AIM:To study the mechanism of 5-fluorouracil(5-FU)resistance in colon cancer cells and to develop strategies for overcoming such resistance by combination treatment.METHODS:We established and characterized a 5-FU resi...AIM:To study the mechanism of 5-fluorouracil(5-FU)resistance in colon cancer cells and to develop strategies for overcoming such resistance by combination treatment.METHODS:We established and characterized a 5-FU resistance(5-FU-R)cell line derived from continuous exposure(25μmol/L)to 5-FU for 20 wk in 5-FU sensitive HCT-116 cells.The proliferation and expression of different representative apoptosis and anti-apoptosis markers in 5-FU sensitive and 5-FU resistance cells were measured by the MTT assay and by Western blotting,respectively,after treatment with Resveratrol(Res)and/or 1,3-Bis(2-chloroethyl)-1-nitrosourea(BCNU).Apoptosis and cell cycle arrest was measured by 4',6'-diamidino-2-phenylindole hydrochloride staining and fluorescence-activated cell sorting analysis,respectively.The extent of DNA damage was measured by the Comet assay.We measured the visible changes in the DNA damage/repair cascade by Western blotting.RESULTS:The widely used chemotherapeutic agents BCNU and Res decreased the growth of 5-FU sensitive HCT-116 cells in a dose dependent manner.Combined application of BCNU and Res caused more apoptosis in5-FU sensitive cells in comparison to individual treatment.In addition,the combined application of BCNU and Res caused a significant decrease of major DNA base excision repair components in 5-FU sensitive cells.We established a 5-FU resistance cell line(5-FU-R)from 5-FU-sensitive HCT-116(mismatch repair deficient)cells that was not resistant to other chemotherapeutic agents(e.g.,BCNU,Res)except 5-FU.The 5-FU resistance of 5-FU-R cells was assessed by exposure to increasing concentrations of 5-FU followed by the MTT assay.There was no significant cell death noted in5-FU-R cells in comparison to 5-FU sensitive cells after5-FU treatment.This resistant cell line overexpressed anti-apoptotic[e.g.,AKT,nuclear factorκB,FLICE-like inhibitory protein),DNA repair(e.g.,DNA polymerase beta(POL-β),DNA polymerase eta(POLH),protein Flap endonuclease 1(FEN1),DNA damage-binding protein 2(DDB2)]and 5-FU-resistance proteins(thymidylate synthase)but under expressed pro-apoptotic proteins(e.g.,DAB2,CK1)in comparison to the parental cells.Increased genotoxicity and apoptosis were observed in resistant cells after combined application of BCNU and Res in comparison to untreated or parental cells.BCNU increased the sensitivity to Res of 5-FU resistant cells compared with parental cells.Fifty percent cell death were noted in parental cells when 18μmol/L of Res was associated with fixed concentration(20μmol/L)of BCNU,but a much lower concentration of Res(8μmol/L)was needed to achieve the same effect in 5-FU resistant cells.Interestingly,increased levels of adenomatous polyposis coli and decreased levels POL-β,POLH,FEN1 and DDB2 were noted after the same combined treatment in resistant cells.CONCLUSION:BCNU combined with Res exerts a synergistic effect that may prove useful for the treatment of colon cancer and to overcome drug resistance.展开更多
An energetic salt of bis(l,5-diamino-lH-tetrazolium)3,3"-bis(nitramino)-4, 4x-azo- furazan (C6H10N2206) was synthesized with the total yield of 61.7% by using 3,4-diaminofurazan (DAF) as the starting material...An energetic salt of bis(l,5-diamino-lH-tetrazolium)3,3"-bis(nitramino)-4, 4x-azo- furazan (C6H10N2206) was synthesized with the total yield of 61.7% by using 3,4-diaminofurazan (DAF) as the starting material. The structure of the title compound was confirmed by NMR, IR, elemental analysis and single-crystal X-ray diffraction. It crystallizes in orthorhombic, space group P21/c with a = 10.739(2), b = 6.4765(12), c = 14.138(3) A, fl= 108.787(3)°, V= 930.9(3) A3, Z = 1, Mr= 486.36, Dc = 1.735 g.cm3, μ= 0.15 mm-1, F(000) = 496, R = 0.042 and wR = 0.121. The thermal stability was analyzed by subsequently differential scanning calorimetry (DSC). And the enthalpy of formation and detonation was calculated theoretically, showing the first decomposition temperature was 142.1℃, the enthalpy of formation was 1614.23 kJ.mol1 and the detonation velocity and detonation pressure were 8.781 km.s-1 and 30.7 GPa, respectively.展开更多
A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single...A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single-crystal X-ray diffraction,elementary analysis,IR spectroscopy,thermogravimetric analysis and X-ray powder diffraction. Single-crystal X-ray diffraction indicates that the complex belongs to triclinic system,space group P 1 with a = 10.0911(1),b = 10.2573(1),c = 10.6393(1) ?,α = 103.793(2),β = 101.041(2),γ = 107.918(3)o,V = 974.9(2) ?~3,Z = 2,D_c = 1.732 g·cm-3,μ = 0.941 mm^(-1),M_r = 508.31,F(000) = 518,the final R = 0.0523 and wR = 0.0935 with I 〉 2σ(I). In the title complex,Co(Ⅱ) ions are connected by Htm2-anions generating 1D ladder-like chains which are linked by 3,3?-Hbpt to form 1D cages. In addition,the thermal decomposition of ammonium perchlorate(AP) with complex 1 was explored by differential scanning calorimetry(DSC). AP is completely decomposed in a shorter time in the presence of complex 1,and the decomposition heat of the mixture is 2.531 kJ·g^(-1),significantly higher than that of pure AP. By Kissinger's method,the ratio of Ea/ln(A) is 11.05 for the mixture,which indicates that complex 1 shows good catalytic activity toward the AP decomposition.展开更多
