The interaction of Ag atoms with a defective MgO（001） surface is systematically studied based on density functional theory. The Ag clusters are deposited on neutral and charged oxygen vacancies of the MgO（001） sur...The interaction of Ag atoms with a defective MgO（001） surface is systematically studied based on density functional theory. The Ag clusters are deposited on neutral and charged oxygen vacancies of the MgO（001） surface. The structures of Ag clusters take the shape of simple models of two- or three-dimensional （2D and 3D） metal particles deposited on the MgO surface. When the nucleation of the metal clusters occurs in the Fs （missing neutral O） centre, the interaction with the substrate is considerably stronger than that in the Fs^＋ （missing O-） centre. The results show that the adsorption of Ag atoms on the MgO surface with oxygcn vacancy is stronger than on a clear MgO surface, thereby attracting more Ag atoms to cluster together, and forming atomic islands.展开更多
Room-temperature ferromagnetism has been experimentally observed in annealed rutile TiO2 single crystals when a magnetic field is applied parallel to the sample plane.By combining X-ray absorption near the edge struct...Room-temperature ferromagnetism has been experimentally observed in annealed rutile TiO2 single crystals when a magnetic field is applied parallel to the sample plane.By combining X-ray absorption near the edge structure spectrum and positron annihilation lifetime spectroscopy,Ti^3＋-V O defect complexes（or clusters） have been identified in annealed crystals at a high vacuum.We elucidate that the unpaired 3d electrons in Ti^3＋ ions provide the observed room-temperature ferromagnetism.In addition,excess oxygen ions in the TiO2 lattice could induce a number of Ti vacancies which obviously increase magnetic moments.展开更多
By using the first-principles calculation, we studied the mechanisms of point defects in Y4AI209 （YAM）, a promising ternary oxide with excellent optical and thermal properties. It is found that the predominant nativ...By using the first-principles calculation, we studied the mechanisms of point defects in Y4AI209 （YAM）, a promising ternary oxide with excellent optical and thermal properties. It is found that the predominant native defect species is closely dependent on the chemical potentials of each constituent. In the case of O-rich condition, the oxygen interstitial has the very low defect formation energy, followed by the anti-site defects and AI vacancy; in the case of AI-rich condition, the oxygen vacancy yields the lowest defect formation energy, followed by the anti-site defects and AI interstitial. The present result shows that in all the possible chemical potential ranges, anti-site defects have relatively low defect formation energy and might exist in high concentration in YAM. Furthermore, AIy anti-site has relatively lower defect formation energy than the YAt anti- site throughout. The behaviors of defect complexes under non-stoichiometric condition, such as the AI203 or Y203 excess, are also investigated. The results provide helpful guide to optimize the experimental synthesizing of YAM.展开更多
The adsorption of O2 over defective La2O3-based OCM catalysts with anionic vacancies , and the reaction of surface oxygen species with CH4 were studied by means of in situ confocal microprobe Raman spectra. The partia...The adsorption of O2 over defective La2O3-based OCM catalysts with anionic vacancies , and the reaction of surface oxygen species with CH4 were studied by means of in situ confocal microprobe Raman spectra. The partially reduced oxygen species O2, O , O (O<&<1 ) and even the lattice oxygen ion O2-can be detected on the surface of O2-pretreated La2O3-based catalysts. At lower temperatures (< 573 K) it is peroxide species O- or O- that is more essential for the coupling of methane,while at higher temperature. the superoxide O2 and lattice oxygen species O2-are rather important. It is easier for fluoride-containing La2O3-based catalysts to induce the oxygen species with fewer negative charges and the basicity of the cat- alyst surface is weakened , so that the C2 selectivity for OCM reaction is improved.展开更多
Defects of polymer-derived Si-C-O fibers were intensively studied by the SEM and TEM techniques and their originations were also discussed on the basis of factors experiments.The defects were found mainly in the form ...Defects of polymer-derived Si-C-O fibers were intensively studied by the SEM and TEM techniques and their originations were also discussed on the basis of factors experiments.The defects were found mainly in the form of strumaes,pits and splits on surfaces as well as microflaw networks,porosity clusters and inclusions in the bulk.Factors experiments reveal that a nonuniform or an insufficient curing would result in larger-sized strumaes or interior microflaws.Gas evolution rates due to different firing rates have a great influence on the formation of internal microflaws or porosity clusters and some oxidation-induced pits or splits may be formed on surfaces because of a trace of oxygen or water vapor accumulated from the flowing inert atmosphere during pyrolysis.展开更多
基金Project supported by the Scientific Research Fund of Hunan Provincial Education Department, China (Grant No. 09B021)
文摘The interaction of Ag atoms with a defective MgO（001） surface is systematically studied based on density functional theory. The Ag clusters are deposited on neutral and charged oxygen vacancies of the MgO（001） surface. The structures of Ag clusters take the shape of simple models of two- or three-dimensional （2D and 3D） metal particles deposited on the MgO surface. When the nucleation of the metal clusters occurs in the Fs （missing neutral O） centre, the interaction with the substrate is considerably stronger than that in the Fs^＋ （missing O-） centre. The results show that the adsorption of Ag atoms on the MgO surface with oxygcn vacancy is stronger than on a clear MgO surface, thereby attracting more Ag atoms to cluster together, and forming atomic islands.
