Three Epimedium species, E. pubescens Maxim., E. sagittatum (Sieb. & Zucc.) Maxim., and E. wushanense T. S. Ying, which are sympatrically distributed in the western Hubei Province, have been used in traditional Chi...Three Epimedium species, E. pubescens Maxim., E. sagittatum (Sieb. & Zucc.) Maxim., and E. wushanense T. S. Ying, which are sympatrically distributed in the western Hubei Province, have been used in traditional Chinese medicine (TCM) for about 2,000 years. Genetic variability and population genetic structure of 11 natural populations of these Epimedium species were investigated using isoelectric focusing in thin-layer polyacrylamide slab gels. Of the 22 enzyme systems prescreened, six coding for 13 loci and 45 alleles were resolved, which were used for analyzing genetic diversity and population structure at both intraspecific and interspecific levels. The results showed that: l) high levels of genetic diversity were observed in all three species (A = 2.6-3.2, P = 69.2%-84.6%, Ho= 0.274-0.377, HE= 0.282-0.369), which were higher than that of other herbaceous and aulmal-pollinated species with similar life-history characteristics; 2) there was significant deviation from Hardy-Weinberg Equilibrium, with one half of the loci showing heterozygote excess and the other homozygote excess, in all populations, suggesting the complicated breeding system of Epimedium species; 3) the low level of intraspecific and interspecific genetic differentiation (GST= 0.0246-0.0409 and 0.0495-0.1213, respectively) indicated a high level of gene flow among populations and close genetic relationship among the three species; and 4) UPGMA cluster analysis further showed that E. pubescens was more closely related to E. sagittatum than to E. wushanense, which was in good agreement with the morphological characters and the recent phylogenetic analysis of these species. On the basis of these results, it was concluded that the mixed breeding system, long-lived perennial life form, ancient evolutionary history, and seed dispersal by ants in Epimedium are responsible for the genetic variation and population structure of these species.展开更多
Creep and anelastic backflow behaviors of pure copper (4N Cu) with grain size dg=40 μm were investigated at low temperatures of T〈0.3Tm (Tm is melting point) and ultra-low creep rates of ε≤1×10^-10 s^-1 b...Creep and anelastic backflow behaviors of pure copper (4N Cu) with grain size dg=40 μm were investigated at low temperatures of T〈0.3Tm (Tm is melting point) and ultra-low creep rates of ε≤1×10^-10 s^-1 by a high strain-resolution measurement (the helicoid spring specimen technique). Analysis of creep data was based on the scaling factors of creep curves instead of the conventional extrapolated steady-state creep rate. Power-law creep equation is suggested to be the best for describing the primary transient creep behavior, because the pre-parameter does not apparently change with elapsed time. The observed anelastic strains are 1/6 of the calculated elastic strains, and linear viscous behavior was identified from the logarithm plot of the anelastic strain rate versus anelastic strain (slope equals 1). Therefore, the creep anelasticity is suggested to be due to the unbowing of there-dimensional network of dislocations.展开更多
Piezoelectric actuator has high stiffness, high frequency and infinite control precision, but a short output displacement which is often 1/1 000 of its length. In order to meet the requirements that tools feeding shou...Piezoelectric actuator has high stiffness, high frequency and infinite control precision, but a short output displacement which is often 1/1 000 of its length. In order to meet the requirements that tools feeding should be long-travel, high-frequency and high-precision in non-circular precision turning, a new one-freedom flexure hinge structure is put forward to amplify the output displacement of piezoelectric actuator. Theoretical analysis is done on the static and dynamic characteristics of the structure, differential equations are presented, and it is also verified by the finite element method. It's proved by experiments that the output displacement of the structure is 293 μm and its resonant frequency is 312 Hz.展开更多
