(1,4-Bis-(4-bromobenzoyl)benzene) as the monomer has been synthesized and characterized by Friedel-Crafts benzoylation reaction.Novel poly(imino ketone)s(PIKs) as high performance polymers have been obtained by ...(1,4-Bis-(4-bromobenzoyl)benzene) as the monomer has been synthesized and characterized by Friedel-Crafts benzoylation reaction.Novel poly(imino ketone)s(PIKs) as high performance polymers have been obtained by the condensation polymerization of(1,4-bis-(4-bromobenzoyl)benzene) and aromatic diamines via palladium-catalyzed aryl amination reaction.The strcture of PIKs is characterized by means of FT-IR and()1H-NMR spectroscopy,and the results show an agreement with the proposed structure.DSC and TG measurements show that PIKs possess high glass transition temperature(Tg>230℃) and good thermal stability with high decomposition temperatures(TD>500℃).PIKs also exhibit the excellent solubility,PIK-3 can be dissolved in common organic solvent CHCl3 at room temperature(20℃).展开更多
Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation...Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation reaction.The structures of PIKs are characterized by means of elemental analysis,FT-IR,~1H-NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structure.The general properties of PIKs are studied by DSC,TG and wide-angle X-ray diffraction,the solubility behavior is...展开更多
Using aromatic bis(4-bromophenyl) ether and various aromatic diamines as the monomers, a series of novel poly(amine ether)s (PAEs) have been synthesized via palladium-catalyzed aryl amination, which is the Hartw...Using aromatic bis(4-bromophenyl) ether and various aromatic diamines as the monomers, a series of novel poly(amine ether)s (PAEs) have been synthesized via palladium-catalyzed aryl amination, which is the Hartwig-Buchwald polycondensation reaction. Their structures were characterized by means of elemental analysis, FT-IR, 1^H NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structures. Their general properties were studied by DSC and TG and it's obvious that they show high glass transition temperatures (Tg〉200 ℃), good thermal stability with high decomposition temperatures (TD〉500℃) and excellent solubility. The mechanical behavior of these polymers suggested that they could be considered a new class of high-performance polymers.展开更多
This report discloses a distinctive palladium-catalyzed sequential tandem cyclization reaction of two molecular haloalkynes and one molecular N-alkylanilines,leading to the efficient assembly of various 3-halo-1,2,5-t...This report discloses a distinctive palladium-catalyzed sequential tandem cyclization reaction of two molecular haloalkynes and one molecular N-alkylanilines,leading to the efficient assembly of various 3-halo-1,2,5-triarylpyrrole derivatives.Two carbon-carbon tri-ple bonds and one carbon-halogen bond in two molecular haloalkynes are transformed conveniently in one single step,which may involve the aminoalkynylation of haloalkyne and cyclization of the newly formed enyne intermediate.The high chemo-and regiose-lectivities,good functional group tolerance and late-stage modification of the halopyrrole products further illustrate the synthetic value of this strategy.展开更多
Recent years have witnessed breakthroughs in the study of zigzag hydrocarbon belts.However,the synthesis of heterocycle-containing zigzag molecular belts remains very rare and challenging despite their interesting str...Recent years have witnessed breakthroughs in the study of zigzag hydrocarbon belts.However,the synthesis of heterocycle-containing zigzag molecular belts remains very rare and challenging despite their interesting structures and potential applications in chemistry and materials science.Here,we report the expeditious construction of a highly strained belt[4]arene[4](1,4-dihydropyridine)structure using the fjords-stitching strategy.The synthesis comprised four-fold abnormal m-bromination of four Npivaloylaniline units and Pd_(2)(dba)_(3)/4-Me_(2)NC_(6)H_(4)Pt Bu_(2)-catalyzed intramolecular C-N bond-forming reactions.Subsequent functionalization through Narylations produced a variety of tetraza-embedded octahydrobelt[8]arenes.Further oxidation of p-methoxyphenyl-substituted belt[4]arene[4](1,4-dihydropyridine)with Ag[Al(O^(t)Bu^(F))^(4)]yielded a singlet diradical dication N-doped zigzag belt.展开更多
文摘(1,4-Bis-(4-bromobenzoyl)benzene) as the monomer has been synthesized and characterized by Friedel-Crafts benzoylation reaction.Novel poly(imino ketone)s(PIKs) as high performance polymers have been obtained by the condensation polymerization of(1,4-bis-(4-bromobenzoyl)benzene) and aromatic diamines via palladium-catalyzed aryl amination reaction.The strcture of PIKs is characterized by means of FT-IR and()1H-NMR spectroscopy,and the results show an agreement with the proposed structure.DSC and TG measurements show that PIKs possess high glass transition temperature(Tg>230℃) and good thermal stability with high decomposition temperatures(TD>500℃).PIKs also exhibit the excellent solubility,PIK-3 can be dissolved in common organic solvent CHCl3 at room temperature(20℃).