基金Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 61006066)the National Natural Science Foundation of China (Grant No. 11175191)
文摘Room-temperature ferromagnetism has been experimentally observed in annealed rutile TiO2 single crystals when a magnetic field is applied parallel to the sample plane.By combining X-ray absorption near the edge structure spectrum and positron annihilation lifetime spectroscopy,Ti^3＋-V O defect complexes（or clusters） have been identified in annealed crystals at a high vacuum.We elucidate that the unpaired 3d electrons in Ti^3＋ ions provide the observed room-temperature ferromagnetism.In addition,excess oxygen ions in the TiO2 lattice could induce a number of Ti vacancies which obviously increase magnetic moments.
基金supported by the National Natural Science Foundation of China under Grant Nos.50672102,50832008 and 51032006
文摘By using the first-principles calculation, we studied the mechanisms of point defects in Y4AI209 （YAM）, a promising ternary oxide with excellent optical and thermal properties. It is found that the predominant native defect species is closely dependent on the chemical potentials of each constituent. In the case of O-rich condition, the oxygen interstitial has the very low defect formation energy, followed by the anti-site defects and AI vacancy; in the case of AI-rich condition, the oxygen vacancy yields the lowest defect formation energy, followed by the anti-site defects and AI interstitial. The present result shows that in all the possible chemical potential ranges, anti-site defects have relatively low defect formation energy and might exist in high concentration in YAM. Furthermore, AIy anti-site has relatively lower defect formation energy than the YAt anti- site throughout. The behaviors of defect complexes under non-stoichiometric condition, such as the AI203 or Y203 excess, are also investigated. The results provide helpful guide to optimize the experimental synthesizing of YAM.
文摘The adsorption of O2 over defective La2O3-based OCM catalysts with anionic vacancies , and the reaction of surface oxygen species with CH4 were studied by means of in situ confocal microprobe Raman spectra. The partially reduced oxygen species O2, O , O (O<&<1 ) and even the lattice oxygen ion O2-can be detected on the surface of O2-pretreated La2O3-based catalysts. At lower temperatures (< 573 K) it is peroxide species O- or O- that is more essential for the coupling of methane,while at higher temperature. the superoxide O2 and lattice oxygen species O2-are rather important. It is easier for fluoride-containing La2O3-based catalysts to induce the oxygen species with fewer negative charges and the basicity of the cat- alyst surface is weakened , so that the C2 selectivity for OCM reaction is improved.
文摘Defects of polymer-derived Si-C-O fibers were intensively studied by the SEM and TEM techniques and their originations were also discussed on the basis of factors experiments.The defects were found mainly in the form of strumaes,pits and splits on surfaces as well as microflaw networks,porosity clusters and inclusions in the bulk.Factors experiments reveal that a nonuniform or an insufficient curing would result in larger-sized strumaes or interior microflaws.Gas evolution rates due to different firing rates have a great influence on the formation of internal microflaws or porosity clusters and some oxidation-induced pits or splits may be formed on surfaces because of a trace of oxygen or water vapor accumulated from the flowing inert atmosphere during pyrolysis.
