ZrO2-mullite nano-ceramics were fabricated by in-situ controlled crystallizing from SiO2-Al2O3-ZrO2 amorphous bulk. The thermal transformation sequences of the SiO2-Al2O3-ZrO2 amorphous bulk were investigated by X-ray...ZrO2-mullite nano-ceramics were fabricated by in-situ controlled crystallizing from SiO2-Al2O3-ZrO2 amorphous bulk. The thermal transformation sequences of the SiO2-Al2O3-ZrO2 amorphous bulk were investigated by X-ray diffraction, infrared spectrum, scanning electron microscope and differential scanning calorimetric. And the mechanical properties of the nano-ceramics were studied. The results show that the bulks are still in amorphous state at 900 ℃ and the t-ZrO2 forms at about 950 ℃ with a faint spinel-like phase which changes into mullite on further heating. ZrO2 and mullite become major phases at 1 100 ℃ and an amount of m-ZrO2 occur at the same time. The sample heated at 950 ℃ for 2 h and then at 1 100 ℃ for 1 h shows very dense and homogenous microstructure with ball-like grains in size of 20-50 nm. With the increase of crystallization temperature up to 1 350 ℃, the grains grow quickly and some grow into lath-shaped grains with major diameter of 5 μm. After two-step treatment the highest micro-hardness, flexural strength and fracture toughness of the samples are 13.72 GPa, 520 MPa and 5.13 MPa·m1/2, respectively.展开更多
Au films with a thickness of about 300 nm were deposited on SiO_2/Si(100) andmica substrates by dc sputtering. X-ray diffraction spectroscopy and field emission scanningelectron microscopy were used to analyze the str...Au films with a thickness of about 300 nm were deposited on SiO_2/Si(100) andmica substrates by dc sputtering. X-ray diffraction spectroscopy and field emission scanningelectron microscopy were used to analyze the structure and internal stress of the Au films. Thefirms grown on SiO_2/Si(100) show a preferential orientation of [111] in the growth direction.However the films grown on mica have mixture crystalline orientations of [111], [200], [220] and[311] in the growth direction and the orientations of [200] and [311] are slightly more than thoseof [111] and [220]. An internal stress in the films grown on SiO_2/Si(100) is tensile. For Au filmsgrown on mica the internal stresses in the [111]- and [311]-orientation grains are compressive whilethose in the [200]- and [220]-orientation grains are tensile. Au films grown SiO_2/Si(100) havesome very large grains with a size of about 400 nm and have a wider grain size distribution comparedwith those grown on mica.展开更多
Novel models （2× 1） of Si（001）-SiO2 interface structure have been established. The method of the first-principle General Gradient Approximation （GGA） is employed to structurally optimize the established the...Novel models （2× 1） of Si（001）-SiO2 interface structure have been established. The method of the first-principle General Gradient Approximation （GGA） is employed to structurally optimize the established theoretical models under the K-point space of periodic boundary condition. The structures after optimization have been analyzed, and the results show that the interfaces present in disordered state and both Si-O-Si and Si=O structures exist. Meanwhile, the bonding of surface structure is analyzed via the graphics of electron localization function（ELF）.展开更多
8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-deso...8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-visible diffuse reflectance spectroscopy （DRS） and scanning transmission electron microscopy-high-angle annular dark field （STEM HAADF）. The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure： The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.展开更多
In order to ameliorate the electrochemical hydrogen storage performance of La-Mg-Ni system A2B7-type electrode alloys, a small amount of Si was added. The La0.8Mg0.2Ni3.3Co0.2Six （x=0-0.2） electrode alloys were prep...In order to ameliorate the electrochemical hydrogen storage performance of La-Mg-Ni system A2B7-type electrode alloys, a small amount of Si was added. The La0.8Mg0.2Ni3.3Co0.2Six （x=0-0.2） electrode alloys were prepared by casting and annealing. The effects of adding Si on the structure and electrochemical hydrogen storage characteristics of the alloys were investigated systematically. The results indicate that the as-cast and annealed alloys hold multiple structures, involving two major phases of （La, Mg）2Ni7 with a Ce2Ni7-type hexagonal structure and LaNi5 with a CaCu5-type hexagonal structure as well as one residual phase LaNi3. The addition of Si results in a decrease in （La, Mg）2Ni7 phase and an increase in LaNi5 phase without changing the phase structure of the alloys. What is more, it brings on an obvious effect on electrochemical hydrogen storage characteristics of the alloys. The discharge capacities of the as-cast and annealed alloys decline with the increase of Si content, but their cycle stabilities clearly grow under the same condition. Furthermore, the measurements of the high rate discharge ability, the limiting current density, hydrogen diffusion coefficient as well as electrochemical impedance spectra all indicate that the electrochemical kinetic properties of the electrode alloys first increase and then decrease with the rising of Si content.展开更多
