波粒相互作用是环电流损失的重要机制之一,但波粒相互作用导致的环电流离子沉降而损失迄今为止缺乏直接的观测证据.基于磁层及电离层卫星的协同观测,本文报道了发生在2015年9月7日,由电磁离子回旋波(EMIC波)导致环电流质子沉降的共轭观...波粒相互作用是环电流损失的重要机制之一,但波粒相互作用导致的环电流离子沉降而损失迄今为止缺乏直接的观测证据.基于磁层及电离层卫星的协同观测,本文报道了发生在2015年9月7日,由电磁离子回旋波(EMIC波)导致环电流质子沉降的共轭观测事件.在等离子体层的内边界,Van Allen Probe B卫星观测到,存在EMIC波的区域和不存在EMIC波的区域相比,离子通量的投掷角分布的各向异性变弱.我们将Van Allen Probe B卫星沿着磁力线投影到电离层高度,同时在该投影区域内DMSP 16卫星在亚极光区域观测到环电流质子沉降.而且,通过从理论上计算质子弹跳平均扩散系数,我们进一步证实观测的EMIC波确实能将环电流质子散射到损失锥中.本文的研究工作为EMIC波导致环电流质子沉降提供了直接的观测证据,揭示了环电流衰减的重要物理机制:EMIC波将环电流质子散射到损失锥中,从而沉降到低高度大气层中而损失.展开更多
To investigate the non-covalent interaction between cyclodextrins （CD） and lithium ion, a stoichiometry of α-CD, β-CD, heptakis（2,6-di-O-methyl）-β-CD （DM-β-CD）, or heptakis（2,3,6-tri-O-methyl）-β-CD （TM-...To investigate the non-covalent interaction between cyclodextrins （CD） and lithium ion, a stoichiometry of α-CD, β-CD, heptakis（2,6-di-O-methyl）-β-CD （DM-β-CD）, or heptakis（2,3,6-tri-O-methyl）-β-CD （TM-β-CD） was mixed with lithium salt, respectively, and then incubated at room temperature for 10 min to reach the equilibrium. In posi- tive mode, the electrospray ionization mass spectrometry （ESI-MS） results demonstrated that lithium ion can conjugate to α-, β-, DM-β- or TM-β-CD and form 1：1 stoichiometric non-covalent complexes. The binding of the complexes was further confirmed by collision- induced dissociation. The dissociation constants Kdl of four complexes （Li＋α-CD, Li＋β- CD, Li＋DM-β-CD, and Li＋TM-β-CD） were determined by mass spectrometric titration. The results showed Kdl were 18.7, 26.7, 33.6, 30.5 μmol/L for the complexes of Li＋ with α-CD, β-CD, DM-β-CD, and TM-β-CD, respectively. Kdl for the Li＋ complexes of/3-CD is smaller than that of DM-β-CD due to its steric effect of the partial substituted -CH3. The Kdl for the Li＋ complexes of DM-β-CD is nearly in agreement with that of TM-β-CD, indicating Li＋ is more likely to locate in the small rim of DM-β-CD＇s hydrophobic cavity. The DFT results showed through electrostatic interaction, one Li＋ can strongly conjugate to four neighboring oxygen atoms. For the （α-CD＋Li）＋ complex, one Li＋ may also situate the small rim of α-CD＇s hydrophobic cavity to form a non-specific host-guest complex.展开更多
As the largest pool of terrestrial organic carbon, soils interact strongly with atmosphere composition, climate, and land change. Soil organic carbon dynamics in ecosystem plays a great role in global carbon cycle and...As the largest pool of terrestrial organic carbon, soils interact strongly with atmosphere composition, climate, and land change. Soil organic carbon dynamics in ecosystem plays a great role in global carbon cycle and global change. With development of mathematical models that simulate changes in soil organic carbon, there have been considerable advances in understanding soil organic carbon dynamics. This paper mainly reviewed the composition of soil organic matter and its influenced factors, and recommended some soil organic matter models worldwide. Based on the analyses of the developed results at home and abroad, it is suggested that future soil organic matter models should be developed toward based-process models, and not always empirical ones. The models are able to reveal their interaction between soil carbon systems, climate and land cover by technique and methods of GIS (Geographical Information System) and RS (Remote Sensing). These models should be developed at a global scale, in dynamically describing the spatial and temporal changes of soil organic matter cycle. Meanwhile, the further researches on models should be strengthen for providing theory basis and foundation in making policy of green house gas emission in China.展开更多
Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a ...Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a temperature>100℃.Here,by employing density functional theory calculations,we studied ORR on flat and stepped Pt(111)surfaces with both(110)and(100)type of steps.We found that,in contrast to ORR under hydrous conditions,(111)terrace sites are not active for ORR under anhydrous conditions,because of weakened binding of ORR intermediates induced by O*accumulation on the surface.On the other hand,step edges,which are generally not active for ORR under hydrous conditions,are predicted to be the active sites for ORR under anhydrous conditions.Among them,(110)type step edge with a unique configuration of accumulated O stabilizes O_(2)adsorption and facilitates O_(2)dissociation,which lead an overpotential<0.4 V.To improve ORR catalysts in high-temperature PEMFCs,it is desirable to maximize(110)step edge sites that present between two(111)facets of nanoparticles.展开更多
On the basis of reported experimental vapor-liquid equilibrium （VLE） data of NH3-1-ethyl-3-methylimidazolium acetate （NH3-[Emim]Ac）, NH3-1-butyl-3-methylimidazolium tetrafluoroborate （NH3-[Bmim][BF4]）, NH3-1,3-d...On the basis of reported experimental vapor-liquid equilibrium （VLE） data of NH3-1-ethyl-3-methylimidazolium acetate （NH3-[Emim]Ac）, NH3-1-butyl-3-methylimidazolium tetrafluoroborate （NH3-[Bmim][BF4]）, NH3-1,3-dimethylimidazolium dimethyl phosphate （NH3-[Mmim]DMP） and NH3-1-ethyl-3-methylimidazolium ethylsulfate （NH3-[Emim]EtOSO3） binary systems, the interaction parameters of 14 new groups have been regressed by means of the UNIFAC model. To validate the reliability of the method, these parameters have been used to calculate the VLE data with the average relative deviation of pressures of less than 9.35%. The infinite dilution activity coefficient （ γ1∞ ） and the absorption potential （ φ1 ） are important evaluation criterions of the affinity between working pair species of the absorption cycle. The UNIFAC model is implemented to predict the values of and φ1 of t6 sets of NH3-ionic liquid （1L） systems. The work found that the φ1 gradually increases following the impact order： φ1（[Cnmim][BF4]）〈φ1（[Cnmim]EtOSO3）〈φ1（[Cnmim]DMP）〈φ1（[Cnmim]Ac） （n= 1, 2, 3, … ） at a given cation of IL species and constant temperature, and φ1（[Mmim]X）〈φ1（[Emim]X）〈φ1（[Pmim]X）〈 φ1（[Bmim]X）（X= Ac, [BF4], DMP or EtOSO3） at a given anion of IL species and constant temperature. Furthermore, the φ1 gradually increases with increasing temperature. Then, it could be concluded that the working pair NH3-[BmimlAc has the best potential research value relatively.展开更多
We study the quark loop effects on the dressed gluon propagator and also on the quark propagator itself.We find that the gluon propagators are different in two phases.The quark mass effects on the gluon propagator are...We study the quark loop effects on the dressed gluon propagator and also on the quark propagator itself.We find that the gluon propagators are different in two phases.The quark mass effects on the gluon propagator aresmall but not negligible.We also study the current quark mass dependence on the bag constant.展开更多