One novel nickel coordination polymer, {[Ni(OTP)(bib)1.5(H2O)]·2H2O}n(1, H2 OTP = 2-hydroxy-5-(3',5'-terephthalic acid) pyridine, bib = 1,4-bis(1-imdazoly)benzene), has been synthesized and characte...One novel nickel coordination polymer, {[Ni(OTP)(bib)1.5(H2O)]·2H2O}n(1, H2 OTP = 2-hydroxy-5-(3',5'-terephthalic acid) pyridine, bib = 1,4-bis(1-imdazoly)benzene), has been synthesized and characterized by elemental analysis(EA), IR, powder X-ray diffraction(PXRD), and thermogravimetric(TG) analyses. The crystal of 1 crystallizes in monoclinic, space group P21/n with a = 12.2860(5), b = 13.8246(6), c = 19.0140(8) A, β = 104.3870(1)°, V = 3128.2(2) A3, Z = 4, C32H28N7 Ni O8, Mr = 697.32, Dc = 1.481 g/cm^3, F(000) = 1444 and μ(Mo Kα) = 0.684 mm-1. The final R = 0.0704 and w R = 0.1764 for 5485 observed reflections with I 2σ(I) and R = 0.1087 and wR = 0.2010 for all data. Topology analysis reveals that complex 1 is a 3D 2-fold interpenetrated {4^4·6^6}-nov net based on the 1D [Ni(OTP)]n chain and the 2D [Ni2(bib)3]n sql sheet. And the variable-temperature magnetic susceptibility measurements exhibit weak antiferromagnetic coupling interaction.展开更多
Sodium 3,5-bis(hydroxyimino)-1-methyl-2,4,6-trioxocyclohexanide C7H5N2NaO5 (I) has been isolated as the only product of the reaction of nitrosation of methylphloroglucinol. The structure of the titled compound has bee...Sodium 3,5-bis(hydroxyimino)-1-methyl-2,4,6-trioxocyclohexanide C7H5N2NaO5 (I) has been isolated as the only product of the reaction of nitrosation of methylphloroglucinol. The structure of the titled compound has been determined from single crystal X-ray diffraction data. The hydrated C7H5N2NaO52.5H2O crystallizes in the monoclinic space group C2/c, with a(?) 16.408(3);b(?) 12.446(3);c(?) 13.716(3);(o) 126.34(3). The planar organic anion exists in a triketo-dihydroxyimino form with the C–O and C–N distances from 1.220(2) to 1.271(2)?? and from 1.292(2) to 1.293?? respectively. In the IR spectrum of I, the sharp absorption band occurred at 1681 cm-1 due to C=O stretching indicating the strong H-interactions. The correlations of theoretical (DFT-B3LYP/aug-cc-pVDZ) and experimental UV-vis absorption spectra in neutral and alkaline ethanolic solutions showed the existence of hydroxyimino-nitroso tautomerism while ionization of I.展开更多
Two new coordination polymers,[Zn(bdc)(1,3-bimb)]n(1) and {[Mn2(ox)2(1,3,5tib)4/3]·4H2O}n(2)(H2ox = oxalic acid,H2bdc = terephthalic acid,1,3-bimb = 1,3-bis(imidazol-1ylmethyl)benzene,1,3,5-tib = 1...Two new coordination polymers,[Zn(bdc)(1,3-bimb)]n(1) and {[Mn2(ox)2(1,3,5tib)4/3]·4H2O}n(2)(H2ox = oxalic acid,H2bdc = terephthalic acid,1,3-bimb = 1,3-bis(imidazol-1ylmethyl)benzene,1,3,5-tib = 1,3,5-tri(imidazol-1-yl)benzene),were synthesized and characterized by elemental analysis,IR,powder X-ray diffraction(PXRD),and thermogravimetric(TG) analyses.X-ray diffracation analysis reveals that two kinds of zigzag chains [Zn(bdc)]n and [Zn(1,3-bimb)]n in compound 1 are interweaved to form a 3D 4-fold interpenetrated 66-dia framework.In compound 2,Mn(1) and Mn(2) are linked via 1,3,5-tib ligands to form two different nets of [Mn6(1,3,5-tib)6 ]n along the ab plane with inner-or outer-shape N–Mn–N angles,which are connected by 1D infinite [Mn2(ox)2 ]n chains via Mn–O bonds to result in a(3,3,3,4,4)-connected(4·8·10)3(4·82)3(4·83·102)6(82·104·3)3(83)4 topology.Moreover,the photoluminescence of 1 has been investigated.The crystal of 1 crystallizes in orthorhombic,space group Pna2 with a = 13.2267(6),b = 9.1717(4),c = 17.4492(8),V = 2116.79(16)3,Z = 4,C22 H18N4O4 Zn,Mr = 467.77,Dc = 1.468 g/cm3,F(000) = 960 and μ(MoKα) = 1.197 mm-1.The final R = 0.0280 and wR = 0.0618 for 3695 observed reflections with I 2(I) and R = 0.0389 and wR = 0.0653 for all data.The crystal of 2 crystallizes in rhombohedral,space group R-3 with a = 22.080(8),c = 31.19(2),V = 13167(11) 3,Z = 18,C24 H25 Mn2 N8 O13,Mr = 743.40,Dc = 1.688 g/cm3,F(000) = 6822 and μ(MoKα) = 0.945 mm-1.The final R = 0.0429 and wR = 0.1035 for 5160 observed reflections with I 2(I) and R = 0.0824 and wR = 0.1244 for all data.展开更多
Hydrothermal reactions of three aromatic polycarboxylic acids and the transitional metal cations in the presence of phen and 1,4-bib afford three new coordination polymers: [Cd2(bpp)1.5(Hbpp)(phen)2]n (1), [...Hydrothermal reactions of three aromatic polycarboxylic acids and the transitional metal cations in the presence of phen and 1,4-bib afford three new coordination polymers: [Cd2(bpp)1.5(Hbpp)(phen)2]n (1), [Mn3(Htptc)2(phen)2(H2O)2]n (2), and {[Cu(btc)0.5(1,4- bib)]·2H2O}n(3) (H2bpp = 2,6-bis(4'-carboxyphenyl)-4-phenylpyridine, H4tptc = terphenyl-2,5,2',5'-tetracar- boxylic acid, H4btc =biphenyl-2,2',4,4'-tetracarboxylic acid, phen =1,10-phenanthroline, and 1,4-bib = 1,4-bis(1H-imidazol-1-yl)benzene). Their structures have been determined by single- crystal X-ray diffraction analyses, elemental analyses, IR spectra, and powder X-ray diffraction (PXRD) analyses. In compound 1, the CdII cations are linked by bpp2- to form one ladder structure, based on which a 3D network is constructed with the help of non-covalent interactions. The topology of 2 is a 3D (3,4,5)-connected framework with the Point Schl?fli symbol of (42.6)2(43.62.8)(45.64.8)2. Compound 3 shows an unprecedented 3D (4,4)-connected framework with the Point Schl?fli symbol of (64.82)2(65.8). Moreover, the luminescent property of 1 has been investigated.展开更多
