In this paper we first deduce the estimates on the linearized Landau operator with Coulomb potential and then analyze its spectrum structure by using semigroup theory and linear operator perturbation theory.Based on t...In this paper we first deduce the estimates on the linearized Landau operator with Coulomb potential and then analyze its spectrum structure by using semigroup theory and linear operator perturbation theory.Based on these estimates,we give the precise time decay rate estimates on the semigroup generated by the linearized Landau operator so that the optimal time decay rates of the nonlinear Landau equation follow.In addition,we present a similar result for the non-angular cutoff Boltzmann equation with soft potentials.展开更多
Based on the statistical characteristics of remote sensing data, the spatial geometric structure characteristics of spectral data and distribution of background, interference and alteration information in characterist...Based on the statistical characteristics of remote sensing data, the spatial geometric structure characteristics of spectral data and distribution of background, interference and alteration information in characteristic space were researched through the analysis of two-dimensional and three-dimensional scatter diagrams. The results indicate that the hyper-space of remote sensing multi-data aggregation belongs to low-dimensional geometric structure, i.e. hyperplane form, and anomalous point groups including alteration information usually dissociate out of hyperplane. Scatter diagrams of remote sensing data band are mainly presented as two distribution forms of single-ellipse and dual-ellipse. Clarifying the relations of three objects of background, disturbance and alteration information in remote sensing images provides an important technical thought and guidance for accurately detecting and extracting remote sensing alteration information.展开更多
It was revealed that an average energy of special boundaries is proportional to APB energy in the alloys with the L12 superstructure. This fact proves the appearance of the GAPBs in the planes of location of special b...It was revealed that an average energy of special boundaries is proportional to APB energy in the alloys with the L12 superstructure. This fact proves the appearance of the GAPBs in the planes of location of special boundaries in coincidence sites of ordered alloys. It was determined that the more energy of special boundaries in ordered alloys, the more energy of complex stacking fault. There is a correlation between the distribution of special boundaries as a function its relative energy and ordering energy: the more ordering energy, the more degree of washed away of distribution. The correlation between average relative energy of special boundaries and ordering energy was detected: the more ordering energy, the more average energy of special boundaries. The reverse dependence between ordering energy and average number of special boundaries in grains limited by boundaries of general type was discovered.展开更多
The femtosecond pulse shaping technique has been shown to be an effective method to control the multi-photon absorption by the light–matter interaction. Previous studies mainly focused on the quantum coherent control...The femtosecond pulse shaping technique has been shown to be an effective method to control the multi-photon absorption by the light–matter interaction. Previous studies mainly focused on the quantum coherent control of the multi-photon absorption by the phase, amplitude and polarization modulation, but the coherent features of the multi-photon absorption depending on the energy level structure, the laser spectrum bandwidth and laser central frequency still lack in-depth systematic research. In this work, we further explore the coherent features of the resonance-mediated two-photon absorption in a rubidium atom by varying the energy level structure, spectrum bandwidth and central frequency of the femtosecond laser field. The theoretical results show that the change of the intermediate state detuning can effectively influence the enhancement of the near-resonant part, which further affects the transform-limited (TL)-normalized final state population maximum. Moreover, as the laser spectrum bandwidth increases, the TL-normalized final state population maximum can be effectively enhanced due to the increase of the enhancement in the near-resonant part, but the TL-normalized final state population maximum is constant by varying the laser central frequency. These studies can provide a clear physical picture for understanding the coherent features of the resonance-mediated two-photon absorption, and can also provide a theoretical guidance for the future applications.展开更多