In the present work, structure changes during （SiO2） composites have been investigated systematically stretching of isotactic polypropylene （iPP） and iPP/silicon dioxide The or-form crystal structure of both iPP a...In the present work, structure changes during （SiO2） composites have been investigated systematically stretching of isotactic polypropylene （iPP） and iPP/silicon dioxide The or-form crystal structure of both iPP and iPP/SiO2 composites is destroyed and transforms into the mesophase as the samples are stretched at a low temperature （35℃）, while stretching at high temperatures （90℃ and 120℃） can restrain the appearance of defects and keep the perfection of crystal structure. FTIR results reveal that the stretching temperatures show no obvious difference of the effect on the orientation of pure iPP, however, the orientation of iPP/SiO2 composites is greatly changed by the tensile temperature. In the case of micron-sized SiO2 particles （average particle diameter d 〉 1 μm）, the orientation of the composites is lower than that of pure iPP at all stretching temperatures. The above results suggest that the stretching temperature and the SiO2 particle size have great influence on the structure variation and orientation behavior of iPP/SiO2 composites.展开更多
The study of nanocrystalline SnO2 (n-SnO2) and SiO2-doped SnO2 (n-Si-SnO2) samples pre-pared by the sol-gel process showed that SiO2 doping can effectively restrained the growth of nanocrystalline SnO2 grains, thus im...The study of nanocrystalline SnO2 (n-SnO2) and SiO2-doped SnO2 (n-Si-SnO2) samples pre-pared by the sol-gel process showed that SiO2 doping can effectively restrained the growth of nanocrystalline SnO2 grains, thus improving thermal stability of the materials.展开更多
By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon ...By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon monocrystal under dry oxygen atmosphere at 1100℃.Compared with their oxidation kinetic curves consisted of three stages,we suggested a mechanism on forming silicon oxide film.According to electron and X-ray diffraction analyses the silicon oxide films consisted of silica with different crystal structure.We also have discussed a stacking fault and a dislocation formed in the Si-Sio_2 interface region simulaneously forming silicon oxide film.展开更多
The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and ...The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and specific magnetization of the FeCo alloy particles depend on the Co content.展开更多
LaF^3＋ Yb^3＋ , Er^3＋ nanoparticles were successfully synthesized using solvothermal treatment, and LaF^3＋ Yb^3＋ , Er^3＋/SiO2 core/shell nanoparticles were also prepared with reverse microemulsion technique. The ...LaF^3＋ Yb^3＋ , Er^3＋ nanoparticles were successfully synthesized using solvothermal treatment, and LaF^3＋ Yb^3＋ , Er^3＋/SiO2 core/shell nanoparticles were also prepared with reverse microemulsion technique. The crystal structure, morphology and photoluminescence properties of as-prepared core/shell nanoparticles were in- vestigated by X-ray diffraction, transmission electron microscopy and fluorescence spectrophotometer. The re- sults showed thatLaF^3＋ Yb^3＋ , Er^3＋ nanoparticles are of hexagonal structure and SiO2 shell is amorphous. The size ofLaF^3＋ Yb^3＋ , Er^3＋. nanoparticles is 13 nm and the LaF^3＋ Yb^3＋ , Er^3＋/SiO2 nanoparticles present clearly a core/shell structure with 12 nm shell thickness. The solubility of LaF^3＋ Yb^3＋ , Er^3＋ nanocrystals in water and the biocompatibility are both improved by the SiO2 shell. The upconversion luminescence spectra suggested that the SiO~ shell has small effect on the upconversion luminescence properties of the LaF^3＋ Yb^3＋ , Er^3＋ nanocrys- tals. The core/shell structure LaF^3＋ Yb^3＋ , Er^3＋ /SiO2. nanopartlcles are expected to be used in biological appli- cations.展开更多
Molecular dynamics simulations of the x CaO (1- x )SiO 2 melts ( x varying with the composition of melt) were performed to achieve some structural information. It is found that the first peak positions of Si Si, Si O ...Molecular dynamics simulations of the x CaO (1- x )SiO 2 melts ( x varying with the composition of melt) were performed to achieve some structural information. It is found that the first peak positions of Si Si, Si O and O O partial radial distribution functions RDFs(3.165 ?, 1.612 ? and 2.6 ?)agree very well with those of x ray diffraction experiments. The discovered relation of coordinate number N Si Si ( r 0) with the molar ratio of CaO is linear and the slope is -0.056 17. The average bond lengths of Si O b and Si O nb are 1.6275～1.630 ? and 1.595～1.60 ?, respectively. Both distribution curves of the angles O Si O and Si O Si show one peak. For the distribution of angle O Si O the positions of the peaks are just a little less than the typical tetrahedral angle 109.5°. And for angle Si O Si the positions of peaks fluctuate in the range from 148° to 151°. At last, the distribution of five Si O tetrahedra was obtained and discussed.展开更多