A Zn(Ⅱ) supramolecular coordination polymer, {[Zn2(L)2(m-bix)(H20)]6H2O}n(1), with an interesting 1D→2D polythreading array from a flexible and angular organic aromaticpolycarboxylate ligand 5-(4-hydroxyp...A Zn(Ⅱ) supramolecular coordination polymer, {[Zn2(L)2(m-bix)(H20)]6H2O}n(1), with an interesting 1D→2D polythreading array from a flexible and angular organic aromaticpolycarboxylate ligand 5-(4-hydroxypyridinium-l-ylmethyl)isophthalic acid (H2L), and N-donorligand 1,3-bis(imidazol-l-ylmethyl)benzene (m-bix), has been obtained under hydrothermalconditions and characterized by elemental analysis, powder X-ray diffraction (PXRD), IR, thermalgravimetric analyses (TGA) and single-crystal X-ray diffraction. In 1, the Zn(Ⅱ) center has twocoordination geometries. One exhibits a trigonal bipyramidal coordination sphere, and the other isa tetrahedral geometry; L2- has two different coordination modes, with one connecting three Zn(Ⅱ)ions through two monodentate carboxylate groups and the monodentate hydroxyl group, and theother bridging two Zn(Ⅱ) ions through two carboxylate groups. The L2- anions connect the Zn(Ⅱ)centers forming an infinite 1D tubular structure. These 1D tubes are interconnected by the m-bixspacers to form a 2D framework. Such 2D layers are further assembled into a 3D supramolecularnetwork via hydrogen bonds. Meanwhile, the luminescent property of 1 has also been investigatedin detail.展开更多
The ring-and side-chain-<sup>14</sup>C-labeled probimane, 1,2-bis (4-morpholinomethy1-3,5-dioxopiperazin-1-yl) propane were synthesized from acetic acid-1-<sup>14</sup>C in 4 steps and from &...The ring-and side-chain-<sup>14</sup>C-labeled probimane, 1,2-bis (4-morpholinomethy1-3,5-dioxopiperazin-1-yl) propane were synthesized from acetic acid-1-<sup>14</sup>C in 4 steps and from <sup>14</sup>C-formaldehyde in 1 step respectively. The radiochemical yeild for the ring labeling was 28.1%; for the side-chain labeling was 18.5%.展开更多
Three energetic ion salts of 3,6-bis[(1H-1,2,3,4-tetrazol-5-yl)-amino]-1,2,4,5-tetrazine(BTATz), namely, methylamine salt(compound 1), ethylenediamine salt(compound 2), and diethylamine salt(compound 3), were synthesi...Three energetic ion salts of 3,6-bis[(1H-1,2,3,4-tetrazol-5-yl)-amino]-1,2,4,5-tetrazine(BTATz), namely, methylamine salt(compound 1), ethylenediamine salt(compound 2), and diethylamine salt(compound 3), were synthesized and characterized by elemental analysis, Fourier transform infrared spectrometry, NMR spectroscopy, and ^13C NMR spectroscopy. The crystal structure of compound 1 was determined by single-crystal X-ray crystallography, and structural analysis revealed that it belonged to the monoclinic system with P21/c space group. In addition, the thermal behavior of the three compounds was studied by differential scanning calorimetry and thermogravimetry techniques. The thermal decomposition peak temperatures of the compounds were 574.89, 545.60, and 606.72 K, indicating that the three ion salts exhibited good thermal stability. Tlie kinetic mechanism equations of the main decomposition process and the entropy of activation(△S^≠), enthalpy of activation(△H^≠), and Gibbs free energy of activation(△G^≠) of the three compounds were also obtained. Moreover, the thermal safety of the compounds was evaluated by the values of the self^accelerated decomposition temperature(Tsadt)5 thermal ignition temperature(TTIT), and critical temperature of thermal explosion(7b). The results showed that all the compounds demonstrated good thermal safety, and the thermal safety of compound 3 was better than that of the others.展开更多
A new coordination polymer [Ni(L)(m-bix)(H2O)]n (1, H2L = 5-iodo-isophthalic acid, m-bix=1,3-bis(imidazol-1-ylmethyl)-benzene) has been synthesized by the hydrothermal method and characterized by IR, element...A new coordination polymer [Ni(L)(m-bix)(H2O)]n (1, H2L = 5-iodo-isophthalic acid, m-bix=1,3-bis(imidazol-1-ylmethyl)-benzene) has been synthesized by the hydrothermal method and characterized by IR, elemental analysis, powder XRD and single-crystal X-ray analysis. The crystal is of triclinic, space group Pī with a = 9.1638(3), b = 10.2319(3), c = 13.2463(4) ?, α = 80.1710(10), β = 83.671(2), γ = 70.3790(10)o,C22H19NiIN4O5, Mr = 605.02, V = 1150.85(6) ?3, Dc = 1.746 g/cm3, F(000) = 600, μ = 2.225 mm-1, S = 1.045 and Z = 2. The final R = 0.0388 and wR = 0.1257 for 5089 observed reflections with I 〉 2σ(I). In the title complex, the M and P layers are arranged alternately to give a double-layer structure by the symmetry related hydrogen bonds, and these double-layers are further joined together to achieve a 2D supramolecular architecture through I···π interaction involving iodine atoms and imidazole rings. The thermal stability of the title complex was studied by thermal gravimetric (TG) and differential thermal analysis (DTA).展开更多
Two novel energetic alkalic metal salts of 3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-l,2,4,5-tetrazine (BTATz), Li2(BTATz). 6H20(compound 1) and Na2(BTATz). 2H20(compound 2), have been synthesized by the rea...Two novel energetic alkalic metal salts of 3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-l,2,4,5-tetrazine (BTATz), Li2(BTATz). 6H20(compound 1) and Na2(BTATz). 2H20(compound 2), have been synthesized by the reac- tion of BTATz with lithinnl hydroxide or sodium hydroxide in dimethylsulfoxide(DMSO) solution, respectively, and their structures were characterized by means of elemental analysis and Fourier transform infrared spectrometry(FTIR) Moreover, the single-crystal structure of compound 1 was determined by single crystal X-ray diffraction. It crystal- lizes in the monoclinic space group P1/c. Furthermore, their thermal decomposition behaviors were investigated by means of differential scanning calorimetry(DSC) and thermogravimetry-differential thermal gravimetry(TG-DTG). The results show that the exothermic decomposition peak temperatures for compounds 1 and 2 were 642.65 and 644.46 K, respectively, and the kinetic equations of the main exothermic decomposition were also derived from non-isothermal method. Additionally, the thermal safety of the two compounds was evaluated by calculating self-accelerating decomposition temperature(TSADT) and critical temperature of thermal explosion(Tb). The results(the TSADT and Tb values are 605.43 and 635.69 K for compound 1; 607.38 and 638.96 K for compound 2) reveal that the two compounds exhibit better thermal safety than BTATz.展开更多
