Summary of main observation and conclusion One unique two-dimensional (2D) Zn-MOF {Na[Zz1.5(μ4-O)(L)]}n (1) was synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction. Four Zn...Summary of main observation and conclusion One unique two-dimensional (2D) Zn-MOF {Na[Zz1.5(μ4-O)(L)]}n (1) was synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction. Four Zn atoms are bridged through μ4-O to form [Zn4O] clusters, which are further linked to form a 2D layer n etwork through shari ng Zn as vertexes. 1 exhibits high thermal stability up to 280 ℃ and keeps stable in comm on solve nts and water solutions with pH ranging from 1 to 13. The catalytic studies reveal that compound 1 exhibits excellent catalytic activity for cycloaddition of CO2 with epoxides into cyclic carb on ates un der mild conditions. Furthermore, 1 dem on strates good gen erality in CO2 coupli ng reactio n with extensive epoxides. Importantly, 1 can be reused for at least five times without significant reduction in catalytic ability.展开更多
The development of promising zinc anodes mainly suffers from their low plating/stripping coulombic efficiencies when using aqueous electrolyte,which are mainly associated with the interfacial formation of irreversible...The development of promising zinc anodes mainly suffers from their low plating/stripping coulombic efficiencies when using aqueous electrolyte,which are mainly associated with the interfacial formation of irreversible by-products.It is urgent to develop technologies that can solve this issue fundamentally.Herein,we report an artificial Sc_(2)O_(3) protective film to construct a new class of interface for Zn anode.The density functional theory simulation and experimental results have proven that the interfacial side reaction was inhibited via a stratified adsorption effect between this artificial layer and Zn anode.Benefiting from this novel structure,the Sc_(2)O_(3)-coated Zn anode can run for more than 100 cycles without short circuit and exhibit low voltage hysteresis,and the coulombic efficiency increases by 1.2%.Importantly,it shows a good application prospect when matched with two of popular manganese-based and vanadium-based cathodes.The excellent electrochemical performance of the Sc_(2)O_(3)-coated Zn anode highlights the importance of rational design of anode materials and demonstrates a good way for developing high-performance Zn anodes with long lifespan and high efficiency.展开更多
In order to explore the effect mechanism of solvent on the synthesis of the metal organic framework materials, the microscopic interaction between solvent and framework and the effects of N,N-dimethyl-formamide(DMF) o...In order to explore the effect mechanism of solvent on the synthesis of the metal organic framework materials, the microscopic interaction between solvent and framework and the effects of N,N-dimethyl-formamide(DMF) or N-methyl- 2-pyrrolidone(NMP) on solvothermal synthesis of [Zn4O(BDC)3]8 were investigated through a combined DFT and experimental study. XRD and SEM showed that the absorbability of NMP in the pore of [Zn4O(BDC)3]8 was weaker than that of DMF. The thermal decomposition temperature of [Zn4O(BDC)3]8 synthesized in DMF was higher than that in NMP according to TG and FT-IR. In addition, the nitrogen sorption isotherms indicated that NMP improved gas sorption property of [Zn4O(BDC)3]8. The COSMO optimized calculations indicated that the total energy of Zn4O(BDC)3 in NMP was higher than that in DMF, and compared with non-solvent system, the charge of zinc atoms decreased and the charge value was the smallest in NMP. Furthermore, the interaction of DMF, NMP or DEF in [Zn4O(BDC)3]8 crystal model was calculated by DFT method. The results suggested that NMP should be easier to be removed from pore of materials than DMF from the point of view of energy state. It can be concluded that NMP was a favorable solvent to synthesize [Zn4O(BDC)3]8 and the microscopic mechanism was that the binding force between Zn4O(BDC)3 and NMP molecule was weaker than DMF.展开更多
Green-photoluminescence material Zn4B6O13: Ce3+, Tb3+ was first synthesized by spread method of high temperature and solid state reaction, which is cubic crystal system with lattice parameters: a(0) = 0.7472 nm, V = 0...Green-photoluminescence material Zn4B6O13: Ce3+, Tb3+ was first synthesized by spread method of high temperature and solid state reaction, which is cubic crystal system with lattice parameters: a(0) = 0.7472 nm, V = 0.4172 nm(3), and structural properties are investigated by XRD. The excitation and emission band of Ce3+ ion single-doped in Zn4B6O13 transfer longer spectra 2.38 similar to 4.94 kk than in other matrices. Emission band of Ce3+ ion better overlaps with the F-7(6)-->(5)G(2),D-5(1),H-5(7) absorption band of Tb3+. It shows that emission of Tb3+ ion is sensitized by Ce3+. In Zn4B6O13:Ce3+, Tb3+, it is due to the energy transfer mechanism, resonance transfer of electric multipolar interaction of the dipole-dipole between Ce3+-->Ce3+ and Ce3+-->Tb3+. The color coordinates of Zn4B6O13: X 0.281, gamma = 0.619. The mean diameter of the particles is 0.23 mum.展开更多
基金the National Natural Science Foundation of China(Grants 21625103,21571107,and 21421001)the Ministry of Education of China(Grant B12015).