In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation meth...In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.展开更多
This paper reported a novel synthetic route to Eu2＋ doped SrSiN2 deep red phosphors for white light-emitting diodes. A series of single-phased and high-efficiency SrSiN2：Eu2＋ red phosphors were synthesized based on...This paper reported a novel synthetic route to Eu2＋ doped SrSiN2 deep red phosphors for white light-emitting diodes. A series of single-phased and high-efficiency SrSiN2：Eu2＋ red phosphors were synthesized based on this method. Their structure, morphology, luminescence, quantum efficiency （QE） and thermal quenching properties were investigated and compared with those of SrSiN2： Eu2＋ prepared by the conventional route. It was found that the addition of a small amount of Si3N4 could promote the formation of SrSiN2 from Sr2SisN8 phase. A highly uniform rod-shaped morphology was obtained based on this method. The X-ray powder diffraction and the Rietveld refinement analysis identified the preferential crystalline orientation growth. Under the blue light excitation, Eu2＋ doped SrSiN2 phosphors showed excellent optical properties. Compared with those prepared by the conventional approaches, the external QE of SrSiN2：Eu2＋ phosphor was greatly improved, allowing it a promising phosphor for white LEDs.展开更多
Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of ...Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.展开更多
X-ray powder diffraction, resistivity and magnetization studies have been performed on polycrystalline Nd（FexMn1-x）2Si2 （0≤x 〈 1） compounds which crystallize in a ThCr2Si2-type structure with the space group 14/...X-ray powder diffraction, resistivity and magnetization studies have been performed on polycrystalline Nd（FexMn1-x）2Si2 （0≤x 〈 1） compounds which crystallize in a ThCr2Si2-type structure with the space group 14/mmm. The field-cooled temperature dependence of the magnetization curves shows that, at low temperatures, NdFe2Si2 is antiferromagnetic, while the other compounds show ferromagnetic behaviour. The substitution of Fe for Mn leads to a decrease in lattice parameters a, c and unit-cell volume V. The Curie temperature of the compounds first increases, reaches a maximum around x=0.7, then decreases with Fe content. However, the saturation magnetization decreases monotonically with increasing Fe content. This Fe concentration dependent magnetization of Nd（FexMn1-x）2Si2 compounds can be well explained by taking into account the complex effect on magnetic properties due to the substitution of Mn by Fe. The temperature＇s square dependence on electrical resistivity indicates that the curve of Nd（Fe0.6Mn0.4）2Si2 has a quasi-linear character above its Curie temperature, which is typical of simple metals.展开更多
Molecular dynamics simulation is applied to investigate the mechanism and variation of self-diffusion in calcium aluminosilicate slags. The self-diffusion coefficients are calculated for eleven slag compositions with ...Molecular dynamics simulation is applied to investigate the mechanism and variation of self-diffusion in calcium aluminosilicate slags. The self-diffusion coefficients are calculated for eleven slag compositions with varying Al2O3/SiO2 ratios at a fixed CaO content. In practice, the results of the study are relevant to the significant changes in transport phenomenon caused by the changes in chemical composition during continuous casting of steels containing high amounts of dissolved aluminum. The cooperative movement between O atoms and network formers is discussed since [AlO4] and [SiO4] tetrahedra are the elementary structural units in the CaO-Al2O3-SiO2 (CAS) slag system. The diffusivities for four atomic types are affected by the degree of polymerization (DOP) of slag network characterized by the proportions of non-bridging oxygen (NBO) and Qn species in the system. On the other hand, a sudden increase in 5-coordinated Al as network modifiers in high alumina regions slightly increases the self-diffusion coefficient for Al. As another structural defect, oxygen tricluster plays an important role in the behavior of self-diffusion for O atoms, while the diffusivity for Ca is deeply influenced by its bonding and coordinating conditions.展开更多
