Three alternating conjugated polymers,namely PFTP,PCz TP,and PSi TP,which combine a thieno[3,4-b]pyrazine(TP)unit with different benzene-based donor units such as 9,9-dioctylfluorene,9-heptadecyl-9H-carbazole and 5,5-...Three alternating conjugated polymers,namely PFTP,PCz TP,and PSi TP,which combine a thieno[3,4-b]pyrazine(TP)unit with different benzene-based donor units such as 9,9-dioctylfluorene,9-heptadecyl-9H-carbazole and 5,5-dioctyl-5H-dibenzo[b,d]silole,were synthesized in good yield(>85%)and high molecular weight up to Mn=5.82×10^(4) via direct arylation polymerization(DAr P).All the resultant polymers exhibit moderate bandgap of about 1.80 e V and strong deep red/near-infrared emitting in the solid state.Among them,the PSi TP-based electroluminescence(EL)devices with an architecture of ITO/PEDOT:PSS/PTAA/emitting layer/TPBi/Li F/Al give the best performance with a maximum luminance of 2543 cd/m^(2) at 478 m A/cm^(2).This work expands the application scope of high-performance conjugated polymers which can be synthesized by DAr P.展开更多
A new coordination polymer {[Cd(C_(21)H_(14)N_6)(C_8H_4O_4)]·H_2O}_n(1) was synthesized by an elaborate design via the reaction of 3-(2,6-di(pyrazin-2-yl)pyridin-4-yl)-1H-indole(bppi),1,4-benzene-...A new coordination polymer {[Cd(C_(21)H_(14)N_6)(C_8H_4O_4)]·H_2O}_n(1) was synthesized by an elaborate design via the reaction of 3-(2,6-di(pyrazin-2-yl)pyridin-4-yl)-1H-indole(bppi),1,4-benzene-dicarboxylic acid(H2bdc) and cadmium(Ⅱ) nitrate in CH_3OH/H_2O mixed solvents. Complex 1 crystallizes in orthorhombic,space group Ccca with a = 20.012(4),b = 31.881(6),c = 19.808(4) ?,V = 12638(4) ?~3,Z = 16,C_(29)H_(20)CdN_6O_5,M_r = 644.91,D_c = 1.356 g·cm^(-3),μ = 0.735 mm^(-1),F(000) = 5184,GOOF = 1.046,the final R = 0.0405 and wR = 0.1063 for 6870 observed reflections(I 〉 2σ(I)). The Cd(Ⅱ) centre is hepta-coordinated by three N and four O atoms from one bppi terminal ligand and two bdc2– ligands,respectively,displaying a capped trigonal prism geometry. Structure extension gives coordination polymeric chains,in which the bdc2– linkers connect Cd(Ⅱ) cations into a one-dimensional(1D) coordination polymer along the c axis,giving zigzag chains with the Cd···Cd separation of 11.178(1) ?. The adjacent bppi terminal ligands in the chains are anti-periplanar conformation. The three-dimensional(3D) structure is stabilized by π···π stacking and hydrogen-bonding interactions to form a supramolecular self-penetrating network with 1D channels. In 1,there are voids 2999.7 ?~3 with 23.7% of per unit cell volume. Thermal analysis indicates that the framework of 1 is stable until 651 K and the photoluminescence of 1 in the solid shows very weak fluorescence at 382 and 560 nm upon excitation at 310 nm.展开更多
Two new one-dimensional chains extended by alternate benzenedicarboxylate(BDC) and 4-(2,6-di(pyrazin-2-yl)pyridin-4-yl)benzoate(L-) connectors, {[Cu(L)(BDC)(0.5)]·3.5 H2 O}n (1) and {[Zn(L)(BD...Two new one-dimensional chains extended by alternate benzenedicarboxylate(BDC) and 4-(2,6-di(pyrazin-2-yl)pyridin-4-yl)benzoate(L-) connectors, {[Cu(L)(BDC)(0.5)]·3.5 H2 O}n (1) and {[Zn(L)(BDC)(0.5)] ·H2 O}n (2), were solvothermally synthesized. Complex 1 is in triclinic system, space group P1 with a = 9.6456(14), b = 11.1160(16), c = 12.0414(18) A, α = 106.266(3), β = 92.277(3), γ =108.104(3)°, V = 1166.6(3) A3, Dc = 1.603 g·cm(-3), Mr = 563.00, Z = 2, F(000) = 578, μ = 0.996 mm(-1), the final R = 0.0575 and wR = 0.1386 for 3704 observed reflections with I > 2σ(I). Complex 2 crystallizes in monoclinic, space group C2/c with a = 28.607(5), b = 8.9767(16), c = 19.705(4) ?, β = 125.396(3)°, V = 4125.0(13) ?3, Dc = 1.674 g·cm(-3), Mr = 519.79, Z = 8, F(000) = 2120, μ = 1.242 mm(-1), the final R = 0.0487 and w R = 0.0907 for 2944 observed reflections with I > 2σ(I). Resulting from the narrower band gap and broader response to visible light, the CuII-chain exhibits better photocatalytic performance towards the degradation of rhodamine B and methylene blue than those of ZnII-chain.展开更多
Isoxazole derivatives were characterized by broad spectrum of biological activities, but the condensed heterocyclic compounds containing isoxazole were scarcely reported. In this paper, we studied the 1,3-dipolar cycl...Isoxazole derivatives were characterized by broad spectrum of biological activities, but the condensed heterocyclic compounds containing isoxazole were scarcely reported. In this paper, we studied the 1,3-dipolar cycloaddition of p-methoxybenzohydroxamoyl chloride with ethyl sodioacetoacetate to obtain a key intermediate 2. Through compound 2, fifteen novel S-triazolo-1,3,4-thiadiazines(5a-5e), imidazolo-1,3,4-thiadiazoles(9a-9e) and imidazolo-1,3,4-oxadiazoles(10a-10e) containing isoxazole, which have potentially useful biological activities, were synthesized. The structures of the products were confirmed by elemental analyses and spectral analysis. And the characteristic data of IR, 1H NMR and MS were explained reasonably.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21604063 and 52173010)the Program for Prominent Young College Teachers of Tianjin Educational Committee。
文摘Three alternating conjugated polymers,namely PFTP,PCz TP,and PSi TP,which combine a thieno[3,4-b]pyrazine(TP)unit with different benzene-based donor units such as 9,9-dioctylfluorene,9-heptadecyl-9H-carbazole and 5,5-dioctyl-5H-dibenzo[b,d]silole,were synthesized in good yield(>85%)and high molecular weight up to Mn=5.82×10^(4) via direct arylation polymerization(DAr P).All the resultant polymers exhibit moderate bandgap of about 1.80 e V and strong deep red/near-infrared emitting in the solid state.Among them,the PSi TP-based electroluminescence(EL)devices with an architecture of ITO/PEDOT:PSS/PTAA/emitting layer/TPBi/Li F/Al give the best performance with a maximum luminance of 2543 cd/m^(2) at 478 m A/cm^(2).This work expands the application scope of high-performance conjugated polymers which can be synthesized by DAr P.