The atomic structure of the active sites in Cu/CeO2 catalysts is intimately associated with the copper-ceria interaction. Both the shape of ceria and the loading of copper affect the chemical bonding of copper species...The atomic structure of the active sites in Cu/CeO2 catalysts is intimately associated with the copper-ceria interaction. Both the shape of ceria and the loading of copper affect the chemical bonding of copper species on ceria surfaces and the electronic and geometric character of the relevant interfaces. Nanostructured ceria, including particles(polyhedra), rods, and cubes, provides anchoring sites for the copper species. The atomic arrangements and chemical properties of the(111),(110) and(100) facets, preferentially exposed depending on the shape of ceria, govern the copper-ceria interactions and in turn determine their catalytic properties. Also, the metal loading significantly influences the dispersion of copper species on ceria with a specific shape, forming copper layers, clusters, and nanoparticles. Lower copper contents result in copper monolayers and/or bilayers while higher copper loadings lead to multi-layered clusters and faceted particles. The active sites are usually generated via interactions between the copper atoms in the metal species and the oxygen vacancies on ceria, which is closely linked to the number and density of surface oxygen vacancies dominated by the shape of ceria.展开更多
Microstructures and mechanical properties of dual-phase AlxCrMnFeCoNi (x=0.4, 0.5, 0.6, at.%) alloys were investigated. Thermomechanical processing leads to a microstructural evolution from cast dendritic structures t...Microstructures and mechanical properties of dual-phase AlxCrMnFeCoNi (x=0.4, 0.5, 0.6, at.%) alloys were investigated. Thermomechanical processing leads to a microstructural evolution from cast dendritic structures to equiaxed ones, consisting of face-centered cubic (fcc) and body-centered cubic (bcc) phases in the two states. The volume fraction of bcc phase increases and the size of fcc grain decreases with increasing Al content, resulting in remarkably improved tensile strength. Specifically, the serrated flow occurring at the medium temperatures varies from type A+B to B+C or C as the testing temperature increases. The average serration amplitude of these Al-containing alloys is larger than that of CoCrFeNiMn alloy due to the enhanced pinning effect. The early small strain produces low-density of dislocation arrays and bowed dislocations in fcc grains while the dislocation climb and shearing mechanism dominate inside bcc grains. The cross-slip and kinks of dislocations are frequently observed and high-density-tangled dislocations lead to dislocation cells after plastic deformation with a high strain.展开更多
Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated (i...Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated (i.e. V-N and Cr-C) and non-compensated (i.e. V-C and Cr-N) codoped anatase TiO2 by performing extensive density functional theory calculations. Theoretical results show that oxygen vacancy prefers to the neighboring site of metal dopant (i.e. V or Cr atom). After introduction of oxygen vacancy, the unoccupied impurity bands located within band gap of these codoped TiO2 will be filled with electrons, and the posi- tion of conduction band offset does not change obviously, which result in the reduction of photoinduced carrier recombination and the good performance for hydrogen production via water splitting. Moreover, we find that oxygen vacancy is easily introduced in V-N codoped TiO2 under O-poor condition. These theoretical insights are helpful for designing codoped TiO2 with high photoelectrochemical performance.展开更多
Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with ...Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.展开更多
The interactions between human erythrocyte spectrin(SP) and Pt(II) complexes with different composition and configuration were studied by fluorescence and circular dichroism spectra. The results showed that there are ...The interactions between human erythrocyte spectrin(SP) and Pt(II) complexes with different composition and configuration were studied by fluorescence and circular dichroism spectra. The results showed that there are 4.7×10 2 binding sites of cisplatin(CDDP) in a spectrin tetramer(SPT). Among them, about 70 sites with apparent binding constant K 1】3.47×10 6 were of highest affinity, 1.8×10 2 sites with K 2 = 3.47×10 6 were of high affinity, and other 2.2×10 2 sites with K 3 = 8.77×10 5 were of low affinity. The conformation change of spectrin, depending on the concentration of Pt(II) complex and molar ratio(R) of Pt(II) complex to spectrin, was induced by the binding of Pt(II) complexes. It indicated that the interaction of both CDDP and cis diaquodiamine platinum(DADP) with SP followed a two step first order kinetic process in the first stage (1 h), and the kinetic constants were determined. In the second stage, the induced conformation change, polymerization and depolymerization of SP were probably involved. It was noticed that in the reaction of SP and Pt(II) complexes with 1,2 cyclohexanediammine isomers as chiral carrier ligand, stereo matching played a more important role than the affinity of Pt(II) to thiol groups of SP.展开更多