A new Cu(Ⅱ) metal-organic coordination polymer, {[Cu2(tbip)2(bie)2]·H2O}n (1, H2tbip = 5-tert-butyl isophthalic acid, bie = 1,2-bis(imidazol-1 '-yl)ethane), was assembled under hydrothermal conditions...A new Cu(Ⅱ) metal-organic coordination polymer, {[Cu2(tbip)2(bie)2]·H2O}n (1, H2tbip = 5-tert-butyl isophthalic acid, bie = 1,2-bis(imidazol-1 '-yl)ethane), was assembled under hydrothermal conditions by the reactions of Cu(Ⅱ) acetate with H2tbip and bie. Complex 1 was characterized by elemental analysis, IR spectroscopy and X-ray single-crystal diffraction. Complex 1 crystallizes in triclinic, space group P1, with a = 9.9145(10), b = 13.2211(13), c = 15.4363(15) nm, a = 87.0250(10), β = 88.3220(10), γ = 83.8240(10)°, V= 2008.4(3) nm3, Z = 2, Dc = 1.505 Mg/m3, F(000) = 944, g = 1.125 mm^-1, S = 1.030, the final R = 0.0336 and wR = 0.0790. The results reveal that complex 1 is a two-dimensional layered structure. In addition, magnetic properties of I were also investigated.展开更多
A new coordination compound, [Co(L223)2(H2O)2]·H2pm(1, L223 = 3,4-bis(2-pyridyl)-5-(3-pyridyl)-1,2,4-triazole and H4 pm = pyromellitic acid), has been synthesized. The structure of complex 1 has been ch...A new coordination compound, [Co(L223)2(H2O)2]·H2pm(1, L223 = 3,4-bis(2-pyridyl)-5-(3-pyridyl)-1,2,4-triazole and H4 pm = pyromellitic acid), has been synthesized. The structure of complex 1 has been characterized by X-ray single-crystal diffraction, elemental analysis, IR spectrum analysis and thermogravimetric analysis. Single-crystal X-ray diffraction analysis reveals that complex 1 belongs to the triclinic system, space group P1 with a = 10.2470(8), b = 10.2879(9), c = 10.2951(11) ?, α = 109.398(2), β = 97.6590(10), γ = 95.3260(10)°, V = 1003.60(16) ?3, Z = 1, Dc = 1.565 g/cm^3, μ = 0.508 mm%^-1, Mr = 945.73, F(000) = 485, the final R = 0.0562 and w R = 0.0783 with I 〉 2σ(I). Two L223 as chelating ligands link one Co(II) ion to form a 0D motif. Furthermore, the 0D motifs are linked into a 2D coordination pattern with hydrogen bonds. In addition, the antifungal effects of the ligand and the complex were evaluated by the disc diffusion method against Colletotrichum gloeosporioides Penz. 1 represents antifungal activity with high levels of inhibitory potency which is larger than the corresponding ligand.展开更多
Three new cobalt(II) coordination compounds, [Co(3,3'-Hbpt)2(H2pm)(H20)2]'2H20 (1), [Co(4,4'-Hbpt)(pm)0.5(H20)]'3H20 (2) and [Co(3,4'-Hbpt)(pm)0.5(H20)3]'2H20 (3) (3,3'-Hbpt = 3,5-bis...Three new cobalt(II) coordination compounds, [Co(3,3'-Hbpt)2(H2pm)(H20)2]'2H20 (1), [Co(4,4'-Hbpt)(pm)0.5(H20)]'3H20 (2) and [Co(3,4'-Hbpt)(pm)0.5(H20)3]'2H20 (3) (3,3'-Hbpt = 3,5-bis(3-pyridyl)-lH-1,2,4-triazole; 4,4'-bpt = 3,5-bis(4-pyridyl)- 1H-1,2,4-triazole, 3,4'-Hbpt = 3-(3-pyridyl)-5-(4'-pyridyl)-lH-1,2,4-triazole and Hapm = pyromellitic acid) have been synthe- sized by hydrothermal reactions. Single-crystal X-ray diffraction reveals that compound 1 has a one-dimensional (1D) chain network, 2 exhibits a four-connected three-dimensional (3D) structure with 1D open channels encapsulated by water molecules, while 3 displays a regular two-dimensional (2D) architecture connected through 1D metal helical chains. In addition, the effi- cacy of compounds 1-3 as additives to promote the thermal decomposition of ammonium perchlorate (AP) is explored by dif- ferential scanning calorimetry (DSC).展开更多
A new high-energy organic magnesium salt [Mg(H2O)6](BTATz)·2H2O[BTATz=3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-1,2,4,5-tetrazine] was synthesized and characterized by elemental analysis and Fourier transform...A new high-energy organic magnesium salt [Mg(H2O)6](BTATz)·2H2O[BTATz=3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-1,2,4,5-tetrazine] was synthesized and characterized by elemental analysis and Fourier transform infrared(FTIR) spectrometry.Its crystal structure was determined by X-ray single crystal diffraction.The crystal belongs to monoclinic system with space group C2/c and a=2.1329(7) nm,b=0.52275(16) nm,c=1.5909(5) nm,β=100.471(6)°,V=1.7443(9) nm3,Z=4,μ=0.361 mm-1,F(000)=900 and Dc=1.644 g/cm3.Meanwhile,the thermal behavior of [Mg(H2O)6](BTATz)·2H2O was studied under the non-isothermal conditions by differential scanning calorimetry(DSC) and thermalgravity-differential thermalgravity(TG-DTG) methods.The enthalpy,apparent activation energy and per-exponential factor of the main exothermic decomposition reaction are 898.88 J/g,139.2 kJ/mol and 1010.48 S-1,respectively.The values of the self-accelerating decomposition temperature(TsADT),the thermal ignition temperature(TTIT) and the critical temperature of thermal explosion(Tb) for [Mg(H2O)6](BTATz).2H2O are 515.13,532.08 and 565.99 K,respectively.展开更多
Thermally activated delayed fluorescence(TADF)organic light-emitting diodes(OLEDs)have been demonstrated in applications such as displays and solid-state lightings.However,weak stability and ineffi-cient emission of b...Thermally activated delayed fluorescence(TADF)organic light-emitting diodes(OLEDs)have been demonstrated in applications such as displays and solid-state lightings.However,weak stability and ineffi-cient emission of blue TADF OLEDs are two key bottlenecks limiting the development of solution processable displays and white light sources.This work presents a solution-processed OLED using a blue-emitting TADF small molecule bis[4-(9,9-dimethyl-9,10-dihydroacridine)phenyl]sulfone(DMAC-DPS)as an emitter.We comparatively investigated the effects of single host poly(Nvinylcarbazole)(PVK)and a co-host of 60%PVK and 30%2,2′-(1,3-phenylene)-bis[5-(4-tert-butylphenyl)-1,3,4-oxadiazole](OXD-7)on the device performance(the last 10%is emitter DMAC-DPS).The co-host device shows lower turn-on voltage,similar maximum luminance,and much slower external quantum efficiency(EQE)rolloff.In other words,device stability improved by doping OXD-7 into PVK,and the device impedance simultaneously and significantly reduced from 8.6103 to 4.2103 W at 1000 Hz.Finally,the electroluminescent stability of the co-host device was significantly enhanced by adjusting the annealing temperature.展开更多