基金This work was financially supported by the National Natural Science Foundation of China(No.15076017).
文摘Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation reaction.The structures of PIKs are characterized by means of elemental analysis,FT-IR,~1H-NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structure.The general properties of PIKs are studied by DSC,TG and wide-angle X-ray diffraction,the solubility behavior is...
基金Project supported by the National Natural Science Foundation of China (No. 10576017).
文摘Using aromatic bis(4-bromophenyl) ether and various aromatic diamines as the monomers, a series of novel poly(amine ether)s (PAEs) have been synthesized via palladium-catalyzed aryl amination, which is the Hartwig-Buchwald polycondensation reaction. Their structures were characterized by means of elemental analysis, FT-IR, 1^H NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structures. Their general properties were studied by DSC and TG and it's obvious that they show high glass transition temperatures (Tg〉200 ℃), good thermal stability with high decomposition temperatures (TD〉500℃) and excellent solubility. The mechanical behavior of these polymers suggested that they could be considered a new class of high-performance polymers.
基金The authors thank the National Natural Science Foundation of China(22071063 and 21871095)the Guangdong Basic and Applied Basic Research Foundation(2021B1515020058)the Key-Area Research and Development Program of Guangdong Province(2020B010188001)forfinancialsupport.
文摘This report discloses a distinctive palladium-catalyzed sequential tandem cyclization reaction of two molecular haloalkynes and one molecular N-alkylanilines,leading to the efficient assembly of various 3-halo-1,2,5-triarylpyrrole derivatives.Two carbon-carbon tri-ple bonds and one carbon-halogen bond in two molecular haloalkynes are transformed conveniently in one single step,which may involve the aminoalkynylation of haloalkyne and cyclization of the newly formed enyne intermediate.The high chemo-and regiose-lectivities,good functional group tolerance and late-stage modification of the halopyrrole products further illustrate the synthetic value of this strategy.
基金We thank the National Natural Science Foundation of China(grant nos.22050005,21732004,and 21821001)the Tsinghua University Initiative Scientific Research Program(grant no.2019Z07L01004)for generous financial support.
文摘Recent years have witnessed breakthroughs in the study of zigzag hydrocarbon belts.However,the synthesis of heterocycle-containing zigzag molecular belts remains very rare and challenging despite their interesting structures and potential applications in chemistry and materials science.Here,we report the expeditious construction of a highly strained belt[4]arene[4](1,4-dihydropyridine)structure using the fjords-stitching strategy.The synthesis comprised four-fold abnormal m-bromination of four Npivaloylaniline units and Pd_(2)(dba)_(3)/4-Me_(2)NC_(6)H_(4)Pt Bu_(2)-catalyzed intramolecular C-N bond-forming reactions.Subsequent functionalization through Narylations produced a variety of tetraza-embedded octahydrobelt[8]arenes.Further oxidation of p-methoxyphenyl-substituted belt[4]arene[4](1,4-dihydropyridine)with Ag[Al(O^(t)Bu^(F))^(4)]yielded a singlet diradical dication N-doped zigzag belt.