron microscope(TEM) grids. The structural characteristics of L-a GST in the form of pair distribution functions(PDF) can be achieved on single dots of L-a GST via selected area electron diffraction(SAED) . This general approach would be convenient for precisely producing laser-irradiation induced materials in submicron scale for structural investigation.