基金Supported by Indian Council of Medical Research and Department of Biotechnology,Government of India
文摘AIM:To study the mechanism of 5-fluorouracil(5-FU)resistance in colon cancer cells and to develop strategies for overcoming such resistance by combination treatment.METHODS:We established and characterized a 5-FU resistance(5-FU-R)cell line derived from continuous exposure(25μmol/L)to 5-FU for 20 wk in 5-FU sensitive HCT-116 cells.The proliferation and expression of different representative apoptosis and anti-apoptosis markers in 5-FU sensitive and 5-FU resistance cells were measured by the MTT assay and by Western blotting,respectively,after treatment with Resveratrol(Res)and/or 1,3-Bis(2-chloroethyl)-1-nitrosourea(BCNU).Apoptosis and cell cycle arrest was measured by 4',6'-diamidino-2-phenylindole hydrochloride staining and fluorescence-activated cell sorting analysis,respectively.The extent of DNA damage was measured by the Comet assay.We measured the visible changes in the DNA damage/repair cascade by Western blotting.RESULTS:The widely used chemotherapeutic agents BCNU and Res decreased the growth of 5-FU sensitive HCT-116 cells in a dose dependent manner.Combined application of BCNU and Res caused more apoptosis in5-FU sensitive cells in comparison to individual treatment.In addition,the combined application of BCNU and Res caused a significant decrease of major DNA base excision repair components in 5-FU sensitive cells.We established a 5-FU resistance cell line(5-FU-R)from 5-FU-sensitive HCT-116(mismatch repair deficient)cells that was not resistant to other chemotherapeutic agents(e.g.,BCNU,Res)except 5-FU.The 5-FU resistance of 5-FU-R cells was assessed by exposure to increasing concentrations of 5-FU followed by the MTT assay.There was no significant cell death noted in5-FU-R cells in comparison to 5-FU sensitive cells after5-FU treatment.This resistant cell line overexpressed anti-apoptotic[e.g.,AKT,nuclear factorκB,FLICE-like inhibitory protein),DNA repair(e.g.,DNA polymerase beta(POL-β),DNA polymerase eta(POLH),protein Flap endonuclease 1(FEN1),DNA damage-binding protein 2(DDB2)]and 5-FU-resistance proteins(thymidylate synthase)but under expressed pro-apoptotic proteins(e.g.,DAB2,CK1)in comparison to the parental cells.Increased genotoxicity and apoptosis were observed in resistant cells after combined application of BCNU and Res in comparison to untreated or parental cells.BCNU increased the sensitivity to Res of 5-FU resistant cells compared with parental cells.Fifty percent cell death were noted in parental cells when 18μmol/L of Res was associated with fixed concentration(20μmol/L)of BCNU,but a much lower concentration of Res(8μmol/L)was needed to achieve the same effect in 5-FU resistant cells.Interestingly,increased levels of adenomatous polyposis coli and decreased levels POL-β,POLH,FEN1 and DDB2 were noted after the same combined treatment in resistant cells.CONCLUSION:BCNU combined with Res exerts a synergistic effect that may prove useful for the treatment of colon cancer and to overcome drug resistance.
文摘An energetic salt of bis(l,5-diamino-lH-tetrazolium)3,3"-bis(nitramino)-4, 4x-azo- furazan (C6H10N2206) was synthesized with the total yield of 61.7% by using 3,4-diaminofurazan (DAF) as the starting material. The structure of the title compound was confirmed by NMR, IR, elemental analysis and single-crystal X-ray diffraction. It crystallizes in orthorhombic, space group P21/c with a = 10.739(2), b = 6.4765(12), c = 14.138(3) A, fl= 108.787(3)°, V= 930.9(3) A3, Z = 1, Mr= 486.36, Dc = 1.735 g.cm3, μ= 0.15 mm-1, F(000) = 496, R = 0.042 and wR = 0.121. The thermal stability was analyzed by subsequently differential scanning calorimetry (DSC). And the enthalpy of formation and detonation was calculated theoretically, showing the first decomposition temperature was 142.1℃, the enthalpy of formation was 1614.23 kJ.mol1 and the detonation velocity and detonation pressure were 8.781 km.s-1 and 30.7 GPa, respectively.
基金Supported by the National Natural Science Foundation of China(No.21263019 and 21467022)
文摘A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single-crystal X-ray diffraction,elementary analysis,IR spectroscopy,thermogravimetric analysis and X-ray powder diffraction. Single-crystal X-ray diffraction indicates that the complex belongs to triclinic system,space group P 1 with a = 10.0911(1),b = 10.2573(1),c = 10.6393(1) ?,α = 103.793(2),β = 101.041(2),γ = 107.918(3)o,V = 974.9(2) ?~3,Z = 2,D_c = 1.732 g·cm-3,μ = 0.941 mm^(-1),M_r = 508.31,F(000) = 518,the final R = 0.0523 and wR = 0.0935 with I 〉 2σ(I). In the title complex,Co(Ⅱ) ions are connected by Htm2-anions generating 1D ladder-like chains which are linked by 3,3?-Hbpt to form 1D cages. In addition,the thermal decomposition of ammonium perchlorate(AP) with complex 1 was explored by differential scanning calorimetry(DSC). AP is completely decomposed in a shorter time in the presence of complex 1,and the decomposition heat of the mixture is 2.531 kJ·g^(-1),significantly higher than that of pure AP. By Kissinger's method,the ratio of Ea/ln(A) is 11.05 for the mixture,which indicates that complex 1 shows good catalytic activity toward the AP decomposition.