Ammonium 5-sulfosalicylic acid monohydrate (NH4·C7H5O6S·H2O, ASSA) was synthesized and optical grade crystal with dimensions of 45ram × 20mm × 18mm was obtained from aqueous solution by the cooli...Ammonium 5-sulfosalicylic acid monohydrate (NH4·C7H5O6S·H2O, ASSA) was synthesized and optical grade crystal with dimensions of 45ram × 20mm × 18mm was obtained from aqueous solution by the cooling solution method. The crystal structure was confirmed by X-ray single-crystal diffraction method and the empirical composition is C7HIINO7S with formula weight 253.23. The crystal belongs to monoclinic space group P21/c with a = 1 1.884(9), b = 7.306(5), c = 12.152(9) A, β = 104.851(13)°, V= 1019.8(13) A3, Z = 4, Dc = 1.649 g/cm3,μ = 0.340 mm-1, F(000) =528, the final R= 0.0307 and wR= 0.0866 for 7494 observed reflections (I〉 2σ(I)), Elemental analysis, 1R and 1H-NMR spectrum were used to characterize the compound. Thermal analysis showed that one coordination water molecule was contained and dehydration temperature of ASSA crystal was 106℃. Optical transmission and fluorescence spectrum revealed that the ASSA crystal exhibited a strong absorption in ultraviolet region with the sharp absorption edge located at 340 nm and a significant blue fluorescent emission band at 442 nm.展开更多
The pointwise space-time behaviors of the Green’s function and the global solution to the Vlasov-Poisson-Fokker-Planck(VPFP)system in three dimensional space are studied in this paper.It is shown that the Green’s fu...The pointwise space-time behaviors of the Green’s function and the global solution to the Vlasov-Poisson-Fokker-Planck(VPFP)system in three dimensional space are studied in this paper.It is shown that the Green’s function consists of the diffusion waves decaying exponentially in time but algebraically in space,and the singular kinetic waves which become smooth for all(t,x,v)when t>0.Furthermore,we establish the pointwise space-time behaviors of the global solution to the nonlinear VPFP system when the initial data is not necessarily smooth in terms of the Green’s function.展开更多
This paper deals with the structure of the spectrum of infinite dimensional Hamiltonian operators.It is shown that the spectrum,the union of the point spectrum and residual spectrum,and the continuous spectrum are all...This paper deals with the structure of the spectrum of infinite dimensional Hamiltonian operators.It is shown that the spectrum,the union of the point spectrum and residual spectrum,and the continuous spectrum are all symmetric with respect to the imaginary axis of the complex plane. Moreover,it is proved that the residual spectrum does not contain any pair of points symmetric with respect to the imaginary axis;and a complete characterization of the residual spectrum in terms of the point spectrum is then given.As applications of these structure results,we obtain several necessary and sufficient conditions for the residual spectrum of a class of infinite dimensional Hamiltonian operators to be empty.展开更多
Recent studies have demonstrated the application of vegetation indices from canopy reflectedspectrum for inversion of chlorophyll concentration. Some indices are both response tovariations of vegetation and environmen...Recent studies have demonstrated the application of vegetation indices from canopy reflectedspectrum for inversion of chlorophyll concentration. Some indices are both response tovariations of vegetation and environmental factors. Canopy chlorophyll concentration, anindicator of photosynthesis activity, is related to nitrogen concentration in green vegetationand serves as an indicator of the crop response to soil nitrogen fertilizer application. Thecombination of normalized difference vegetation index (NDVI) and photochemical reflectanceindex (PRI) can reduce the effect of leaf area index (LAI) and soil background. The canopychlorophyll inversion index (CCII) was proved to be sensitive to chlorophyll concentration andvery resistant to the other variations. This paper introduced the ratio of TCARI/OSAVI to makeaccurate predictions of winter wheat chlorophyll concentration under different cultivars. Itindicated that canopy chlorophyll concentration could be evaluated by some combined vegetationindices.展开更多
A new boroantimonate K2SbB3O8 has been synthesized by high-temperature solidstate reactions, and its crystals have been obtained by the flux method. The crystal structure has been determined from single-crystal X-ray ...A new boroantimonate K2SbB3O8 has been synthesized by high-temperature solidstate reactions, and its crystals have been obtained by the flux method. The crystal structure has been determined from single-crystal X-ray diffraction analysis. The compound crystallizes in the monoclinic space group P21/c with a = 5.8890(2), b = 11.0512(4), c = 10.8951(4)A, β =103.200(4)°, V = 690.32(4) A^3, Z = 4, F(000) = 672, ρc = 3.467 g/cm^3, Mr = 360.38 and μ = 5.215mm^-1. Its structure feature is a three-dimensional framework composed of SbO6 octahedra and isolated [B3O8]^7- groups with K+ cations residing in the one-dimensional tunnels along the a-axis.Interestingly, the isolated [B3O8]^7- groups are distinct from the known [B3O8]^7- groups, which always connect to each other. The UV-vis-NIR absorption, thermal stability and infrared spectrum are also discussed in this paper.展开更多