MnFeCoCuNix high-entropy alloys(HEAs)with different Ni contents were fabricated by vacuum induction melting.XRD and SEM−EDS were used to analyze the phase constitution and structure,and the tensile properties of the s...MnFeCoCuNix high-entropy alloys(HEAs)with different Ni contents were fabricated by vacuum induction melting.XRD and SEM−EDS were used to analyze the phase constitution and structure,and the tensile properties of the samples were determined using a universal tensile tester.The results show that the HEAs consist of a dual-phase structure,in which FCC1 phase is rich in Fe and Co,while the FCC2 phase has high contents of Cu and Mn.As Ni content increases,the segregation of Cu decreases,accompanied by the decrease of FCC2 phase.Moreover,the tensile strength of the HEAs increases first and then decreases,and the elongation increases slightly.This is attributed to the combined effect of interface strengthening and solid solution strengthening.The in-situ stretched MnFeCoCuNi0.5 alloy shows obvious neck shrinkage during the tensile fracture process.In the initial deformation stage,the slip lines show different morphologies in the dual-phase structure.However,in the later stage,the surface slip lines become longer and denser due to the redistribution of atoms and the re-separation of the dissolved phase.展开更多
To solve the problem of variations in radio frequency characteristics among different devices,transfer learning is applied to transform device diversity to domain adaptation in the indoor localization algorithm.A robu...To solve the problem of variations in radio frequency characteristics among different devices,transfer learning is applied to transform device diversity to domain adaptation in the indoor localization algorithm.A robust indoor localization algorithm based on the aligned fingerprints and ensemble learning called correlation alignment for localization(CALoc)is proposed with low computational complexity.The second-order statistical properties of fingerprints in the offline and online phase are needed to be aligned.The real-time online calibration method mitigates the impact of device heterogeneity largely.Without any time-consuming deep learning retraining process,CALoc online only needs 0.11 s.The effectiveness and efficiency of CALoc are verified by realistic experiments.The results show that compared to the traditional algorithms,a significant performance gain is achieved and that it achieves better positioning accuracy with a 19%improvement.展开更多
The title compound, C30H18O2P2, is a chiral biphospbine ligand. Itscrystal structure was determined by X-ray diffraction analysis. The crystal is or-thorhombic I space group, P212121 1 greement factor for 2326 indepen...The title compound, C30H18O2P2, is a chiral biphospbine ligand. Itscrystal structure was determined by X-ray diffraction analysis. The crystal is or-thorhombic I space group, P212121 1 greement factor for 2326 independent reflections with (I)- In the molecu1e, two diphenylphosphino groups are in the same side of two rigidtetrahydrofuran rings and point out from each other resulting in the non-chelate charac-ter of this bidentate ligand, the title compound.展开更多
We consider a statically determinate structural truss problem where all of the physical model parameters are uncertain: not just the material values and applied loads, but also the positions of the nodes are assumed ...We consider a statically determinate structural truss problem where all of the physical model parameters are uncertain: not just the material values and applied loads, but also the positions of the nodes are assumed to be inexact but bounded and are represented by intervals. Such uncertainty may typically arise from imprecision during the process of manufacturing or construction, or round-off errors. In this case the application of the finite element method results in a system of linear equations with numerous interval parameters which cannot be solved conventionally. Applying a suitable variable substitution, an iteration method for the solution of a parametric system of linear equations is firstly employed to obtain initial bounds on the node displacements. Thereafter, an interval tightening (pruning) technique is applied, firstly on the element forces and secondly on the node displacements, in order to obtain tight guaranteed enclosures for the interval solutions for the forces and displacements.展开更多
The hydro(solvo)thermal reactions of cobalt powder or its chloride with 2,5- pyridine dicarboxylic acid (H2PYDC) yielded two new complexes: [Co(II)2(PYDC)2(H2O)2- (H2O)4]n 1 and {Co(II)[NH2(CH3)2]2(PYDC)2}n 2. It is o...The hydro(solvo)thermal reactions of cobalt powder or its chloride with 2,5- pyridine dicarboxylic acid (H2PYDC) yielded two new complexes: [Co(II)2(PYDC)2(H2O)2- (H2O)4]n 1 and {Co(II)[NH2(CH3)2]2(PYDC)2}n 2. It is observed that the reactive solvents result in different connectivity modes of ligand and diverse dimensional extension of crystal structures. The correlation between structure and magnetic property will be discussed in this paper. Crystal data for 1: space group P1, a = 7.0419(17), b = 8.937(2), c = 9.6182(19) ?, α = 91.532(4), β = 99.869(10), γ = 107.889(11)o, V = 565.5(2) ?3, Z = 1, Dc = 1.845 g/cm3, μ = 1.56 mm-1, F(000) = 322 , R = 0.0505 and wR = 0.1580; and those for 2: space group C2/c, a = 14.9075(6), b = 8.2523(3), c = 16.9643(2) ?, β = 100.982(2)o, V = 2048.75(11) ?3, Z = 4, Dc = 1.560 g/cm3, μ = 0.892 mm-1, F(000) = 996, R = 0.0443 and wR = 0.1134.展开更多