基金supported by the Natural Science Foundation of Shandong Province(ZR2011BL020,ZR2012CM019)National Natural Science Foundation of China(21451001)Key Discipline and Innovation Team of Qilu Normal University
文摘One novel nickel coordination polymer, {[Ni(OTP)(bib)1.5(H2O)]·2H2O}n(1, H2 OTP = 2-hydroxy-5-(3',5'-terephthalic acid) pyridine, bib = 1,4-bis(1-imdazoly)benzene), has been synthesized and characterized by elemental analysis(EA), IR, powder X-ray diffraction(PXRD), and thermogravimetric(TG) analyses. The crystal of 1 crystallizes in monoclinic, space group P21/n with a = 12.2860(5), b = 13.8246(6), c = 19.0140(8) A, β = 104.3870(1)°, V = 3128.2(2) A3, Z = 4, C32H28N7 Ni O8, Mr = 697.32, Dc = 1.481 g/cm^3, F(000) = 1444 and μ(Mo Kα) = 0.684 mm-1. The final R = 0.0704 and w R = 0.1764 for 5485 observed reflections with I 2σ(I) and R = 0.1087 and wR = 0.2010 for all data. Topology analysis reveals that complex 1 is a 3D 2-fold interpenetrated {4^4·6^6}-nov net based on the 1D [Ni(OTP)]n chain and the 2D [Ni2(bib)3]n sql sheet. And the variable-temperature magnetic susceptibility measurements exhibit weak antiferromagnetic coupling interaction.
文摘Sodium 3,5-bis(hydroxyimino)-1-methyl-2,4,6-trioxocyclohexanide C7H5N2NaO5 (I) has been isolated as the only product of the reaction of nitrosation of methylphloroglucinol. The structure of the titled compound has been determined from single crystal X-ray diffraction data. The hydrated C7H5N2NaO52.5H2O crystallizes in the monoclinic space group C2/c, with a(?) 16.408(3);b(?) 12.446(3);c(?) 13.716(3);(o) 126.34(3). The planar organic anion exists in a triketo-dihydroxyimino form with the C–O and C–N distances from 1.220(2) to 1.271(2)?? and from 1.292(2) to 1.293?? respectively. In the IR spectrum of I, the sharp absorption band occurred at 1681 cm-1 due to C=O stretching indicating the strong H-interactions. The correlations of theoretical (DFT-B3LYP/aug-cc-pVDZ) and experimental UV-vis absorption spectra in neutral and alkaline ethanolic solutions showed the existence of hydroxyimino-nitroso tautomerism while ionization of I.
基金Supported by the National Natural Science Foundation of China(20873150)Natural Science Foundation of Shandong Province(ZR2010BQ023)
文摘Two new coordination polymers,[Zn(bdc)(1,3-bimb)]n(1) and {[Mn2(ox)2(1,3,5tib)4/3]·4H2O}n(2)(H2ox = oxalic acid,H2bdc = terephthalic acid,1,3-bimb = 1,3-bis(imidazol-1ylmethyl)benzene,1,3,5-tib = 1,3,5-tri(imidazol-1-yl)benzene),were synthesized and characterized by elemental analysis,IR,powder X-ray diffraction(PXRD),and thermogravimetric(TG) analyses.X-ray diffracation analysis reveals that two kinds of zigzag chains [Zn(bdc)]n and [Zn(1,3-bimb)]n in compound 1 are interweaved to form a 3D 4-fold interpenetrated 66-dia framework.In compound 2,Mn(1) and Mn(2) are linked via 1,3,5-tib ligands to form two different nets of [Mn6(1,3,5-tib)6 ]n along the ab plane with inner-or outer-shape N–Mn–N angles,which are connected by 1D infinite [Mn2(ox)2 ]n chains via Mn–O bonds to result in a(3,3,3,4,4)-connected(4·8·10)3(4·82)3(4·83·102)6(82·104·3)3(83)4 topology.Moreover,the photoluminescence of 1 has been investigated.The crystal of 1 crystallizes in orthorhombic,space group Pna2 with a = 13.2267(6),b = 9.1717(4),c = 17.4492(8),V = 2116.79(16)3,Z = 4,C22 H18N4O4 Zn,Mr = 467.77,Dc = 1.468 g/cm3,F(000) = 960 and μ(MoKα) = 1.197 mm-1.The final R = 0.0280 and wR = 0.0618 for 3695 observed reflections with I 2(I) and R = 0.0389 and wR = 0.0653 for all data.The crystal of 2 crystallizes in rhombohedral,space group R-3 with a = 22.080(8),c = 31.19(2),V = 13167(11) 3,Z = 18,C24 H25 Mn2 N8 O13,Mr = 743.40,Dc = 1.688 g/cm3,F(000) = 6822 and μ(MoKα) = 0.945 mm-1.The final R = 0.0429 and wR = 0.1035 for 5160 observed reflections with I 2(I) and R = 0.0824 and wR = 0.1244 for all data.
基金supported by the National Natural Science Foundation of China(20873150)the Natural Science Foundation of Shandong Province(ZR2010BL012,ZR2010BQ023)
文摘Hydrothermal reactions of three aromatic polycarboxylic acids and the transitional metal cations in the presence of phen and 1,4-bib afford three new coordination polymers: [Cd2(bpp)1.5(Hbpp)(phen)2]n (1), [Mn3(Htptc)2(phen)2(H2O)2]n (2), and {[Cu(btc)0.5(1,4- bib)]·2H2O}n(3) (H2bpp = 2,6-bis(4'-carboxyphenyl)-4-phenylpyridine, H4tptc = terphenyl-2,5,2',5'-tetracar- boxylic acid, H4btc =biphenyl-2,2',4,4'-tetracarboxylic acid, phen =1,10-phenanthroline, and 1,4-bib = 1,4-bis(1H-imidazol-1-yl)benzene). Their structures have been determined by single- crystal X-ray diffraction analyses, elemental analyses, IR spectra, and powder X-ray diffraction (PXRD) analyses. In compound 1, the CdII cations are linked by bpp2- to form one ladder structure, based on which a 3D network is constructed with the help of non-covalent interactions. The topology of 2 is a 3D (3,4,5)-connected framework with the Point Schl?fli symbol of (42.6)2(43.62.8)(45.64.8)2. Compound 3 shows an unprecedented 3D (4,4)-connected framework with the Point Schl?fli symbol of (64.82)2(65.8). Moreover, the luminescent property of 1 has been investigated.