Isobaric vapor-liquid equilibria (VLE) are experimentally measured for the binary systems of dimethyl carbonate (DMC)+ ethylene carbonate and methanol + ethylene carbonate at 101.325kPa. The thermodynamic consistency ...Isobaric vapor-liquid equilibria (VLE) are experimentally measured for the binary systems of dimethyl carbonate (DMC)+ ethylene carbonate and methanol + ethylene carbonate at 101.325kPa. The thermodynamic consistency of these experimental data is tested with an available statistic method. Interaction parameters of the carbonate group -OCOO- with the group -CH3, ACH, CH3OH and CH3COO- in UNIFAC model are determined using the experimental and literature VLE data. The results show that the calculated VLE data using the new UNIFAC parameters agree excellently with the experimental data in this work and in literature. These results are useful in the research on DMC and diphenyl carbonate synthesis by transesterification in design of reactor and distillation tower.展开更多
A hl-quality website is crucial to a company for a successful e-business. The technique maintainers are always faced with the problem how to locate the prime factors which affect the quality of the websites. In view o...A hl-quality website is crucial to a company for a successful e-business. The technique maintainers are always faced with the problem how to locate the prime factors which affect the quality of the websites. In view of the complexity and fuzziness of BtoC webslte, a quality diagnosis method based on the multl-attribute and multi-layer fuzzy comprehensive evaluation model including all the quality factors is proposed. A simple example of diagnosis on a famous domestic BtoC websites shows the specific steps of this method and proves its validity. The process of quality evaluation and diagnosis system is illustrated and the computer program of diagnosis is Oven.展开更多
The Coulomb effect in high energy antiproton-nucleus elastic and inelastic scattering from 12C and 16O is studied in the framework of Glauber multiple scattering theory for five kinetic energies ranged from 0.23 to 1....The Coulomb effect in high energy antiproton-nucleus elastic and inelastic scattering from 12C and 16O is studied in the framework of Glauber multiple scattering theory for five kinetic energies ranged from 0.23 to 1.83 GeV.A microscopic shell-model nuclear wave functions, Woods-Saxon single-particle wave functions, and experimental pN amplitudes are used in the calculations. The results show that the Coulomb effect is of paramount importance for filling up the dips of differential cross sections. We claim that the present result for inelastic scattering of antiproton-12C is sufficiently reliable to be a guide for measurements in the very near future. We also believe that antiproton nucleus elastic and inelastic scattering may produce new information on both the nuclear structure and the antinucleon-nucleon interaction, in particular the p-neutron interaction.展开更多
The geometries and electronic spectra of a series of N-protonated corroles, including unsub- stituted H4Cor＋ and meso-triaryl substituted H4TPC＋, H4TpFPC＋, and H4TdCPC＋, were theoretically studied with density fun...The geometries and electronic spectra of a series of N-protonated corroles, including unsub- stituted H4Cor＋ and meso-triaryl substituted H4TPC＋, H4TpFPC＋, and H4TdCPC＋, were theoretically studied with density functional theory （DFT）. The results indicate that all these compounds have two conformers, one with C2 symmetry （denoted as Sl） is more stable than the other （denoted as $2, C1 symmetry） by 15.8-18.5 kJ/mol. The corrole macrocycles of these compounds show significant out-of-plane deformation. The enantiomerizations of the chiral S1 conformers were found to be a multi-step process with the $2 conformers as the intermediates. Electronic absorption spectra and electronic circular dichroism （ECD） of these compounds were calculated with time-dependent DFT. In comparison with H4Cor＋, the UV- Vis absorptions of meso-triaryl species are significantly red-shifted and their Q bands are enhanced due to the π-π conjugation between the aryl and corrole rings. Several neighboring electronic transitions were calculated with opposite signs in rotatory strengths, suggesting that ECD spectroscopy may be a useful tool in studying the electronic transitions of these compounds.展开更多
