Making full use of coordination-driven self-assembly strategy,we herein described the selective synthesis of a molecular Borromean rings and two cases of “U”-shaped tweezer-like molecular assemblies in high yield by...Making full use of coordination-driven self-assembly strategy,we herein described the selective synthesis of a molecular Borromean rings and two cases of “U”-shaped tweezer-like molecular assemblies in high yield by using bipyridyl ligands based on biphenyl unit and half-sandwich binuclear rhodium(III)/iridium(III) building blocks.The selective synthesis was realized by adjusting the length of dipyridyl arms.The utilization of curved U-shaped bipyridyl ligand L1 led to tweezer-like molecular assemblies.Subsequently,olefinic bonds were introduced to elongate dipyridyl arms obtaining ligand L2.The ligand L2 has two stable conformations,U-shape and Z-shape,which facilitated the formation of different topologies including the tetranuclear macrocycle and Borromean rings with different building blocks in this work.These structures in solid and solution all have been further confirmed by single-crystal X-ray diffraction,NMR analysis,and mass spectrometry.In addition,as an important driving force,π-π stacking interactions not only played a significant role in the stability of structures but also further triggered photothermal conversion in solution.The experimental results demonstrated that compounds 1a and 2 had good NIR photothermal conversion efficiency (11.83% and 17.76%),and further analysis found the photothermal conversion efficiency had a gradual increase in the trend with the π-π stacking interactions increasing.This research expands the application of topological structures in materials science and provides a new idea for the synthesis of novel photothermal conversion materials.展开更多
The NMR and FT\|IR Spectra of ten (ηC 6H\-9CRR′ Cp)\-2MCl\-2 (M=Ti,Zr) were measured.The constructions of the compounds were identified by 1H NMR and 13 C NMR spectra.All complexes are bonded by M\|Cp through center...The NMR and FT\|IR Spectra of ten (ηC 6H\-9CRR′ Cp)\-2MCl\-2 (M=Ti,Zr) were measured.The constructions of the compounds were identified by 1H NMR and 13 C NMR spectra.All complexes are bonded by M\|Cp through center of Cp.The vibration modes were reasonably assigned,absorption of ν s M\|Cp (A\-1) (M=Ti and Zr) vibration all appear in 310?cm -1 or so,while ν as M\|Cp (B) appear around 410?cm -1 and 360?cm -1 for Ti and Zr respectively.The influence of the center metal atoms and the substituents upon the NMR and FT\|IR spectra were discussed.展开更多
A simple arylhydrazone containing the benzothiazole moiety which may be used as an efficient ligand in the palladium-catalyzed Mizoroki-Heck and Suzuki-Miyaura cross-coupling reactions, under infrared irradiation as a...A simple arylhydrazone containing the benzothiazole moiety which may be used as an efficient ligand in the palladium-catalyzed Mizoroki-Heck and Suzuki-Miyaura cross-coupling reactions, under infrared irradiation as an alternative source of energy, is presented. The reactions proceeded with extremely high efficiency under mild conditions and produced very good yields.展开更多
Changes of surface shape, aggregate state, and microstructure of Apocynum fiber before and after irradia-tion were studied by XRD, IR, SEM, ESR, and solid state 13C CP/ MAS NMR. The results show that the surface shape...Changes of surface shape, aggregate state, and microstructure of Apocynum fiber before and after irradia-tion were studied by XRD, IR, SEM, ESR, and solid state 13C CP/ MAS NMR. The results show that the surface shape and microstructure were not spoiled under 50 kGy gamma irradiation, while the crystallization of Apocynum fiber changed under 280 kGy . It also shows that different free radicals appear after irradiation and their concentration increases with the increase of irradiation dose.展开更多
An Ir-catalyzed selective mono-sulfamidation of 2-arylquinazolinones has been achieved with a low catalyst loading under mild conditions.A series of regioselective mono-sulfamided 2-arylquinazolinones were obtained in...An Ir-catalyzed selective mono-sulfamidation of 2-arylquinazolinones has been achieved with a low catalyst loading under mild conditions.A series of regioselective mono-sulfamided 2-arylquinazolinones were obtained in up to 90%yields.Compared with our previous work of constructing di-sulfamidated 2-arylquinazolinones,the mono-sulfamided products could be obtained selectively by changing the ratio of substrates,the loading of catalyst,acid additive,and reaction time.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22031003,21720102004)the Shanghai Science Technology Committee(No.19DZ2270100)G.-X.J.thanks the Alexander von Humboldt Foundation for a Humboldt Research Award.
