Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenera...Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenerated charge carries and photocatalyzed organic reactions for the conversion of solar energy into chemical energy. Herein, we deposited well-dispersed Pd NPs with small size on crystallized carbon nitride(CN–C) to construct a Schottky-type Pd/CN–C hybrid for photocatalyzed Ullmann C–C homocoupling of aryl halides under visible light irradiation at room temperature. Compared to Pd NPs supported g-C_3N_4(Pd/g-C_3N_4), Pd/CN–C exhibits excellent visible light photocatalytic activity for Ullmann C–C coupling of aryl halides due to high crystallinity of CN–C support, high dispersion and smaller size of Pd NPs, and the interfacial heterojunction of Pd/CN–C. Upon visible light irradiation, more photogenerated electrons from CN–C flow across the Schottky junction to metallic Pd and trigger the Ullmann C–C coupling of aryl halides. The photogenerated holes on CN–C surface are captured by a protic solvent(such as EtOH). In the presence of base K_2CO_3, the solvent undergoes dissociation, dehydrogenation, and finally can be oxidized by captured photogenerated holes. Moreover, Pd/CN–C has general applicability for various substrates and shows excellent stability and reusability for more than nine cycles.展开更多
The crystal structure of the new title compound （E）-ethyl 6-benzyl-2-[（cyclopropylmethylamino）（4-fluorophenylamino）methyleneamino]-4,5,6,7-tetrahydrothieno[2,3-c]pyridine-3-carboxylate ethanol monosolvate （C28H...The crystal structure of the new title compound （E）-ethyl 6-benzyl-2-[（cyclopropylmethylamino）（4-fluorophenylamino）methyleneamino]-4,5,6,7-tetrahydrothieno[2,3-c]pyridine-3-carboxylate ethanol monosolvate （C28H31FN 4O2S·C2H6O, Mr=552.70） has been prepared and determined by single-crystal X-ray diffraction. The crystal is of monoclinic system, space group P21/c with a=13.806（10）, b=10.850（7）, c=19.938（14）, β=98.842（9）° , V=2951（4）3 , Z=4, Dc=1.244g/cm 3 , F（000）=1176, μ=0.153 mm-1 , MoKα radiation （λ=0.71073）, R=0.0758 and wR=0.2234 for 4262 observed reflections with I 〉 2σ（I）. Intramolecular N-H…S and C-H…N interactions as well as intermolecular N-H…O and O-H…N hydrogen bonds help to stabilize the crystal structure. X-ray diffraction analysis reveals that the asymmetric unit contains one title molecule and one ethanol molecule.展开更多
Novel bent shape tenary facial amphiphilic imidazolium ILC which consist of a ^-conjugated bent aromatic cores （2,5-dithiophenylethynyl phenyl bent core）, two terminal poliphilic alkyl chains and lateral n-alky chai...Novel bent shape tenary facial amphiphilic imidazolium ILC which consist of a ^-conjugated bent aromatic cores （2,5-dithiophenylethynyl phenyl bent core）, two terminal poliphilic alkyl chains and lateral n-alky chain terminated by an imidazolium bromide unit were synthesized by using Kumada and Sonogashira coupling reactions as key steps and both their thermotropic and lyotropic mesophase behaviors were studied by POM, DSC and XRD. Columnar phases were found in these compounds, a hexagonal cylinder model with core shell structure is supposed for the columnar phase formed by compound 1/8. Our study may provide a new strategy for designing new LC functional material.展开更多
基金financially supported by the National Natural Science Foundation of China(No.21503127)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2017JM2008)the 111 Project(B14041)
文摘Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenerated charge carries and photocatalyzed organic reactions for the conversion of solar energy into chemical energy. Herein, we deposited well-dispersed Pd NPs with small size on crystallized carbon nitride(CN–C) to construct a Schottky-type Pd/CN–C hybrid for photocatalyzed Ullmann C–C homocoupling of aryl halides under visible light irradiation at room temperature. Compared to Pd NPs supported g-C_3N_4(Pd/g-C_3N_4), Pd/CN–C exhibits excellent visible light photocatalytic activity for Ullmann C–C coupling of aryl halides due to high crystallinity of CN–C support, high dispersion and smaller size of Pd NPs, and the interfacial heterojunction of Pd/CN–C. Upon visible light irradiation, more photogenerated electrons from CN–C flow across the Schottky junction to metallic Pd and trigger the Ullmann C–C coupling of aryl halides. The photogenerated holes on CN–C surface are captured by a protic solvent(such as EtOH). In the presence of base K_2CO_3, the solvent undergoes dissociation, dehydrogenation, and finally can be oxidized by captured photogenerated holes. Moreover, Pd/CN–C has general applicability for various substrates and shows excellent stability and reusability for more than nine cycles.
基金Supported by the National Natural Science Foundation of China (No.21102084)the Key Project of Hubei Provincial Department of Education (No.D20091301)Doctoral Startup Foundation of China Three Gorges University (No.KJ2009B004)
文摘The crystal structure of the new title compound （E）-ethyl 6-benzyl-2-[（cyclopropylmethylamino）（4-fluorophenylamino）methyleneamino]-4,5,6,7-tetrahydrothieno[2,3-c]pyridine-3-carboxylate ethanol monosolvate （C28H31FN 4O2S·C2H6O, Mr=552.70） has been prepared and determined by single-crystal X-ray diffraction. The crystal is of monoclinic system, space group P21/c with a=13.806（10）, b=10.850（7）, c=19.938（14）, β=98.842（9）° , V=2951（4）3 , Z=4, Dc=1.244g/cm 3 , F（000）=1176, μ=0.153 mm-1 , MoKα radiation （λ=0.71073）, R=0.0758 and wR=0.2234 for 4262 observed reflections with I 〉 2σ（I）. Intramolecular N-H…S and C-H…N interactions as well as intermolecular N-H…O and O-H…N hydrogen bonds help to stabilize the crystal structure. X-ray diffraction analysis reveals that the asymmetric unit contains one title molecule and one ethanol molecule.
基金the National Natural Science Foundation of China，the Yunnan Science Foundation
文摘Novel bent shape tenary facial amphiphilic imidazolium ILC which consist of a ^-conjugated bent aromatic cores （2,5-dithiophenylethynyl phenyl bent core）, two terminal poliphilic alkyl chains and lateral n-alky chain terminated by an imidazolium bromide unit were synthesized by using Kumada and Sonogashira coupling reactions as key steps and both their thermotropic and lyotropic mesophase behaviors were studied by POM, DSC and XRD. Columnar phases were found in these compounds, a hexagonal cylinder model with core shell structure is supposed for the columnar phase formed by compound 1/8. Our study may provide a new strategy for designing new LC functional material.