基金supported by the National Natural Science Foundation of China(Nos.21571118&21271121)
文摘A new coordination polymer {[Cd(C_(21)H_(14)N_6)(C_8H_4O_4)]·H_2O}_n(1) was synthesized by an elaborate design via the reaction of 3-(2,6-di(pyrazin-2-yl)pyridin-4-yl)-1H-indole(bppi),1,4-benzene-dicarboxylic acid(H2bdc) and cadmium(Ⅱ) nitrate in CH_3OH/H_2O mixed solvents. Complex 1 crystallizes in orthorhombic,space group Ccca with a = 20.012(4),b = 31.881(6),c = 19.808(4) ?,V = 12638(4) ?~3,Z = 16,C_(29)H_(20)CdN_6O_5,M_r = 644.91,D_c = 1.356 g·cm^(-3),μ = 0.735 mm^(-1),F(000) = 5184,GOOF = 1.046,the final R = 0.0405 and wR = 0.1063 for 6870 observed reflections(I 〉 2σ(I)). The Cd(Ⅱ) centre is hepta-coordinated by three N and four O atoms from one bppi terminal ligand and two bdc2– ligands,respectively,displaying a capped trigonal prism geometry. Structure extension gives coordination polymeric chains,in which the bdc2– linkers connect Cd(Ⅱ) cations into a one-dimensional(1D) coordination polymer along the c axis,giving zigzag chains with the Cd···Cd separation of 11.178(1) ?. The adjacent bppi terminal ligands in the chains are anti-periplanar conformation. The three-dimensional(3D) structure is stabilized by π···π stacking and hydrogen-bonding interactions to form a supramolecular self-penetrating network with 1D channels. In 1,there are voids 2999.7 ?~3 with 23.7% of per unit cell volume. Thermal analysis indicates that the framework of 1 is stable until 651 K and the photoluminescence of 1 in the solid shows very weak fluorescence at 382 and 560 nm upon excitation at 310 nm.
文摘Two new one-dimensional chains extended by alternate benzenedicarboxylate(BDC) and 4-(2,6-di(pyrazin-2-yl)pyridin-4-yl)benzoate(L-) connectors, {[Cu(L)(BDC)(0.5)]·3.5 H2 O}n (1) and {[Zn(L)(BDC)(0.5)] ·H2 O}n (2), were solvothermally synthesized. Complex 1 is in triclinic system, space group P1 with a = 9.6456(14), b = 11.1160(16), c = 12.0414(18) A, α = 106.266(3), β = 92.277(3), γ =108.104(3)°, V = 1166.6(3) A3, Dc = 1.603 g·cm(-3), Mr = 563.00, Z = 2, F(000) = 578, μ = 0.996 mm(-1), the final R = 0.0575 and wR = 0.1386 for 3704 observed reflections with I > 2σ(I). Complex 2 crystallizes in monoclinic, space group C2/c with a = 28.607(5), b = 8.9767(16), c = 19.705(4) ?, β = 125.396(3)°, V = 4125.0(13) ?3, Dc = 1.674 g·cm(-3), Mr = 519.79, Z = 8, F(000) = 2120, μ = 1.242 mm(-1), the final R = 0.0487 and w R = 0.0907 for 2944 observed reflections with I > 2σ(I). Resulting from the narrower band gap and broader response to visible light, the CuII-chain exhibits better photocatalytic performance towards the degradation of rhodamine B and methylene blue than those of ZnII-chain.
文摘Isoxazole derivatives were characterized by broad spectrum of biological activities, but the condensed heterocyclic compounds containing isoxazole were scarcely reported. In this paper, we studied the 1,3-dipolar cycloaddition of p-methoxybenzohydroxamoyl chloride with ethyl sodioacetoacetate to obtain a key intermediate 2. Through compound 2, fifteen novel S-triazolo-1,3,4-thiadiazines(5a-5e), imidazolo-1,3,4-thiadiazoles(9a-9e) and imidazolo-1,3,4-oxadiazoles(10a-10e) containing isoxazole, which have potentially useful biological activities, were synthesized. The structures of the products were confirmed by elemental analyses and spectral analysis. And the characteristic data of IR, 1H NMR and MS were explained reasonably.