The confined longitudinal-optical （LO） phonon and surface-optical （SO） phonon modes of a free-standing annular cylindrical quantum dot are derived within the framework of dielectric continuum approximation. It is ...The confined longitudinal-optical （LO） phonon and surface-optical （SO） phonon modes of a free-standing annular cylindrical quantum dot are derived within the framework of dielectric continuum approximation. It is found that there exist two types of SO phonon modes： top SO （TSO） mode and side SO（SSO） mode in a cylindrical quantum annulus. Numerical calculation on CdS annulus system has been performed. Results reveal that the two different solutions of SSO mode distribute mainly at the inner or outer surfaces of the annulus. The dispersion relations and the coupling intensions of phonons in a quantum annulus are compared with those in a cylindrical quantum dot. It is found that the dispersion relations of the two different structures are similar, but the coupling intension of the phonon-electron interaction in quantum annulus is larger than that in quantum dot. The Hamiltonians describing the free phonon modes and their interactions with electrons in the system are also derived.展开更多
文摘波粒相互作用是环电流损失的重要机制之一,但波粒相互作用导致的环电流离子沉降而损失迄今为止缺乏直接的观测证据.基于磁层及电离层卫星的协同观测,本文报道了发生在2015年9月7日,由电磁离子回旋波(EMIC波)导致环电流质子沉降的共轭观测事件.在等离子体层的内边界,Van Allen Probe B卫星观测到,存在EMIC波的区域和不存在EMIC波的区域相比,离子通量的投掷角分布的各向异性变弱.我们将Van Allen Probe B卫星沿着磁力线投影到电离层高度,同时在该投影区域内DMSP 16卫星在亚极光区域观测到环电流质子沉降.而且,通过从理论上计算质子弹跳平均扩散系数,我们进一步证实观测的EMIC波确实能将环电流质子散射到损失锥中.本文的研究工作为EMIC波导致环电流质子沉降提供了直接的观测证据,揭示了环电流衰减的重要物理机制:EMIC波将环电流质子散射到损失锥中,从而沉降到低高度大气层中而损失.
文摘To investigate the non-covalent interaction between cyclodextrins （CD） and lithium ion, a stoichiometry of α-CD, β-CD, heptakis（2,6-di-O-methyl）-β-CD （DM-β-CD）, or heptakis（2,3,6-tri-O-methyl）-β-CD （TM-β-CD） was mixed with lithium salt, respectively, and then incubated at room temperature for 10 min to reach the equilibrium. In posi- tive mode, the electrospray ionization mass spectrometry （ESI-MS） results demonstrated that lithium ion can conjugate to α-, β-, DM-β- or TM-β-CD and form 1：1 stoichiometric non-covalent complexes. The binding of the complexes was further confirmed by collision- induced dissociation. The dissociation constants Kdl of four complexes （Li＋α-CD, Li＋β- CD, Li＋DM-β-CD, and Li＋TM-β-CD） were determined by mass spectrometric titration. The results showed Kdl were 18.7, 26.7, 33.6, 30.5 μmol/L for the complexes of Li＋ with α-CD, β-CD, DM-β-CD, and TM-β-CD, respectively. Kdl for the Li＋ complexes of/3-CD is smaller than that of DM-β-CD due to its steric effect of the partial substituted -CH3. The Kdl for the Li＋ complexes of DM-β-CD is nearly in agreement with that of TM-β-CD, indicating Li＋ is more likely to locate in the small rim of DM-β-CD＇s hydrophobic cavity. The DFT results showed through electrostatic interaction, one Li＋ can strongly conjugate to four neighboring oxygen atoms. For the （α-CD＋Li）＋ complex, one Li＋ may also situate the small rim of α-CD＇s hydrophobic cavity to form a non-specific host-guest complex.
基金The research is funded by National Natural Science Foundation (40231016) and Canadian International Development Agency (CIDA).