The electron paramagnetic resonance(EPR) spectra of trigonal Mn^(2+) centers in Zn(ClO4)2·6(H2O) and Mg(ClO4)2·6(H2O) crystals were studied on the basis of the complete energy matrices for a d^5...The electron paramagnetic resonance(EPR) spectra of trigonal Mn^(2+) centers in Zn(ClO4)2·6(H2O) and Mg(ClO4)2·6(H2O) crystals were studied on the basis of the complete energy matrices for a d^5 configuration ion in a trigonal ligand field. It was demonstrated that the local lattice structure around a trigonal Mn^(2+) center has an compressed distortion along the crystalline c3 axis, and when Mn^(2+) is doped in the Zn(ClO4)2·6(H2O) and Mg(ClO4)2·6(H2O) crystals, there is a similar local distortion. From the EPR calculation, the local lattice structure parameters R=2.183 2 ?, for Zn(ClO4)2·6(H2O), R=2.130 2 ?, for Mg(ClO4)2·6(H2O) have been determined.展开更多
In this paper a series of ab initio SCF and configuration calculations were reported for the ground state and excited states X^2E, A^2E,~2B_2 and ~2A_1 of allene.For ground state X^2E Jahn- Teller distorsion was discu...In this paper a series of ab initio SCF and configuration calculations were reported for the ground state and excited states X^2E, A^2E,~2B_2 and ~2A_1 of allene.For ground state X^2E Jahn- Teller distorsion was discussed and a twisted angle of 50° and a torsional barriers of 0.21—0.51 eV were derived.Based on calculated results,the experimental photoelectron spectrum of allene has been assigned.展开更多
CH_3CCo_3(CO)_9 was synthesized from the reaction between chloralose and Co_2(CO)_. The radical anion was generated by electrochemical reduction,and electron spin resonance spectra in THF were recorded by in situ elec...CH_3CCo_3(CO)_9 was synthesized from the reaction between chloralose and Co_2(CO)_. The radical anion was generated by electrochemical reduction,and electron spin resonance spectra in THF were recorded by in situ electrolysis in the sample tube in the ESR cavity at 298 and 110K with the spectral data展开更多
Searching for effective biomarkers is one of the most challenging tasks in the research ?eld of Autism Spectrum Disorder(ASD). Magnetic resonance imaging(MRI) provides a non-invasive and powerful tool for investi...Searching for effective biomarkers is one of the most challenging tasks in the research ?eld of Autism Spectrum Disorder(ASD). Magnetic resonance imaging(MRI) provides a non-invasive and powerful tool for investigating changes in the structure, function, maturation,connectivity, and metabolism of the brain of children with ASD. Here, we review the more recent MRI studies in young children with ASD, aiming to provide candidate biomarkers for the diagnosis of childhood ASD. The review covers structural imaging methods, diffusion tensor imaging, resting-state functional MRI, and magnetic resonance spectroscopy. Future advances in neuroimaging techniques, as well as cross-disciplinary studies and largescale collaborations will be needed for an integrated approach linking neuroimaging, genetics, and phenotypic data to allow the discovery of new, effective biomarkers.展开更多
Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as ...Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).展开更多
The elastic, dynamical, and electronic properties of cubic LiHg and Li3Hg were investigated based on first-principles methods. The elastic constants and phonon spectral calculations confirmed the mechanical and dynami...The elastic, dynamical, and electronic properties of cubic LiHg and Li3Hg were investigated based on first-principles methods. The elastic constants and phonon spectral calculations confirmed the mechanical and dynamical stability of the materials at ambient conditions. The obtained elastic moduli of LiHg are slightly larger than those of Li3Hg. Both LiHg and Li3Hg are ductile materials with strong shear anisotropy as metals with mixed ionic, covalent, and metallic interactions. The calculated Debye temperatures are 223.5 K and 230.6 K for LiHg and Li3Hg, respectively. The calculated phonon frequency of the T2g mode in Li3Hg is 326.8 cm-1. The p states from the Hg and Li atoms dominate the electronic structure near the Fermi level. These findings may inspire further experimental and theoretical study on the potential technical and engineering applications of similar alkali metal-based intermetallic compounds.展开更多
基金supported by the Research Grants Council of the Hong Kong Special Administrative Region of the People’s Republic of China (Grant No.SRF2021-1S01)National Natural Science Foundation of China (Grant No.11971200)+1 种基金supported by National Natural Science Foundation of China (Grant No.11871229)the Project Supported by Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2017。
文摘In this paper we first deduce the estimates on the linearized Landau operator with Coulomb potential and then analyze its spectrum structure by using semigroup theory and linear operator perturbation theory.Based on these estimates,we give the precise time decay rate estimates on the semigroup generated by the linearized Landau operator so that the optimal time decay rates of the nonlinear Landau equation follow.In addition,we present a similar result for the non-angular cutoff Boltzmann equation with soft potentials.