文摘Summary of main observation and conclusion One unique two-dimensional (2D) Zn-MOF {Na[Zz1.5(μ4-O)(L)]}n (1) was synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction. Four Zn atoms are bridged through μ4-O to form [Zn4O] clusters, which are further linked to form a 2D layer n etwork through shari ng Zn as vertexes. 1 exhibits high thermal stability up to 280 ℃ and keeps stable in comm on solve nts and water solutions with pH ranging from 1 to 13. The catalytic studies reveal that compound 1 exhibits excellent catalytic activity for cycloaddition of CO2 with epoxides into cyclic carb on ates un der mild conditions. Furthermore, 1 dem on strates good gen erality in CO2 coupli ng reactio n with extensive epoxides. Importantly, 1 can be reused for at least five times without significant reduction in catalytic ability.
基金supported by the National Natural Science Foundation of China(Grant no.51932011)。
文摘The development of promising zinc anodes mainly suffers from their low plating/stripping coulombic efficiencies when using aqueous electrolyte,which are mainly associated with the interfacial formation of irreversible by-products.It is urgent to develop technologies that can solve this issue fundamentally.Herein,we report an artificial Sc_(2)O_(3) protective film to construct a new class of interface for Zn anode.The density functional theory simulation and experimental results have proven that the interfacial side reaction was inhibited via a stratified adsorption effect between this artificial layer and Zn anode.Benefiting from this novel structure,the Sc_(2)O_(3)-coated Zn anode can run for more than 100 cycles without short circuit and exhibit low voltage hysteresis,and the coulombic efficiency increases by 1.2%.Importantly,it shows a good application prospect when matched with two of popular manganese-based and vanadium-based cathodes.The excellent electrochemical performance of the Sc_(2)O_(3)-coated Zn anode highlights the importance of rational design of anode materials and demonstrates a good way for developing high-performance Zn anodes with long lifespan and high efficiency.
基金Project(51104185)supported by the National Natural Science Foundation of ChinaProject(2010QZZD003)supported by the Key Project of Central South University of Fundamental Research Funds for the Central Universities of China
文摘In order to explore the effect mechanism of solvent on the synthesis of the metal organic framework materials, the microscopic interaction between solvent and framework and the effects of N,N-dimethyl-formamide(DMF) or N-methyl- 2-pyrrolidone(NMP) on solvothermal synthesis of [Zn4O(BDC)3]8 were investigated through a combined DFT and experimental study. XRD and SEM showed that the absorbability of NMP in the pore of [Zn4O(BDC)3]8 was weaker than that of DMF. The thermal decomposition temperature of [Zn4O(BDC)3]8 synthesized in DMF was higher than that in NMP according to TG and FT-IR. In addition, the nitrogen sorption isotherms indicated that NMP improved gas sorption property of [Zn4O(BDC)3]8. The COSMO optimized calculations indicated that the total energy of Zn4O(BDC)3 in NMP was higher than that in DMF, and compared with non-solvent system, the charge of zinc atoms decreased and the charge value was the smallest in NMP. Furthermore, the interaction of DMF, NMP or DEF in [Zn4O(BDC)3]8 crystal model was calculated by DFT method. The results suggested that NMP should be easier to be removed from pore of materials than DMF from the point of view of energy state. It can be concluded that NMP was a favorable solvent to synthesize [Zn4O(BDC)3]8 and the microscopic mechanism was that the binding force between Zn4O(BDC)3 and NMP molecule was weaker than DMF.
文摘Green-photoluminescence material Zn4B6O13: Ce3+, Tb3+ was first synthesized by spread method of high temperature and solid state reaction, which is cubic crystal system with lattice parameters: a(0) = 0.7472 nm, V = 0.4172 nm(3), and structural properties are investigated by XRD. The excitation and emission band of Ce3+ ion single-doped in Zn4B6O13 transfer longer spectra 2.38 similar to 4.94 kk than in other matrices. Emission band of Ce3+ ion better overlaps with the F-7(6)-->(5)G(2),D-5(1),H-5(7) absorption band of Tb3+. It shows that emission of Tb3+ ion is sensitized by Ce3+. In Zn4B6O13:Ce3+, Tb3+, it is due to the energy transfer mechanism, resonance transfer of electric multipolar interaction of the dipole-dipole between Ce3+-->Ce3+ and Ce3+-->Tb3+. The color coordinates of Zn4B6O13: X 0.281, gamma = 0.619. The mean diameter of the particles is 0.23 mum.