Electrochemical water splitting is regarded as the most promising approach to produce hydrogen.However,the sluggish electrochemical reactions occurring at the anode and cathode,namely,the oxygen evolution reaction(OER...Electrochemical water splitting is regarded as the most promising approach to produce hydrogen.However,the sluggish electrochemical reactions occurring at the anode and cathode,namely,the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),respectively,consume a tremendous amount of energy,seriously hampering its wide application.Recently,single-atom catalysts(SACs)have been proposed to effectively enhance the kinetics of these two reactions.In this minireview,we focus on the recent progress in SACs for OER and HER applications.Three classes of SACs have been reviewed,i.e.,alloy-based SACs,carbon-based SACs and SACs supported on other compounds.Different factors affecting the activities of SACs are also highlighted,including the inherent element property,the coordination environment,the geometric structure and the loading amount of metal atoms.Finally,we summarize the current problems and directions for future development in SACs.展开更多
Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic r...Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon dioxide.This review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external perspectives.The structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement catalysis.We expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.展开更多
A special form of the Stewart platform is presented in which the top platform and base platform are similar and corresponding vertices are connected by six prismatic joints.A closed-from solution for the forward displ...A special form of the Stewart platform is presented in which the top platform and base platform are similar and corresponding vertices are connected by six prismatic joints.A closed-from solution for the forward displacement analysis of this mechanism is developed.When the six vertices of the top platform are in a quadratic curve,this mechanism becomes singular.This new theoretical result is confirmed with a numerical example.展开更多
Cobalt‐based materials have been considered as promising candidates to electrocatalyze water oxidation.However,the structure‐performance correlation remains largely elusive,due to the com‐plex material structures a...Cobalt‐based materials have been considered as promising candidates to electrocatalyze water oxidation.However,the structure‐performance correlation remains largely elusive,due to the com‐plex material structures and diverse performance‐influencing factors in those Co‐based catalysts.In this work,we designed two cobalt phosphates with distinct Co symmetry to explore the effect of coordination symmetry on electrocatalytic water oxidation.The two analogues have similar mor‐phology,Co valence and 6‐coordinated Co octahedron,but with different coordination symmetry.In contrast to symmetric Co_(3)(PO_(4))2·8H_(2)O,asymmetric NH_(4)CoPO_(4)·H_(2)O exhibited enhanced electrocata‐lytic water oxidation activity in a neutral aqueous solution.It is proven that,by experimental and theoretical studies,the asymmetric Co coordination sites can facilitate the surface reconstruction under anodic polarization to boost the electrocatalysis.Based on this contrastive platform with distinct symmetry differences,the preferred configuration in cobalt‐oxygen octahedrons for water oxidation has been straightforwardly assigned.展开更多
Properties of the chair doublet bands of the odd-odd Cs isotopes built on the πh11/2× vh11/2 configuration are investigated systematically within the supersymmetry scheme including many-body interactions and pos...Properties of the chair doublet bands of the odd-odd Cs isotopes built on the πh11/2× vh11/2 configuration are investigated systematically within the supersymmetry scheme including many-body interactions and possessing the SO(5)(or SU(5)) symmetry on the rotational symmetry. Quantitatively good results of the energy spectra, the energy staggering parameter as a function of the spin are obtained. The calculation shows that the stronger competition between the pairing and anti-pairing effects and the SU(3) symmetry broking more seriously exist in the stable chiral structure.展开更多
基金This work was supported by the National Natural Science Foundation of China (No. 30570171), 100 Talents Program of Chinese Academy of Sciences (No. 05045112), and Wuhan Chenguang Project (No. 20055003059-45).