基金Project(2006BAB01A06) supported by the National Science and Technology Pillar Program Project during the 11th Five-Year Plan PeriodProject(1212010761503) supported by Land and Resources Investigation Project
文摘Based on the statistical characteristics of remote sensing data, the spatial geometric structure characteristics of spectral data and distribution of background, interference and alteration information in characteristic space were researched through the analysis of two-dimensional and three-dimensional scatter diagrams. The results indicate that the hyper-space of remote sensing multi-data aggregation belongs to low-dimensional geometric structure, i.e. hyperplane form, and anomalous point groups including alteration information usually dissociate out of hyperplane. Scatter diagrams of remote sensing data band are mainly presented as two distribution forms of single-ellipse and dual-ellipse. Clarifying the relations of three objects of background, disturbance and alteration information in remote sensing images provides an important technical thought and guidance for accurately detecting and extracting remote sensing alteration information.
基金B.V.Konovalova., N.A. Koneva and E.V.Kozlov acknowledge the INTAS for the partial support of this research under INTAS97-319
文摘It was revealed that an average energy of special boundaries is proportional to APB energy in the alloys with the L12 superstructure. This fact proves the appearance of the GAPBs in the planes of location of special boundaries in coincidence sites of ordered alloys. It was determined that the more energy of special boundaries in ordered alloys, the more energy of complex stacking fault. There is a correlation between the distribution of special boundaries as a function its relative energy and ordering energy: the more ordering energy, the more degree of washed away of distribution. The correlation between average relative energy of special boundaries and ordering energy was detected: the more ordering energy, the more average energy of special boundaries. The reverse dependence between ordering energy and average number of special boundaries in grains limited by boundaries of general type was discovered.
基金Supported by the National Natural Science Foundation of China under Grant Nos 51132004,11474096 and 11604199the Science and Technology Commission of Shanghai Municipality under Grant No 14JC1401500the Higher Education Key Program of He'nan Province under Grant Nos 17A140025 and 16A140030
文摘The femtosecond pulse shaping technique has been shown to be an effective method to control the multi-photon absorption by the light–matter interaction. Previous studies mainly focused on the quantum coherent control of the multi-photon absorption by the phase, amplitude and polarization modulation, but the coherent features of the multi-photon absorption depending on the energy level structure, the laser spectrum bandwidth and laser central frequency still lack in-depth systematic research. In this work, we further explore the coherent features of the resonance-mediated two-photon absorption in a rubidium atom by varying the energy level structure, spectrum bandwidth and central frequency of the femtosecond laser field. The theoretical results show that the change of the intermediate state detuning can effectively influence the enhancement of the near-resonant part, which further affects the transform-limited (TL)-normalized final state population maximum. Moreover, as the laser spectrum bandwidth increases, the TL-normalized final state population maximum can be effectively enhanced due to the increase of the enhancement in the near-resonant part, but the TL-normalized final state population maximum is constant by varying the laser central frequency. These studies can provide a clear physical picture for understanding the coherent features of the resonance-mediated two-photon absorption, and can also provide a theoretical guidance for the future applications.