基金supported by Education Chamber of Henan Province(No.15A150068)
文摘A Zn(Ⅱ) supramolecular coordination polymer, {[Zn2(L)2(m-bix)(H20)]6H2O}n(1), with an interesting 1D→2D polythreading array from a flexible and angular organic aromaticpolycarboxylate ligand 5-(4-hydroxypyridinium-l-ylmethyl)isophthalic acid (H2L), and N-donorligand 1,3-bis(imidazol-l-ylmethyl)benzene (m-bix), has been obtained under hydrothermalconditions and characterized by elemental analysis, powder X-ray diffraction (PXRD), IR, thermalgravimetric analyses (TGA) and single-crystal X-ray diffraction. In 1, the Zn(Ⅱ) center has twocoordination geometries. One exhibits a trigonal bipyramidal coordination sphere, and the other isa tetrahedral geometry; L2- has two different coordination modes, with one connecting three Zn(Ⅱ)ions through two monodentate carboxylate groups and the monodentate hydroxyl group, and theother bridging two Zn(Ⅱ) ions through two carboxylate groups. The L2- anions connect the Zn(Ⅱ)centers forming an infinite 1D tubular structure. These 1D tubes are interconnected by the m-bixspacers to form a 2D framework. Such 2D layers are further assembled into a 3D supramolecularnetwork via hydrogen bonds. Meanwhile, the luminescent property of 1 has also been investigatedin detail.
文摘The ring-and side-chain-<sup>14</sup>C-labeled probimane, 1,2-bis (4-morpholinomethy1-3,5-dioxopiperazin-1-yl) propane were synthesized from acetic acid-1-<sup>14</sup>C in 4 steps and from <sup>14</sup>C-formaldehyde in 1 step respectively. The radiochemical yeild for the ring labeling was 28.1%; for the side-chain labeling was 18.5%.
基金the National Natural Science Foundation of China(No.21673179)the Key-point Natural Science Foundation of Shaanxi Province,China(No.2016JZ003)the Graduate Innovation and Creativity Funds of Northwest University, China (No.YZZ17137).
文摘Three energetic ion salts of 3,6-bis[(1H-1,2,3,4-tetrazol-5-yl)-amino]-1,2,4,5-tetrazine(BTATz), namely, methylamine salt(compound 1), ethylenediamine salt(compound 2), and diethylamine salt(compound 3), were synthesized and characterized by elemental analysis, Fourier transform infrared spectrometry, NMR spectroscopy, and ^13C NMR spectroscopy. The crystal structure of compound 1 was determined by single-crystal X-ray crystallography, and structural analysis revealed that it belonged to the monoclinic system with P21/c space group. In addition, the thermal behavior of the three compounds was studied by differential scanning calorimetry and thermogravimetry techniques. The thermal decomposition peak temperatures of the compounds were 574.89, 545.60, and 606.72 K, indicating that the three ion salts exhibited good thermal stability. Tlie kinetic mechanism equations of the main decomposition process and the entropy of activation(△S^≠), enthalpy of activation(△H^≠), and Gibbs free energy of activation(△G^≠) of the three compounds were also obtained. Moreover, the thermal safety of the compounds was evaluated by the values of the self^accelerated decomposition temperature(Tsadt)5 thermal ignition temperature(TTIT), and critical temperature of thermal explosion(7b). The results showed that all the compounds demonstrated good thermal safety, and the thermal safety of compound 3 was better than that of the others.
基金supported by the International Technology Cooperation Project of Science and Technology Department of Henan Province(No.124300510050)
文摘A new coordination polymer [Ni(L)(m-bix)(H2O)]n (1, H2L = 5-iodo-isophthalic acid, m-bix=1,3-bis(imidazol-1-ylmethyl)-benzene) has been synthesized by the hydrothermal method and characterized by IR, elemental analysis, powder XRD and single-crystal X-ray analysis. The crystal is of triclinic, space group Pī with a = 9.1638(3), b = 10.2319(3), c = 13.2463(4) ?, α = 80.1710(10), β = 83.671(2), γ = 70.3790(10)o,C22H19NiIN4O5, Mr = 605.02, V = 1150.85(6) ?3, Dc = 1.746 g/cm3, F(000) = 600, μ = 2.225 mm-1, S = 1.045 and Z = 2. The final R = 0.0388 and wR = 0.1257 for 5089 observed reflections with I 〉 2σ(I). In the title complex, the M and P layers are arranged alternately to give a double-layer structure by the symmetry related hydrogen bonds, and these double-layers are further joined together to achieve a 2D supramolecular architecture through I···π interaction involving iodine atoms and imidazole rings. The thermal stability of the title complex was studied by thermal gravimetric (TG) and differential thermal analysis (DTA).
基金Supported by the National Natural Science Foundation of China(Nos.21101127, 21673179) and the National Defense Pre-Research Foundation of China(No.9140A28020111BQ3401).
文摘Two novel energetic alkalic metal salts of 3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-l,2,4,5-tetrazine (BTATz), Li2(BTATz). 6H20(compound 1) and Na2(BTATz). 2H20(compound 2), have been synthesized by the reac- tion of BTATz with lithinnl hydroxide or sodium hydroxide in dimethylsulfoxide(DMSO) solution, respectively, and their structures were characterized by means of elemental analysis and Fourier transform infrared spectrometry(FTIR) Moreover, the single-crystal structure of compound 1 was determined by single crystal X-ray diffraction. It crystal- lizes in the monoclinic space group P1/c. Furthermore, their thermal decomposition behaviors were investigated by means of differential scanning calorimetry(DSC) and thermogravimetry-differential thermal gravimetry(TG-DTG). The results show that the exothermic decomposition peak temperatures for compounds 1 and 2 were 642.65 and 644.46 K, respectively, and the kinetic equations of the main exothermic decomposition were also derived from non-isothermal method. Additionally, the thermal safety of the two compounds was evaluated by calculating self-accelerating decomposition temperature(TSADT) and critical temperature of thermal explosion(Tb). The results(the TSADT and Tb values are 605.43 and 635.69 K for compound 1; 607.38 and 638.96 K for compound 2) reveal that the two compounds exhibit better thermal safety than BTATz.