基金Project(2003AA332040) supported by the National High Technology Research and Development Program of China
文摘ZrO2-mullite nano-ceramics were fabricated by in-situ controlled crystallizing from SiO2-Al2O3-ZrO2 amorphous bulk. The thermal transformation sequences of the SiO2-Al2O3-ZrO2 amorphous bulk were investigated by X-ray diffraction, infrared spectrum, scanning electron microscope and differential scanning calorimetric. And the mechanical properties of the nano-ceramics were studied. The results show that the bulks are still in amorphous state at 900 ℃ and the t-ZrO2 forms at about 950 ℃ with a faint spinel-like phase which changes into mullite on further heating. ZrO2 and mullite become major phases at 1 100 ℃ and an amount of m-ZrO2 occur at the same time. The sample heated at 950 ℃ for 2 h and then at 1 100 ℃ for 1 h shows very dense and homogenous microstructure with ball-like grains in size of 20-50 nm. With the increase of crystallization temperature up to 1 350 ℃, the grains grow quickly and some grow into lath-shaped grains with major diameter of 5 μm. After two-step treatment the highest micro-hardness, flexural strength and fracture toughness of the samples are 13.72 GPa, 520 MPa and 5.13 MPa·m1/2, respectively.
文摘Au films with a thickness of about 300 nm were deposited on SiO_2/Si(100) andmica substrates by dc sputtering. X-ray diffraction spectroscopy and field emission scanningelectron microscopy were used to analyze the structure and internal stress of the Au films. Thefirms grown on SiO_2/Si(100) show a preferential orientation of [111] in the growth direction.However the films grown on mica have mixture crystalline orientations of [111], [200], [220] and[311] in the growth direction and the orientations of [200] and [311] are slightly more than thoseof [111] and [220]. An internal stress in the films grown on SiO_2/Si(100) is tensile. For Au filmsgrown on mica the internal stresses in the [111]- and [311]-orientation grains are compressive whilethose in the [200]- and [220]-orientation grains are tensile. Au films grown SiO_2/Si(100) havesome very large grains with a size of about 400 nm and have a wider grain size distribution comparedwith those grown on mica.
基金Supported by the National Grand Fundamental Research 973 Program of China (No. 51310Z07-3) and the Research Program of Application of Sichuan Department of Science and Technology (No. 02GY029-006)
文摘Novel models （2× 1） of Si（001）-SiO2 interface structure have been established. The method of the first-principle General Gradient Approximation （GGA） is employed to structurally optimize the established theoretical models under the K-point space of periodic boundary condition. The structures after optimization have been analyzed, and the results show that the interfaces present in disordered state and both Si-O-Si and Si=O structures exist. Meanwhile, the bonding of surface structure is analyzed via the graphics of electron localization function（ELF）.
文摘8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-visible diffuse reflectance spectroscopy （DRS） and scanning transmission electron microscopy-high-angle annular dark field （STEM HAADF）. The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure： The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.
基金Projects(50961009,51161015)supported by the National Natural Science Foundation of ChinaProject(2011AA03A408)supported by the High-tech Research and Development Program of ChinaProjects(2011ZD10,2010ZD05)supported by the Natural Science Foundation of Inner Mongolia,China
文摘In order to ameliorate the electrochemical hydrogen storage performance of La-Mg-Ni system A2B7-type electrode alloys, a small amount of Si was added. The La0.8Mg0.2Ni3.3Co0.2Six （x=0-0.2） electrode alloys were prepared by casting and annealing. The effects of adding Si on the structure and electrochemical hydrogen storage characteristics of the alloys were investigated systematically. The results indicate that the as-cast and annealed alloys hold multiple structures, involving two major phases of （La, Mg）2Ni7 with a Ce2Ni7-type hexagonal structure and LaNi5 with a CaCu5-type hexagonal structure as well as one residual phase LaNi3. The addition of Si results in a decrease in （La, Mg）2Ni7 phase and an increase in LaNi5 phase without changing the phase structure of the alloys. What is more, it brings on an obvious effect on electrochemical hydrogen storage characteristics of the alloys. The discharge capacities of the as-cast and annealed alloys decline with the increase of Si content, but their cycle stabilities clearly grow under the same condition. Furthermore, the measurements of the high rate discharge ability, the limiting current density, hydrogen diffusion coefficient as well as electrochemical impedance spectra all indicate that the electrochemical kinetic properties of the electrode alloys first increase and then decrease with the rising of Si content.