基金carried out under the sponsorship and financial support from the Key Laboratory of Optoelectronic Materials Chemistry and Physics,Chinese Academy of Sciences
文摘Ammonium 5-sulfosalicylic acid monohydrate (NH4·C7H5O6S·H2O, ASSA) was synthesized and optical grade crystal with dimensions of 45ram × 20mm × 18mm was obtained from aqueous solution by the cooling solution method. The crystal structure was confirmed by X-ray single-crystal diffraction method and the empirical composition is C7HIINO7S with formula weight 253.23. The crystal belongs to monoclinic space group P21/c with a = 1 1.884(9), b = 7.306(5), c = 12.152(9) A, β = 104.851(13)°, V= 1019.8(13) A3, Z = 4, Dc = 1.649 g/cm3,μ = 0.340 mm-1, F(000) =528, the final R= 0.0307 and wR= 0.0866 for 7494 observed reflections (I〉 2σ(I)), Elemental analysis, 1R and 1H-NMR spectrum were used to characterize the compound. Thermal analysis showed that one coordination water molecule was contained and dehydration temperature of ASSA crystal was 106℃. Optical transmission and fluorescence spectrum revealed that the ASSA crystal exhibited a strong absorption in ultraviolet region with the sharp absorption edge located at 340 nm and a significant blue fluorescent emission band at 442 nm.
基金supported by National Natural Science Foundation of China(11671100 and 12171104)the National Science Fund for Excellent Young Scholars(11922107)Guangxi Natural Science Foundation(2018GXNSFAA138210 and 2019JJG110010)。
文摘The pointwise space-time behaviors of the Green’s function and the global solution to the Vlasov-Poisson-Fokker-Planck(VPFP)system in three dimensional space are studied in this paper.It is shown that the Green’s function consists of the diffusion waves decaying exponentially in time but algebraically in space,and the singular kinetic waves which become smooth for all(t,x,v)when t>0.Furthermore,we establish the pointwise space-time behaviors of the global solution to the nonlinear VPFP system when the initial data is not necessarily smooth in terms of the Green’s function.
基金the National Natural Science Foundation of China (Grant No.10562002) the Natural Science Foundation of Inner Mongolia (Grant Nos.200508010103,200711020106)
文摘This paper deals with the structure of the spectrum of infinite dimensional Hamiltonian operators.It is shown that the spectrum,the union of the point spectrum and residual spectrum,and the continuous spectrum are all symmetric with respect to the imaginary axis of the complex plane. Moreover,it is proved that the residual spectrum does not contain any pair of points symmetric with respect to the imaginary axis;and a complete characterization of the residual spectrum in terms of the point spectrum is then given.As applications of these structure results,we obtain several necessary and sufficient conditions for the residual spectrum of a class of infinite dimensional Hamiltonian operators to be empty.
基金support provided for this research by the Special Funds for Major State Basic Research Project(G20000779)the 863 National Project(2002AA243011,2003AA209010 and H020821020130)
文摘Recent studies have demonstrated the application of vegetation indices from canopy reflectedspectrum for inversion of chlorophyll concentration. Some indices are both response tovariations of vegetation and environmental factors. Canopy chlorophyll concentration, anindicator of photosynthesis activity, is related to nitrogen concentration in green vegetationand serves as an indicator of the crop response to soil nitrogen fertilizer application. Thecombination of normalized difference vegetation index (NDVI) and photochemical reflectanceindex (PRI) can reduce the effect of leaf area index (LAI) and soil background. The canopychlorophyll inversion index (CCII) was proved to be sensitive to chlorophyll concentration andvery resistant to the other variations. This paper introduced the ratio of TCARI/OSAVI to makeaccurate predictions of winter wheat chlorophyll concentration under different cultivars. Itindicated that canopy chlorophyll concentration could be evaluated by some combined vegetationindices.
基金Supported by NSFC(21171166,21222102,21301172,21373220,21571178,21525104,51277091,51402296,51502288 and 51502290)Chunmiao Project of Haixi Institute of Chinese Academy of Sciences(CMZX-2015-003)NSF of Fujian Province(2015J01219,2015J05040)
文摘A new boroantimonate K2SbB3O8 has been synthesized by high-temperature solidstate reactions, and its crystals have been obtained by the flux method. The crystal structure has been determined from single-crystal X-ray diffraction analysis. The compound crystallizes in the monoclinic space group P21/c with a = 5.8890(2), b = 11.0512(4), c = 10.8951(4)A, β =103.200(4)°, V = 690.32(4) A^3, Z = 4, F(000) = 672, ρc = 3.467 g/cm^3, Mr = 360.38 and μ = 5.215mm^-1. Its structure feature is a three-dimensional framework composed of SbO6 octahedra and isolated [B3O8]^7- groups with K+ cations residing in the one-dimensional tunnels along the a-axis.Interestingly, the isolated [B3O8]^7- groups are distinct from the known [B3O8]^7- groups, which always connect to each other. The UV-vis-NIR absorption, thermal stability and infrared spectrum are also discussed in this paper.
