An efficient and environmentally friendly procedure for the one-pot synthesis of 13-acetyl-9-methyl-ll-oxo-8-oxa-10,12-diazatricyclo[7.3.1.0^2,7]trideca-2,4,6-triene from salicylaldehyde, acetylacetone and urea via Bi...An efficient and environmentally friendly procedure for the one-pot synthesis of 13-acetyl-9-methyl-ll-oxo-8-oxa-10,12-diazatricyclo[7.3.1.0^2,7]trideca-2,4,6-triene from salicylaldehyde, acetylacetone and urea via Biginelli condensation and intramolecular Michael-addition by using magnesium bromide as an inexpensive and easily available catalyst in a solvent-free condition is described. The structural elucidation of the product is reported by ^1H- and ^13C NMR spectra. The product can also be identified by its EI TOF mass spectrometry based on the molecular ion at m/s 246(10%) and on the fragment ions in which two nitrogen atoms are remained. Three kinds of characteristic fragmentation pathways from the molecular ion were observed. One is the loss of the OH radical to form the dihydropyrimidinone cation at m/z 229(48%), followed by elimination of a molecular methane forming the pyrimidinone cation at m/z 213(27%). The second is the cleavage of the C6H4OH radical, and the formation of the dihydropyrimidinone cation at m/z 153(24%). The third one is the loss of MeC-O radical to afford the oxygen-bridged fragment ion at m/z 203(33%).展开更多
Printing is a method of additive manufacturing that can reduce material costs and environmental contamination during the fabrication process.Ag ink is commonly used in printed electronics,such as interconnects,inducto...Printing is a method of additive manufacturing that can reduce material costs and environmental contamination during the fabrication process.Ag ink is commonly used in printed electronics,such as interconnects,inductors,and antennas.However,the high cost of noble Ag restricts its massive applications.To reduce the cost of the state-of-the-art Ag ink and realize large-scale manufacturing,we develop a molecule-bridged graphene/Ag(MB-G/A)composite to produce highly conductive and cost-effective paperbased electronics.Graphene can be used to substitute part of Ag nanoparticles to reduce costs,form a conducive percolation network,and retain a reasonable level of conductivity.We adopt cysteamine as a molecular linker,because it anchors on the surface of graphene via the diazonium reaction.Additionally,the thiol functional group on the other end of cysteamine can bond to a Ag atom,forming a molecular bridge between graphene and Ag and promoting electron transport between Ag and graphene.As a result,the maximum conductivity of MB-G/A inks can reach 2.0×10^(5)S m^(−1),enabling their successful application in various printable electronics.In addition,the optimum MB-G/A ink costs less than half as much as pure Ag inks,showing the great potential of MB-G/A ink in commercial electronic devices.展开更多
Three new homochiral bis-diamine-bridged bi-Mn(salen) complexes were synthesized. Their catalysis on asymmetric epoxidation of a-methylstyrene, styrene and indene was studied with NaC10 and m-CPBA as oxidants respec...Three new homochiral bis-diamine-bridged bi-Mn(salen) complexes were synthesized. Their catalysis on asymmetric epoxidation of a-methylstyrene, styrene and indene was studied with NaC10 and m-CPBA as oxidants respectively. This homogeneous catalyst exhibited comparable catalytic activity and enantioselectivity to the Jacobsen's catalyst in the asymmetric epoxidation of unfunctionalized olefins. Furthermore, the catalyst could be conveniently recovered and reused at least five times without significant losses of both activity and enantioselectivity. Specially, it also could be efficiently used in large-scale reactions with superior catalytic disposition being maintained at the same level, which provided the potential for the applications in industry. The effect of axial bases, temperature and solvent on activity and enantioselectivity of the catalytic system were also studied.展开更多
基金This work was supported by the Natural Science Foundation of China (No.20425309).
文摘An efficient and environmentally friendly procedure for the one-pot synthesis of 13-acetyl-9-methyl-ll-oxo-8-oxa-10,12-diazatricyclo[7.3.1.0^2,7]trideca-2,4,6-triene from salicylaldehyde, acetylacetone and urea via Biginelli condensation and intramolecular Michael-addition by using magnesium bromide as an inexpensive and easily available catalyst in a solvent-free condition is described. The structural elucidation of the product is reported by ^1H- and ^13C NMR spectra. The product can also be identified by its EI TOF mass spectrometry based on the molecular ion at m/s 246(10%) and on the fragment ions in which two nitrogen atoms are remained. Three kinds of characteristic fragmentation pathways from the molecular ion were observed. One is the loss of the OH radical to form the dihydropyrimidinone cation at m/z 229(48%), followed by elimination of a molecular methane forming the pyrimidinone cation at m/z 213(27%). The second is the cleavage of the C6H4OH radical, and the formation of the dihydropyrimidinone cation at m/z 153(24%). The third one is the loss of MeC-O radical to afford the oxygen-bridged fragment ion at m/z 203(33%).
基金financially supported by Hong Kong Scholars Program(XJ2019025)The Hong Kong Polytechnic University(CD42)Shenzhen Science and Technology Innovation Commission(JCYJ20180507183424383)。
文摘Printing is a method of additive manufacturing that can reduce material costs and environmental contamination during the fabrication process.Ag ink is commonly used in printed electronics,such as interconnects,inductors,and antennas.However,the high cost of noble Ag restricts its massive applications.To reduce the cost of the state-of-the-art Ag ink and realize large-scale manufacturing,we develop a molecule-bridged graphene/Ag(MB-G/A)composite to produce highly conductive and cost-effective paperbased electronics.Graphene can be used to substitute part of Ag nanoparticles to reduce costs,form a conducive percolation network,and retain a reasonable level of conductivity.We adopt cysteamine as a molecular linker,because it anchors on the surface of graphene via the diazonium reaction.Additionally,the thiol functional group on the other end of cysteamine can bond to a Ag atom,forming a molecular bridge between graphene and Ag and promoting electron transport between Ag and graphene.As a result,the maximum conductivity of MB-G/A inks can reach 2.0×10^(5)S m^(−1),enabling their successful application in various printable electronics.In addition,the optimum MB-G/A ink costs less than half as much as pure Ag inks,showing the great potential of MB-G/A ink in commercial electronic devices.
基金financially supported by National Ministry of Science and Technology Innovation Fund for High-tech Small and Medium Enterprise Technology (09C26215112399)National Ministry of Human Resources and Social Security Start-up Support Projects for Students Returned to Business, Office of Human Resources and Social Security Issued 2009 (143)
文摘Three new homochiral bis-diamine-bridged bi-Mn(salen) complexes were synthesized. Their catalysis on asymmetric epoxidation of a-methylstyrene, styrene and indene was studied with NaC10 and m-CPBA as oxidants respectively. This homogeneous catalyst exhibited comparable catalytic activity and enantioselectivity to the Jacobsen's catalyst in the asymmetric epoxidation of unfunctionalized olefins. Furthermore, the catalyst could be conveniently recovered and reused at least five times without significant losses of both activity and enantioselectivity. Specially, it also could be efficiently used in large-scale reactions with superior catalytic disposition being maintained at the same level, which provided the potential for the applications in industry. The effect of axial bases, temperature and solvent on activity and enantioselectivity of the catalytic system were also studied.