文摘As the largest pool of terrestrial organic carbon, soils interact strongly with atmosphere composition, climate, and land change. Soil organic carbon dynamics in ecosystem plays a great role in global carbon cycle and global change. With development of mathematical models that simulate changes in soil organic carbon, there have been considerable advances in understanding soil organic carbon dynamics. This paper mainly reviewed the composition of soil organic matter and its influenced factors, and recommended some soil organic matter models worldwide. Based on the analyses of the developed results at home and abroad, it is suggested that future soil organic matter models should be developed toward based-process models, and not always empirical ones. The models are able to reveal their interaction between soil carbon systems, climate and land cover by technique and methods of GIS (Geographical Information System) and RS (Remote Sensing). These models should be developed at a global scale, in dynamically describing the spatial and temporal changes of soil organic matter cycle. Meanwhile, the further researches on models should be strengthen for providing theory basis and foundation in making policy of green house gas emission in China.
基金supported through the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical, Biological, and Geosciences Division under DE-SC0010379the support from an ECS Toyota Young Investigator Fellowship
文摘Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a temperature>100℃.Here,by employing density functional theory calculations,we studied ORR on flat and stepped Pt(111)surfaces with both(110)and(100)type of steps.We found that,in contrast to ORR under hydrous conditions,(111)terrace sites are not active for ORR under anhydrous conditions,because of weakened binding of ORR intermediates induced by O*accumulation on the surface.On the other hand,step edges,which are generally not active for ORR under hydrous conditions,are predicted to be the active sites for ORR under anhydrous conditions.Among them,(110)type step edge with a unique configuration of accumulated O stabilizes O_(2)adsorption and facilitates O_(2)dissociation,which lead an overpotential<0.4 V.To improve ORR catalysts in high-temperature PEMFCs,it is desirable to maximize(110)step edge sites that present between two(111)facets of nanoparticles.
基金Supported by the National Natural Science Foundation of China(50890184,51276010)the National Basic Research Program of China(2010CB227304)
文摘On the basis of reported experimental vapor-liquid equilibrium （VLE） data of NH3-1-ethyl-3-methylimidazolium acetate （NH3-[Emim]Ac）, NH3-1-butyl-3-methylimidazolium tetrafluoroborate （NH3-[Bmim][BF4]）, NH3-1,3-dimethylimidazolium dimethyl phosphate （NH3-[Mmim]DMP） and NH3-1-ethyl-3-methylimidazolium ethylsulfate （NH3-[Emim]EtOSO3） binary systems, the interaction parameters of 14 new groups have been regressed by means of the UNIFAC model. To validate the reliability of the method, these parameters have been used to calculate the VLE data with the average relative deviation of pressures of less than 9.35%. The infinite dilution activity coefficient （ γ1∞ ） and the absorption potential （ φ1 ） are important evaluation criterions of the affinity between working pair species of the absorption cycle. The UNIFAC model is implemented to predict the values of and φ1 of t6 sets of NH3-ionic liquid （1L） systems. The work found that the φ1 gradually increases following the impact order： φ1（[Cnmim][BF4]）〈φ1（[Cnmim]EtOSO3）〈φ1（[Cnmim]DMP）〈φ1（[Cnmim]Ac） （n= 1, 2, 3, … ） at a given cation of IL species and constant temperature, and φ1（[Mmim]X）〈φ1（[Emim]X）〈φ1（[Pmim]X）〈 φ1（[Bmim]X）（X= Ac, [BF4], DMP or EtOSO3） at a given anion of IL species and constant temperature. Furthermore, the φ1 gradually increases with increasing temperature. Then, it could be concluded that the working pair NH3-[BmimlAc has the best potential research value relatively.
文摘We study the quark loop effects on the dressed gluon propagator and also on the quark propagator itself.We find that the gluon propagators are different in two phases.The quark mass effects on the gluon propagator aresmall but not negligible.We also study the current quark mass dependence on the bag constant.