文摘Three Epimedium species, E. pubescens Maxim., E. sagittatum (Sieb. & Zucc.) Maxim., and E. wushanense T. S. Ying, which are sympatrically distributed in the western Hubei Province, have been used in traditional Chinese medicine (TCM) for about 2,000 years. Genetic variability and population genetic structure of 11 natural populations of these Epimedium species were investigated using isoelectric focusing in thin-layer polyacrylamide slab gels. Of the 22 enzyme systems prescreened, six coding for 13 loci and 45 alleles were resolved, which were used for analyzing genetic diversity and population structure at both intraspecific and interspecific levels. The results showed that: l) high levels of genetic diversity were observed in all three species (A = 2.6-3.2, P = 69.2%-84.6%, Ho= 0.274-0.377, HE= 0.282-0.369), which were higher than that of other herbaceous and aulmal-pollinated species with similar life-history characteristics; 2) there was significant deviation from Hardy-Weinberg Equilibrium, with one half of the loci showing heterozygote excess and the other homozygote excess, in all populations, suggesting the complicated breeding system of Epimedium species; 3) the low level of intraspecific and interspecific genetic differentiation (GST= 0.0246-0.0409 and 0.0495-0.1213, respectively) indicated a high level of gene flow among populations and close genetic relationship among the three species; and 4) UPGMA cluster analysis further showed that E. pubescens was more closely related to E. sagittatum than to E. wushanense, which was in good agreement with the morphological characters and the recent phylogenetic analysis of these species. On the basis of these results, it was concluded that the mixed breeding system, long-lived perennial life form, ancient evolutionary history, and seed dispersal by ants in Epimedium are responsible for the genetic variation and population structure of these species.
基金Project(12JCYBJC32100)supported by the Tianjin Research Program of Application Foundation and Advanced Technology,ChinaProject([2013]693)supported by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry,China
文摘Creep and anelastic backflow behaviors of pure copper (4N Cu) with grain size dg=40 μm were investigated at low temperatures of T〈0.3Tm (Tm is melting point) and ultra-low creep rates of ε≤1×10^-10 s^-1 by a high strain-resolution measurement (the helicoid spring specimen technique). Analysis of creep data was based on the scaling factors of creep curves instead of the conventional extrapolated steady-state creep rate. Power-law creep equation is suggested to be the best for describing the primary transient creep behavior, because the pre-parameter does not apparently change with elapsed time. The observed anelastic strains are 1/6 of the calculated elastic strains, and linear viscous behavior was identified from the logarithm plot of the anelastic strain rate versus anelastic strain (slope equals 1). Therefore, the creep anelasticity is suggested to be due to the unbowing of there-dimensional network of dislocations.
文摘Piezoelectric actuator has high stiffness, high frequency and infinite control precision, but a short output displacement which is often 1/1 000 of its length. In order to meet the requirements that tools feeding should be long-travel, high-frequency and high-precision in non-circular precision turning, a new one-freedom flexure hinge structure is put forward to amplify the output displacement of piezoelectric actuator. Theoretical analysis is done on the static and dynamic characteristics of the structure, differential equations are presented, and it is also verified by the finite element method. It's proved by experiments that the output displacement of the structure is 293 μm and its resonant frequency is 312 Hz.