基金financially supported by the National Natural Science Foundation of China (Nos. 51073004 and 21074141)the China National Funds for Distinguished Young Scientists (No. 50925313)
文摘In the present work, structure changes during （SiO2） composites have been investigated systematically stretching of isotactic polypropylene （iPP） and iPP/silicon dioxide The or-form crystal structure of both iPP and iPP/SiO2 composites is destroyed and transforms into the mesophase as the samples are stretched at a low temperature （35℃）, while stretching at high temperatures （90℃ and 120℃） can restrain the appearance of defects and keep the perfection of crystal structure. FTIR results reveal that the stretching temperatures show no obvious difference of the effect on the orientation of pure iPP, however, the orientation of iPP/SiO2 composites is greatly changed by the tensile temperature. In the case of micron-sized SiO2 particles （average particle diameter d 〉 1 μm）, the orientation of the composites is lower than that of pure iPP at all stretching temperatures. The above results suggest that the stretching temperature and the SiO2 particle size have great influence on the structure variation and orientation behavior of iPP/SiO2 composites.
文摘The study of nanocrystalline SnO2 (n-SnO2) and SiO2-doped SnO2 (n-Si-SnO2) samples pre-pared by the sol-gel process showed that SiO2 doping can effectively restrained the growth of nanocrystalline SnO2 grains, thus improving thermal stability of the materials.
文摘By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon monocrystal under dry oxygen atmosphere at 1100℃.Compared with their oxidation kinetic curves consisted of three stages,we suggested a mechanism on forming silicon oxide film.According to electron and X-ray diffraction analyses the silicon oxide films consisted of silica with different crystal structure.We also have discussed a stacking fault and a dislocation formed in the Si-Sio_2 interface region simulaneously forming silicon oxide film.
文摘The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and specific magnetization of the FeCo alloy particles depend on the Co content.
文摘LaF^3＋ Yb^3＋ , Er^3＋ nanoparticles were successfully synthesized using solvothermal treatment, and LaF^3＋ Yb^3＋ , Er^3＋/SiO2 core/shell nanoparticles were also prepared with reverse microemulsion technique. The crystal structure, morphology and photoluminescence properties of as-prepared core/shell nanoparticles were in- vestigated by X-ray diffraction, transmission electron microscopy and fluorescence spectrophotometer. The re- sults showed thatLaF^3＋ Yb^3＋ , Er^3＋ nanoparticles are of hexagonal structure and SiO2 shell is amorphous. The size ofLaF^3＋ Yb^3＋ , Er^3＋. nanoparticles is 13 nm and the LaF^3＋ Yb^3＋ , Er^3＋/SiO2 nanoparticles present clearly a core/shell structure with 12 nm shell thickness. The solubility of LaF^3＋ Yb^3＋ , Er^3＋ nanocrystals in water and the biocompatibility are both improved by the SiO2 shell. The upconversion luminescence spectra suggested that the SiO~ shell has small effect on the upconversion luminescence properties of the LaF^3＋ Yb^3＋ , Er^3＋ nanocrys- tals. The core/shell structure LaF^3＋ Yb^3＋ , Er^3＋ /SiO2. nanopartlcles are expected to be used in biological appli- cations.