文摘Isobaric vapor-liquid equilibria (VLE) are experimentally measured for the binary systems of dimethyl carbonate (DMC)+ ethylene carbonate and methanol + ethylene carbonate at 101.325kPa. The thermodynamic consistency of these experimental data is tested with an available statistic method. Interaction parameters of the carbonate group -OCOO- with the group -CH3, ACH, CH3OH and CH3COO- in UNIFAC model are determined using the experimental and literature VLE data. The results show that the calculated VLE data using the new UNIFAC parameters agree excellently with the experimental data in this work and in literature. These results are useful in the research on DMC and diphenyl carbonate synthesis by transesterification in design of reactor and distillation tower.
基金Supported by Key Discipline Project fromScience and Technology Committee of Shanghai(No.04JC14009) and the Research Fund ofDonghua University(No.108 10 0044934)
文摘A hl-quality website is crucial to a company for a successful e-business. The technique maintainers are always faced with the problem how to locate the prime factors which affect the quality of the websites. In view of the complexity and fuzziness of BtoC webslte, a quality diagnosis method based on the multl-attribute and multi-layer fuzzy comprehensive evaluation model including all the quality factors is proposed. A simple example of diagnosis on a famous domestic BtoC websites shows the specific steps of this method and proves its validity. The process of quality evaluation and diagnosis system is illustrated and the computer program of diagnosis is Oven.
文摘The Coulomb effect in high energy antiproton-nucleus elastic and inelastic scattering from 12C and 16O is studied in the framework of Glauber multiple scattering theory for five kinetic energies ranged from 0.23 to 1.83 GeV.A microscopic shell-model nuclear wave functions, Woods-Saxon single-particle wave functions, and experimental pN amplitudes are used in the calculations. The results show that the Coulomb effect is of paramount importance for filling up the dips of differential cross sections. We claim that the present result for inelastic scattering of antiproton-12C is sufficiently reliable to be a guide for measurements in the very near future. We also believe that antiproton nucleus elastic and inelastic scattering may produce new information on both the nuclear structure and the antinucleon-nucleon interaction, in particular the p-neutron interaction.
文摘The geometries and electronic spectra of a series of N-protonated corroles, including unsub- stituted H4Cor＋ and meso-triaryl substituted H4TPC＋, H4TpFPC＋, and H4TdCPC＋, were theoretically studied with density functional theory （DFT）. The results indicate that all these compounds have two conformers, one with C2 symmetry （denoted as Sl） is more stable than the other （denoted as $2, C1 symmetry） by 15.8-18.5 kJ/mol. The corrole macrocycles of these compounds show significant out-of-plane deformation. The enantiomerizations of the chiral S1 conformers were found to be a multi-step process with the $2 conformers as the intermediates. Electronic absorption spectra and electronic circular dichroism （ECD） of these compounds were calculated with time-dependent DFT. In comparison with H4Cor＋, the UV- Vis absorptions of meso-triaryl species are significantly red-shifted and their Q bands are enhanced due to the π-π conjugation between the aryl and corrole rings. Several neighboring electronic transitions were calculated with opposite signs in rotatory strengths, suggesting that ECD spectroscopy may be a useful tool in studying the electronic transitions of these compounds.
基金the Scientific and Technology Project of Guangzhou Municipal Government under Grant No.2004J1-C0327
文摘The confined longitudinal-optical （LO） phonon and surface-optical （SO） phonon modes of a free-standing annular cylindrical quantum dot are derived within the framework of dielectric continuum approximation. It is found that there exist two types of SO phonon modes： top SO （TSO） mode and side SO（SSO） mode in a cylindrical quantum annulus. Numerical calculation on CdS annulus system has been performed. Results reveal that the two different solutions of SSO mode distribute mainly at the inner or outer surfaces of the annulus. The dispersion relations and the coupling intensions of phonons in a quantum annulus are compared with those in a cylindrical quantum dot. It is found that the dispersion relations of the two different structures are similar, but the coupling intension of the phonon-electron interaction in quantum annulus is larger than that in quantum dot. The Hamiltonians describing the free phonon modes and their interactions with electrons in the system are also derived.