文摘The atomic structure of the active sites in Cu/CeO2 catalysts is intimately associated with the copper-ceria interaction. Both the shape of ceria and the loading of copper affect the chemical bonding of copper species on ceria surfaces and the electronic and geometric character of the relevant interfaces. Nanostructured ceria, including particles(polyhedra), rods, and cubes, provides anchoring sites for the copper species. The atomic arrangements and chemical properties of the(111),(110) and(100) facets, preferentially exposed depending on the shape of ceria, govern the copper-ceria interactions and in turn determine their catalytic properties. Also, the metal loading significantly influences the dispersion of copper species on ceria with a specific shape, forming copper layers, clusters, and nanoparticles. Lower copper contents result in copper monolayers and/or bilayers while higher copper loadings lead to multi-layered clusters and faceted particles. The active sites are usually generated via interactions between the copper atoms in the metal species and the oxygen vacancies on ceria, which is closely linked to the number and density of surface oxygen vacancies dominated by the shape of ceria.
基金Project(11572306)supported by the National Natural Science Foundation of ChinaProject(WK2090050040)supported by the Fundamental Research Funds for Central Universities,China
文摘Microstructures and mechanical properties of dual-phase AlxCrMnFeCoNi (x=0.4, 0.5, 0.6, at.%) alloys were investigated. Thermomechanical processing leads to a microstructural evolution from cast dendritic structures to equiaxed ones, consisting of face-centered cubic (fcc) and body-centered cubic (bcc) phases in the two states. The volume fraction of bcc phase increases and the size of fcc grain decreases with increasing Al content, resulting in remarkably improved tensile strength. Specifically, the serrated flow occurring at the medium temperatures varies from type A+B to B+C or C as the testing temperature increases. The average serration amplitude of these Al-containing alloys is larger than that of CoCrFeNiMn alloy due to the enhanced pinning effect. The early small strain produces low-density of dislocation arrays and bowed dislocations in fcc grains while the dislocation climb and shearing mechanism dominate inside bcc grains. The cross-slip and kinks of dislocations are frequently observed and high-density-tangled dislocations lead to dislocation cells after plastic deformation with a high strain.
基金This work was supported by the National Natural Sci- ence Foundation of China (No.11034006, No.21273208, and No.21473168), the Anhui Provincial Natural Sci- ence Foundation (No.1408085QB26), the hmdamental Research Funds for the Central Universities, the China Postdoctoral Science Foundation (No.2012M511409), and the Supercomputing Center of Chinese Academy of Sciences, Shanghai and USTC Supercomputer Cen- ters.
文摘Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated (i.e. V-N and Cr-C) and non-compensated (i.e. V-C and Cr-N) codoped anatase TiO2 by performing extensive density functional theory calculations. Theoretical results show that oxygen vacancy prefers to the neighboring site of metal dopant (i.e. V or Cr atom). After introduction of oxygen vacancy, the unoccupied impurity bands located within band gap of these codoped TiO2 will be filled with electrons, and the posi- tion of conduction band offset does not change obviously, which result in the reduction of photoinduced carrier recombination and the good performance for hydrogen production via water splitting. Moreover, we find that oxygen vacancy is easily introduced in V-N codoped TiO2 under O-poor condition. These theoretical insights are helpful for designing codoped TiO2 with high photoelectrochemical performance.
文摘Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.
文摘The interactions between human erythrocyte spectrin(SP) and Pt(II) complexes with different composition and configuration were studied by fluorescence and circular dichroism spectra. The results showed that there are 4.7×10 2 binding sites of cisplatin(CDDP) in a spectrin tetramer(SPT). Among them, about 70 sites with apparent binding constant K 1】3.47×10 6 were of highest affinity, 1.8×10 2 sites with K 2 = 3.47×10 6 were of high affinity, and other 2.2×10 2 sites with K 3 = 8.77×10 5 were of low affinity. The conformation change of spectrin, depending on the concentration of Pt(II) complex and molar ratio(R) of Pt(II) complex to spectrin, was induced by the binding of Pt(II) complexes. It indicated that the interaction of both CDDP and cis diaquodiamine platinum(DADP) with SP followed a two step first order kinetic process in the first stage (1 h), and the kinetic constants were determined. In the second stage, the induced conformation change, polymerization and depolymerization of SP were probably involved. It was noticed that in the reaction of SP and Pt(II) complexes with 1,2 cyclohexanediammine isomers as chiral carrier ligand, stereo matching played a more important role than the affinity of Pt(II) to thiol groups of SP.