文摘Molecular dynamics simulations of the x CaO (1- x )SiO 2 melts ( x varying with the composition of melt) were performed to achieve some structural information. It is found that the first peak positions of Si Si, Si O and O O partial radial distribution functions RDFs(3.165 ?, 1.612 ? and 2.6 ?)agree very well with those of x ray diffraction experiments. The discovered relation of coordinate number N Si Si ( r 0) with the molar ratio of CaO is linear and the slope is -0.056 17. The average bond lengths of Si O b and Si O nb are 1.6275～1.630 ? and 1.595～1.60 ?, respectively. Both distribution curves of the angles O Si O and Si O Si show one peak. For the distribution of angle O Si O the positions of the peaks are just a little less than the typical tetrahedral angle 109.5°. And for angle Si O Si the positions of peaks fluctuate in the range from 148° to 151°. At last, the distribution of five Si O tetrahedra was obtained and discussed.
基金support from the Ministry of Science and Technology (Nos.2012BAC20B10)the National Natural Science Foundation of China (Nos. 21321061 and 20976109)
文摘In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.
基金supported by the National Basic Research Program of China(9732014CB643801)+1 种基金the National Natural Science Foundation of China(5110202151302016)
文摘This paper reported a novel synthetic route to Eu2＋ doped SrSiN2 deep red phosphors for white light-emitting diodes. A series of single-phased and high-efficiency SrSiN2：Eu2＋ red phosphors were synthesized based on this method. Their structure, morphology, luminescence, quantum efficiency （QE） and thermal quenching properties were investigated and compared with those of SrSiN2： Eu2＋ prepared by the conventional route. It was found that the addition of a small amount of Si3N4 could promote the formation of SrSiN2 from Sr2SisN8 phase. A highly uniform rod-shaped morphology was obtained based on this method. The X-ray powder diffraction and the Rietveld refinement analysis identified the preferential crystalline orientation growth. Under the blue light excitation, Eu2＋ doped SrSiN2 phosphors showed excellent optical properties. Compared with those prepared by the conventional approaches, the external QE of SrSiN2：Eu2＋ phosphor was greatly improved, allowing it a promising phosphor for white LEDs.
基金supported by the National Natural Science Foundation of China-Excellent Young Scholars(No.51922068)the National Key Research and Development Program(No.2017YFA0403800)+1 种基金the National Natural Science Foundation of China(Nos.51727802,51821001 and 51971138)Shanghai Pujiang Program(No.19PJ1404400)。
文摘Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.
基金Project supported by the National Basic Research Program of China (Grant No 2006CB601101)
文摘X-ray powder diffraction, resistivity and magnetization studies have been performed on polycrystalline Nd（FexMn1-x）2Si2 （0≤x 〈 1） compounds which crystallize in a ThCr2Si2-type structure with the space group 14/mmm. The field-cooled temperature dependence of the magnetization curves shows that, at low temperatures, NdFe2Si2 is antiferromagnetic, while the other compounds show ferromagnetic behaviour. The substitution of Fe for Mn leads to a decrease in lattice parameters a, c and unit-cell volume V. The Curie temperature of the compounds first increases, reaches a maximum around x=0.7, then decreases with Fe content. However, the saturation magnetization decreases monotonically with increasing Fe content. This Fe concentration dependent magnetization of Nd（FexMn1-x）2Si2 compounds can be well explained by taking into account the complex effect on magnetic properties due to the substitution of Mn by Fe. The temperature＇s square dependence on electrical resistivity indicates that the curve of Nd（Fe0.6Mn0.4）2Si2 has a quasi-linear character above its Curie temperature, which is typical of simple metals.
文摘Molecular dynamics simulation is applied to investigate the mechanism and variation of self-diffusion in calcium aluminosilicate slags. The self-diffusion coefficients are calculated for eleven slag compositions with varying Al2O3/SiO2 ratios at a fixed CaO content. In practice, the results of the study are relevant to the significant changes in transport phenomenon caused by the changes in chemical composition during continuous casting of steels containing high amounts of dissolved aluminum. The cooperative movement between O atoms and network formers is discussed since [AlO4] and [SiO4] tetrahedra are the elementary structural units in the CaO-Al2O3-SiO2 (CAS) slag system. The diffusivities for four atomic types are affected by the degree of polymerization (DOP) of slag network characterized by the proportions of non-bridging oxygen (NBO) and Qn species in the system. On the other hand, a sudden increase in 5-coordinated Al as network modifiers in high alumina regions slightly increases the self-diffusion coefficient for Al. As another structural defect, oxygen tricluster plays an important role in the behavior of self-diffusion for O atoms, while the diffusivity for Ca is deeply influenced by its bonding and coordinating conditions.