文摘Making full use of coordination-driven self-assembly strategy,we herein described the selective synthesis of a molecular Borromean rings and two cases of “U”-shaped tweezer-like molecular assemblies in high yield by using bipyridyl ligands based on biphenyl unit and half-sandwich binuclear rhodium(III)/iridium(III) building blocks.The selective synthesis was realized by adjusting the length of dipyridyl arms.The utilization of curved U-shaped bipyridyl ligand L1 led to tweezer-like molecular assemblies.Subsequently,olefinic bonds were introduced to elongate dipyridyl arms obtaining ligand L2.The ligand L2 has two stable conformations,U-shape and Z-shape,which facilitated the formation of different topologies including the tetranuclear macrocycle and Borromean rings with different building blocks in this work.These structures in solid and solution all have been further confirmed by single-crystal X-ray diffraction,NMR analysis,and mass spectrometry.In addition,as an important driving force,π-π stacking interactions not only played a significant role in the stability of structures but also further triggered photothermal conversion in solution.The experimental results demonstrated that compounds 1a and 2 had good NIR photothermal conversion efficiency (11.83% and 17.76%),and further analysis found the photothermal conversion efficiency had a gradual increase in the trend with the π-π stacking interactions increasing.This research expands the application of topological structures in materials science and provides a new idea for the synthesis of novel photothermal conversion materials.
文摘The NMR and FT\|IR Spectra of ten (ηC 6H\-9CRR′ Cp)\-2MCl\-2 (M=Ti,Zr) were measured.The constructions of the compounds were identified by 1H NMR and 13 C NMR spectra.All complexes are bonded by M\|Cp through center of Cp.The vibration modes were reasonably assigned,absorption of ν s M\|Cp (A\-1) (M=Ti and Zr) vibration all appear in 310?cm -1 or so,while ν as M\|Cp (B) appear around 410?cm -1 and 360?cm -1 for Ti and Zr respectively.The influence of the center metal atoms and the substituents upon the NMR and FT\|IR spectra were discussed.
文摘A simple arylhydrazone containing the benzothiazole moiety which may be used as an efficient ligand in the palladium-catalyzed Mizoroki-Heck and Suzuki-Miyaura cross-coupling reactions, under infrared irradiation as an alternative source of energy, is presented. The reactions proceeded with extremely high efficiency under mild conditions and produced very good yields.
基金Supported by National National Science Foundation (20464002)
文摘Changes of surface shape, aggregate state, and microstructure of Apocynum fiber before and after irradia-tion were studied by XRD, IR, SEM, ESR, and solid state 13C CP/ MAS NMR. The results show that the surface shape and microstructure were not spoiled under 50 kGy gamma irradiation, while the crystallization of Apocynum fiber changed under 280 kGy . It also shows that different free radicals appear after irradiation and their concentration increases with the increase of irradiation dose.
基金supported by the National Natural Science Foundation of China (No.21572072)Xiamen Southern Oceanographic Center (No.15PYY052SF01)+3 种基金111 Project (No.BC2018061)the Postgraduates Innovative Fund in Scientific Research of Huaqiao Universitythe financial support of Scientific Research Foundation of Xiamen Huaxia University (No. HX201807)Outstanding Youth Scientific Research Cultivation Plan in Fujian Province University (2018)
文摘An Ir-catalyzed selective mono-sulfamidation of 2-arylquinazolinones has been achieved with a low catalyst loading under mild conditions.A series of regioselective mono-sulfamided 2-arylquinazolinones were obtained in up to 90%yields.Compared with our previous work of constructing di-sulfamidated 2-arylquinazolinones,the mono-sulfamided products could be obtained selectively by changing the ratio of substrates,the loading of catalyst,acid additive,and reaction time.