基金The authors are grateful for the financial supports from the Jiangsu Provincial Science and Technology Plan Project,China(BE2018753/KJ185629)the National Natural Science Foundation of China(51571118)the 2020 Extracurricular Academic Research Fund for College Students of Nanjing University of Science and Technology,China.Zong-han XIE acknowledges the support of the Australian Research Council Discovery Projects.
文摘MnFeCoCuNix high-entropy alloys(HEAs)with different Ni contents were fabricated by vacuum induction melting.XRD and SEM−EDS were used to analyze the phase constitution and structure,and the tensile properties of the samples were determined using a universal tensile tester.The results show that the HEAs consist of a dual-phase structure,in which FCC1 phase is rich in Fe and Co,while the FCC2 phase has high contents of Cu and Mn.As Ni content increases,the segregation of Cu decreases,accompanied by the decrease of FCC2 phase.Moreover,the tensile strength of the HEAs increases first and then decreases,and the elongation increases slightly.This is attributed to the combined effect of interface strengthening and solid solution strengthening.The in-situ stretched MnFeCoCuNi0.5 alloy shows obvious neck shrinkage during the tensile fracture process.In the initial deformation stage,the slip lines show different morphologies in the dual-phase structure.However,in the later stage,the surface slip lines become longer and denser due to the redistribution of atoms and the re-separation of the dissolved phase.
基金The National Key Research and Development Program of China(No.2018YFB1802400)the National Natural Science Foundation of China(No.61571123)the Research Fund of National M obile Communications Research Laboratory,Southeast University(No.2020A03)
文摘To solve the problem of variations in radio frequency characteristics among different devices,transfer learning is applied to transform device diversity to domain adaptation in the indoor localization algorithm.A robust indoor localization algorithm based on the aligned fingerprints and ensemble learning called correlation alignment for localization(CALoc)is proposed with low computational complexity.The second-order statistical properties of fingerprints in the offline and online phase are needed to be aligned.The real-time online calibration method mitigates the impact of device heterogeneity largely.Without any time-consuming deep learning retraining process,CALoc online only needs 0.11 s.The effectiveness and efficiency of CALoc are verified by realistic experiments.The results show that compared to the traditional algorithms,a significant performance gain is achieved and that it achieves better positioning accuracy with a 19%improvement.
文摘The title compound, C30H18O2P2, is a chiral biphospbine ligand. Itscrystal structure was determined by X-ray diffraction analysis. The crystal is or-thorhombic I space group, P212121 1 greement factor for 2326 independent reflections with (I)- In the molecu1e, two diphenylphosphino groups are in the same side of two rigidtetrahydrofuran rings and point out from each other resulting in the non-chelate charac-ter of this bidentate ligand, the title compound.
文摘We consider a statically determinate structural truss problem where all of the physical model parameters are uncertain: not just the material values and applied loads, but also the positions of the nodes are assumed to be inexact but bounded and are represented by intervals. Such uncertainty may typically arise from imprecision during the process of manufacturing or construction, or round-off errors. In this case the application of the finite element method results in a system of linear equations with numerous interval parameters which cannot be solved conventionally. Applying a suitable variable substitution, an iteration method for the solution of a parametric system of linear equations is firstly employed to obtain initial bounds on the node displacements. Thereafter, an interval tightening (pruning) technique is applied, firstly on the element forces and secondly on the node displacements, in order to obtain tight guaranteed enclosures for the interval solutions for the forces and displacements.