基金supported financially by Henan Province basic and frontier technology research projects of Henan Provincial Department of Science and Technology(No.142300410083)
文摘A new Cu(Ⅱ) metal-organic coordination polymer, {[Cu2(tbip)2(bie)2]·H2O}n (1, H2tbip = 5-tert-butyl isophthalic acid, bie = 1,2-bis(imidazol-1 '-yl)ethane), was assembled under hydrothermal conditions by the reactions of Cu(Ⅱ) acetate with H2tbip and bie. Complex 1 was characterized by elemental analysis, IR spectroscopy and X-ray single-crystal diffraction. Complex 1 crystallizes in triclinic, space group P1, with a = 9.9145(10), b = 13.2211(13), c = 15.4363(15) nm, a = 87.0250(10), β = 88.3220(10), γ = 83.8240(10)°, V= 2008.4(3) nm3, Z = 2, Dc = 1.505 Mg/m3, F(000) = 944, g = 1.125 mm^-1, S = 1.030, the final R = 0.0336 and wR = 0.0790. The results reveal that complex 1 is a two-dimensional layered structure. In addition, magnetic properties of I were also investigated.
基金Supported by the Natural Science Foundation of Ningxia(No.NZ15015)
文摘A new coordination compound, [Co(L223)2(H2O)2]·H2pm(1, L223 = 3,4-bis(2-pyridyl)-5-(3-pyridyl)-1,2,4-triazole and H4 pm = pyromellitic acid), has been synthesized. The structure of complex 1 has been characterized by X-ray single-crystal diffraction, elemental analysis, IR spectrum analysis and thermogravimetric analysis. Single-crystal X-ray diffraction analysis reveals that complex 1 belongs to the triclinic system, space group P1 with a = 10.2470(8), b = 10.2879(9), c = 10.2951(11) ?, α = 109.398(2), β = 97.6590(10), γ = 95.3260(10)°, V = 1003.60(16) ?3, Z = 1, Dc = 1.565 g/cm^3, μ = 0.508 mm%^-1, Mr = 945.73, F(000) = 485, the final R = 0.0562 and w R = 0.0783 with I 〉 2σ(I). Two L223 as chelating ligands link one Co(II) ion to form a 0D motif. Furthermore, the 0D motifs are linked into a 2D coordination pattern with hydrogen bonds. In addition, the antifungal effects of the ligand and the complex were evaluated by the disc diffusion method against Colletotrichum gloeosporioides Penz. 1 represents antifungal activity with high levels of inhibitory potency which is larger than the corresponding ligand.
基金supported by the National Natural Science Foundation of China(21073142,21173168and21127004)the Natural Science Foundation of Shaanxi Province(SJ08B09)the Natural Science Foundation of the Department of Education of Shaanxi Province(2010JK882,2010JQ2007and11JS110)
文摘Three new cobalt(II) coordination compounds, [Co(3,3'-Hbpt)2(H2pm)(H20)2]'2H20 (1), [Co(4,4'-Hbpt)(pm)0.5(H20)]'3H20 (2) and [Co(3,4'-Hbpt)(pm)0.5(H20)3]'2H20 (3) (3,3'-Hbpt = 3,5-bis(3-pyridyl)-lH-1,2,4-triazole; 4,4'-bpt = 3,5-bis(4-pyridyl)- 1H-1,2,4-triazole, 3,4'-Hbpt = 3-(3-pyridyl)-5-(4'-pyridyl)-lH-1,2,4-triazole and Hapm = pyromellitic acid) have been synthe- sized by hydrothermal reactions. Single-crystal X-ray diffraction reveals that compound 1 has a one-dimensional (1D) chain network, 2 exhibits a four-connected three-dimensional (3D) structure with 1D open channels encapsulated by water molecules, while 3 displays a regular two-dimensional (2D) architecture connected through 1D metal helical chains. In addition, the effi- cacy of compounds 1-3 as additives to promote the thermal decomposition of ammonium perchlorate (AP) is explored by dif- ferential scanning calorimetry (DSC).
基金Supported by the National Natural Science Foundation of China(No.21101127), the Natural Science Basic Research Plan in Shaanxi Province of China(No.2011JQ2002), the China Postdoctoral Science Foundation Funded Proj ect(No.20110491676), the National Defense Pre-research Foundation of China(No.9140A28020111BQ3401) and the National Defense Pre-research Foun-dation of China(No.A312011005).
文摘A new high-energy organic magnesium salt [Mg(H2O)6](BTATz)·2H2O[BTATz=3,6-bis(1H-1,2,3,4-tetrazol-5-yl-amino)-1,2,4,5-tetrazine] was synthesized and characterized by elemental analysis and Fourier transform infrared(FTIR) spectrometry.Its crystal structure was determined by X-ray single crystal diffraction.The crystal belongs to monoclinic system with space group C2/c and a=2.1329(7) nm,b=0.52275(16) nm,c=1.5909(5) nm,β=100.471(6)°,V=1.7443(9) nm3,Z=4,μ=0.361 mm-1,F(000)=900 and Dc=1.644 g/cm3.Meanwhile,the thermal behavior of [Mg(H2O)6](BTATz)·2H2O was studied under the non-isothermal conditions by differential scanning calorimetry(DSC) and thermalgravity-differential thermalgravity(TG-DTG) methods.The enthalpy,apparent activation energy and per-exponential factor of the main exothermic decomposition reaction are 898.88 J/g,139.2 kJ/mol and 1010.48 S-1,respectively.The values of the self-accelerating decomposition temperature(TsADT),the thermal ignition temperature(TTIT) and the critical temperature of thermal explosion(Tb) for [Mg(H2O)6](BTATz).2H2O are 515.13,532.08 and 565.99 K,respectively.
基金the National Key Research and Development Program of China(No.2017YFB0404404)the Open Fund of State Key Laboratory of Luminescent Materials and Devices(South China University of Technology),China。
文摘Thermally activated delayed fluorescence(TADF)organic light-emitting diodes(OLEDs)have been demonstrated in applications such as displays and solid-state lightings.However,weak stability and ineffi-cient emission of blue TADF OLEDs are two key bottlenecks limiting the development of solution processable displays and white light sources.This work presents a solution-processed OLED using a blue-emitting TADF small molecule bis[4-(9,9-dimethyl-9,10-dihydroacridine)phenyl]sulfone(DMAC-DPS)as an emitter.We comparatively investigated the effects of single host poly(Nvinylcarbazole)(PVK)and a co-host of 60%PVK and 30%2,2′-(1,3-phenylene)-bis[5-(4-tert-butylphenyl)-1,3,4-oxadiazole](OXD-7)on the device performance(the last 10%is emitter DMAC-DPS).The co-host device shows lower turn-on voltage,similar maximum luminance,and much slower external quantum efficiency(EQE)rolloff.In other words,device stability improved by doping OXD-7 into PVK,and the device impedance simultaneously and significantly reduced from 8.6103 to 4.2103 W at 1000 Hz.Finally,the electroluminescent stability of the co-host device was significantly enhanced by adjusting the annealing temperature.