The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H...The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H- and Zr3O7H- are observed after the reaction. Den-sity functional theory calculations indicate that the hydrogen abstraction is favorable in the reaction of Zr2O5- with C2H6, which supports that the observed Zr2O5H- and Zr3O7H- are due to hydrogen atom abstraction from the alkane molecules. This work shows a newpossible pathway in the reaction of zirconium oxide cluster anions with alkane molecules.展开更多
A new silicate fluoride,NaBa3 Si207 F,has been successfully synthesized by a high-temperature solution method.It crystallizes in the orthorhombic space group Cmcm(No.63).NaBa3 Si2 O7 F is the first barium-containing a...A new silicate fluoride,NaBa3 Si207 F,has been successfully synthesized by a high-temperature solution method.It crystallizes in the orthorhombic space group Cmcm(No.63).NaBa3 Si2 O7 F is the first barium-containing alkali metal silicate fluoride with the[NaO6]polyhedra,the[BaO8 F]polyhedra and isolated[Si2 O7]units.The optical characterizations indicate that NaBa3 Si2 O7 F possesses wide transparent window and available luminescence properties.To confirm the coordination surroundings of anionic groups and its thermostability,infrared spectroscopy and thermal behaviors were also analyzed,which proved the existence of tetrahedronly coordinated silicium atoms and the good stability of NaBa3 Si2 O7 F at high temperature.First-principles calculation was also implemented for better understanding the relationship between the structure of NaBa3 Si207 F and its property.Additionally,to further explore the structural novelty of NaBa3 Si2 O7 F,the comparison of the anionic structures was carried out in mixed alkali and alkaline-earth metal silicate fluorides.Interestingly,the result indicates the isolated[Si2 O7]dimer is rare among the above systems,which enriches the structural chemistry of silicate fluorides.展开更多
Abstract The structural and energetic properties of bimetallic AgmCun （m ＋n ≤ 5） in the cationic and anionic charged states have been investigated by density functional theory with relativistic effective core pote...Abstract The structural and energetic properties of bimetallic AgmCun （m ＋n ≤ 5） in the cationic and anionic charged states have been investigated by density functional theory with relativistic effective core potentails. The stable cationic pentamers have three-dimensional structures in contrast to anionic clusters assume planar structures. For the given cluster size the electron affinities decrease as the Cu content increases, while no clear trend can be found in adiabatic ionization potentials. The binding energy per atom also increases with the increasing Cu content and follows the order anion 〈 cation. The most probable dissociation channels of the clusters considered are also discussed.展开更多
基金This work was supported by the Chinese Academy of Sciences （Hundred Talents Fund）, the National Natural Science Foundation of China （No.20703048 and No.20803083）, and the Center of Molecular Science Foundation of Institute of Chemistry, Chinese Academy of Sciences （No.CMS-LX200902）.
文摘The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H- and Zr3O7H- are observed after the reaction. Den-sity functional theory calculations indicate that the hydrogen abstraction is favorable in the reaction of Zr2O5- with C2H6, which supports that the observed Zr2O5H- and Zr3O7H- are due to hydrogen atom abstraction from the alkane molecules. This work shows a newpossible pathway in the reaction of zirconium oxide cluster anions with alkane molecules.
基金supported by the National Natural Science Foundation of China(U1703132,51872325 and 61835014)Tianshan Innovation Team Program(2018D14001)+5 种基金Xinjiang International Science&Technology Cooperation Program(2017E01014)the National Key Research Project(2016YFB0402104)the Science and Technology Project of Urumqi(P161010002)Xinjiang Key Research and Development Program(2016B02021)Major Program of Xinjiang Uygur Autonomous Region of China during the 13th Five-Year Plan Period(2016A02003)West Light Foundation of the Chinese Academy of Sciences(2016-YJRC-2)
文摘A new silicate fluoride,NaBa3 Si207 F,has been successfully synthesized by a high-temperature solution method.It crystallizes in the orthorhombic space group Cmcm(No.63).NaBa3 Si2 O7 F is the first barium-containing alkali metal silicate fluoride with the[NaO6]polyhedra,the[BaO8 F]polyhedra and isolated[Si2 O7]units.The optical characterizations indicate that NaBa3 Si2 O7 F possesses wide transparent window and available luminescence properties.To confirm the coordination surroundings of anionic groups and its thermostability,infrared spectroscopy and thermal behaviors were also analyzed,which proved the existence of tetrahedronly coordinated silicium atoms and the good stability of NaBa3 Si2 O7 F at high temperature.First-principles calculation was also implemented for better understanding the relationship between the structure of NaBa3 Si207 F and its property.Additionally,to further explore the structural novelty of NaBa3 Si2 O7 F,the comparison of the anionic structures was carried out in mixed alkali and alkaline-earth metal silicate fluorides.Interestingly,the result indicates the isolated[Si2 O7]dimer is rare among the above systems,which enriches the structural chemistry of silicate fluorides.
基金Supported by the National Natural Science Foundation of China under Grant No. 20873036the Fund for Doctorates of Henan University of Science and Technology
文摘Abstract The structural and energetic properties of bimetallic AgmCun （m ＋n ≤ 5） in the cationic and anionic charged states have been investigated by density functional theory with relativistic effective core potentails. The stable cationic pentamers have three-dimensional structures in contrast to anionic clusters assume planar structures. For the given cluster size the electron affinities decrease as the Cu content increases, while no clear trend can be found in adiabatic ionization potentials. The binding energy per atom also increases with the increasing Cu content and follows the order anion 〈 cation. The most probable dissociation channels of the clusters considered are also discussed.