基金Funded in Part by the National Natural Science Foundation of China(No.61601384)
文摘The electron paramagnetic resonance(EPR) spectra of trigonal Mn^(2+) centers in Zn(ClO4)2·6(H2O) and Mg(ClO4)2·6(H2O) crystals were studied on the basis of the complete energy matrices for a d^5 configuration ion in a trigonal ligand field. It was demonstrated that the local lattice structure around a trigonal Mn^(2+) center has an compressed distortion along the crystalline c3 axis, and when Mn^(2+) is doped in the Zn(ClO4)2·6(H2O) and Mg(ClO4)2·6(H2O) crystals, there is a similar local distortion. From the EPR calculation, the local lattice structure parameters R=2.183 2 ?, for Zn(ClO4)2·6(H2O), R=2.130 2 ?, for Mg(ClO4)2·6(H2O) have been determined.
基金Project supported by the National Natural Science Foundation of China.
文摘In this paper a series of ab initio SCF and configuration calculations were reported for the ground state and excited states X^2E, A^2E,~2B_2 and ~2A_1 of allene.For ground state X^2E Jahn- Teller distorsion was discussed and a twisted angle of 50° and a torsional barriers of 0.21—0.51 eV were derived.Based on calculated results,the experimental photoelectron spectrum of allene has been assigned.
文摘CH_3CCo_3(CO)_9 was synthesized from the reaction between chloralose and Co_2(CO)_. The radical anion was generated by electrochemical reduction,and electron spin resonance spectra in THF were recorded by in situ electrolysis in the sample tube in the ESR cavity at 298 and 110K with the spectral data
文摘Searching for effective biomarkers is one of the most challenging tasks in the research ?eld of Autism Spectrum Disorder(ASD). Magnetic resonance imaging(MRI) provides a non-invasive and powerful tool for investigating changes in the structure, function, maturation,connectivity, and metabolism of the brain of children with ASD. Here, we review the more recent MRI studies in young children with ASD, aiming to provide candidate biomarkers for the diagnosis of childhood ASD. The review covers structural imaging methods, diffusion tensor imaging, resting-state functional MRI, and magnetic resonance spectroscopy. Future advances in neuroimaging techniques, as well as cross-disciplinary studies and largescale collaborations will be needed for an integrated approach linking neuroimaging, genetics, and phenotypic data to allow the discovery of new, effective biomarkers.
基金supported in part by the National Key R&D Program of China(2017YFA0303500)the National Natural Science Foundation of China(U1932201,21727801,and 51902303)+4 种基金the National Natural Science Foundation of China-Ministry of Foreign Affairs and International Cooperation of Italy(51861135202)CAS International Partnership Program(211134KYSB20190063)Key Research Program of Frontier Sciences(QYZDB-SSW-SLH018)the University of Science and Technology of China start-up fundCAS Interdisciplinary Innovation Team。
文摘Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).
基金This study was supported by the National Natural Science Foundation of China under Grant Nos. 11347007 and 11674131, the Qing Lan Project, the Colleges and Universities in Jiangsu Province Natural Science Research Project under Grant No 14KJB460013, and the Priority Academic Program Develop- ment of Jiangsu Higher Education Institutions. Y. L. Li thanks the support from the Chinese Scholarship Council. C. M. Hao thanks the support from the Postgraduate Research 8z Practice Innovation Program of Jiangsu Province under Grant No. KYCX17_1652.
文摘The elastic, dynamical, and electronic properties of cubic LiHg and Li3Hg were investigated based on first-principles methods. The elastic constants and phonon spectral calculations confirmed the mechanical and dynamical stability of the materials at ambient conditions. The obtained elastic moduli of LiHg are slightly larger than those of Li3Hg. Both LiHg and Li3Hg are ductile materials with strong shear anisotropy as metals with mixed ionic, covalent, and metallic interactions. The calculated Debye temperatures are 223.5 K and 230.6 K for LiHg and Li3Hg, respectively. The calculated phonon frequency of the T2g mode in Li3Hg is 326.8 cm-1. The p states from the Hg and Li atoms dominate the electronic structure near the Fermi level. These findings may inspire further experimental and theoretical study on the potential technical and engineering applications of similar alkali metal-based intermetallic compounds.