基金Financially support by NNSFC (No. 20031020) NSF of Fujian Province and the Key Project from CAS
文摘The hydro(solvo)thermal reactions of cobalt powder or its chloride with 2,5- pyridine dicarboxylic acid (H2PYDC) yielded two new complexes: [Co(II)2(PYDC)2(H2O)2- (H2O)4]n 1 and {Co(II)[NH2(CH3)2]2(PYDC)2}n 2. It is observed that the reactive solvents result in different connectivity modes of ligand and diverse dimensional extension of crystal structures. The correlation between structure and magnetic property will be discussed in this paper. Crystal data for 1: space group P1, a = 7.0419(17), b = 8.937(2), c = 9.6182(19) ?, α = 91.532(4), β = 99.869(10), γ = 107.889(11)o, V = 565.5(2) ?3, Z = 1, Dc = 1.845 g/cm3, μ = 1.56 mm-1, F(000) = 322 , R = 0.0505 and wR = 0.1580; and those for 2: space group C2/c, a = 14.9075(6), b = 8.2523(3), c = 16.9643(2) ?, β = 100.982(2)o, V = 2048.75(11) ?3, Z = 4, Dc = 1.560 g/cm3, μ = 0.892 mm-1, F(000) = 996, R = 0.0443 and wR = 0.1134.
文摘Electrochemical water splitting is regarded as the most promising approach to produce hydrogen.However,the sluggish electrochemical reactions occurring at the anode and cathode,namely,the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),respectively,consume a tremendous amount of energy,seriously hampering its wide application.Recently,single-atom catalysts(SACs)have been proposed to effectively enhance the kinetics of these two reactions.In this minireview,we focus on the recent progress in SACs for OER and HER applications.Three classes of SACs have been reviewed,i.e.,alloy-based SACs,carbon-based SACs and SACs supported on other compounds.Different factors affecting the activities of SACs are also highlighted,including the inherent element property,the coordination environment,the geometric structure and the loading amount of metal atoms.Finally,we summarize the current problems and directions for future development in SACs.
文摘Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon dioxide.This review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external perspectives.The structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement catalysis.We expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.
文摘A special form of the Stewart platform is presented in which the top platform and base platform are similar and corresponding vertices are connected by six prismatic joints.A closed-from solution for the forward displacement analysis of this mechanism is developed.When the six vertices of the top platform are in a quadratic curve,this mechanism becomes singular.This new theoretical result is confirmed with a numerical example.
文摘Cobalt‐based materials have been considered as promising candidates to electrocatalyze water oxidation.However,the structure‐performance correlation remains largely elusive,due to the com‐plex material structures and diverse performance‐influencing factors in those Co‐based catalysts.In this work,we designed two cobalt phosphates with distinct Co symmetry to explore the effect of coordination symmetry on electrocatalytic water oxidation.The two analogues have similar mor‐phology,Co valence and 6‐coordinated Co octahedron,but with different coordination symmetry.In contrast to symmetric Co_(3)(PO_(4))2·8H_(2)O,asymmetric NH_(4)CoPO_(4)·H_(2)O exhibited enhanced electrocata‐lytic water oxidation activity in a neutral aqueous solution.It is proven that,by experimental and theoretical studies,the asymmetric Co coordination sites can facilitate the surface reconstruction under anodic polarization to boost the electrocatalysis.Based on this contrastive platform with distinct symmetry differences,the preferred configuration in cobalt‐oxygen octahedrons for water oxidation has been straightforwardly assigned.
基金Supported by the National Natural Science Foundation of China under Grant No.10475026the Natural Science Foundation of Zhejiang Province under Grant No.KY607518
文摘Properties of the chair doublet bands of the odd-odd Cs isotopes built on the πh11/2× vh11/2 configuration are investigated systematically within the supersymmetry scheme including many-body interactions and possessing the SO(5)(or SU(5)) symmetry on the rotational symmetry. Quantitatively good results of the energy spectra, the energy staggering parameter as a function of the spin are obtained. The calculation shows that the stronger competition between the pairing and anti-pairing effects and the SU(3) symmetry broking more seriously exist in the stable chiral structure.