The structures,mechanical properties and electronic structures of M metals(M=Ti,V,Cr,Mn and Fe)dopedβ-Si_(3)N_(4) were investigated by First-principles calculations within CASTEP.The calculated lattice parameters of...The structures,mechanical properties and electronic structures of M metals(M=Ti,V,Cr,Mn and Fe)dopedβ-Si_(3)N_(4) were investigated by First-principles calculations within CASTEP.The calculated lattice parameters ofβ-Si_(3)N_(4) were consistent with previous date.The cohesive energy and formation enthalpy show that initialβ-Si_(3)N_(4) has the highest structural stability.The calculated elastic constant and the Voigt-Reuss-Hill approximation indicate that elastic moduli ofβ-Si_(3)N_(4) are slightly reduced by M doping.Based on Poisson’s and Pugh’s ratio,β-Si_(3)N_(4) is a ductile material and the toughness ofβ-Si_(3)N_(4) increases with M doping,and Fe doping exhibited the best toughness.The results of density of states,charge distributions and overlapping populations indicate thatβ-Si_(3)N_(4) has the strong covalent and ionic bond strength between N and Si.展开更多
In the traditional process, m-phenylenediamine reacts with fuming sulfuric acid at high temperature to get intermediates, and then after dehydration occurs intramolecular rearrangement to get 2,4-diaminobenzenesulfoni...In the traditional process, m-phenylenediamine reacts with fuming sulfuric acid at high temperature to get intermediates, and then after dehydration occurs intramolecular rearrangement to get 2,4-diaminobenzenesulfonic acid. Traditional methods need to consume a lot of fuming sulfuric acid or concentrated sulfuric acid, resulting in high industrial large-scale production cost, more waste, and posing a serious environmental pollution risk. In this thesis, three different sulfonation reagents were used for the sulfonation reaction of m-phenylenediamine, and the reaction mechanisms and crystal structures of the three pathways were investigated. The three routes are: 1) one-step synthesis of monosulfonated compound 1 from raw material and sulfur trioxide (SO<sub>3</sub>);2) rapid reaction of raw material and chlorosulfonic acid to synthesize bisulfonated compound 2;3) direct eutectic crystallization of raw material and ordinary sulfuric acid to obtain compound 3. The crystal structure of the compounds synthesized by three paths was analyzed by X-ray single crystal diffraction, and compound 1 was characterized by NMR, Fourier infrared spectra, UV-visible spectrum and Mass spectrometry. The one-step synthesis of SO<sub>3</sub> as a sulfonation reagent has the advantages of mild reaction conditions, simple operation and low cost.展开更多
In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and exper...In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and experimental data have shown that the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure has a stronger light absorption capacity and larger specific surface area than pure g-C_(3)N_(4) NCs and g-C_(3)N_(4) nanosheets(NSs),and the presence of the co-catalysts 1T'-MoS_(2) can effectively inhibit the photoinduced carrier recombination.As a result,the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure with an optimum 1T'-MoS_(2) loading of 9 wt%displays a hydrogen evolution rate of 1949 mmol h^(-1) g^(-1),162.4,1.2,1.5,1.6 and 1.2 times than pure g-C_(3)N_(4) NCs(12 mmol h^(-1) g^(-1)),Pt/g-C_(3)N_(4) NCs(1615 mmol h^(-1) g^(-1))and Pt/g-C_(3)N_(4) nanosheets(NSs,1297 mmol h^(-1) g^(-1)),1T'-MoS_(2)/g-C_(3)N_(4) nanosheets(1216 mmol h^(-1) g^(-1))and 2H-MoS_(2)/g-C_(3)N_(4) nanocages(1573 mmol h^(-1) g^(-1)),respectively,and exhibits excellent cycle stability.Therefore,1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure is a suitable photocatalyst for green H_(2) production.展开更多
The crystal structure of 2(1-phenyl-3-methyl-5-chloro-1H-pyrazol-4-yl)-3-(1- naphthoylamido)-4-thiazolidinone (C24H19ClN4O2S, Mr = 462.94) has been determined by single- crystal X-ray diffraction method. The crystal b...The crystal structure of 2(1-phenyl-3-methyl-5-chloro-1H-pyrazol-4-yl)-3-(1- naphthoylamido)-4-thiazolidinone (C24H19ClN4O2S, Mr = 462.94) has been determined by single- crystal X-ray diffraction method. The crystal belongs to monoclinic, space group P21/c with a = 11.623(5), b = 11.579(5), c = 16.619(7) ? b = 90.112(8), V = 2237(2) 3, Z = 4, Dc = 1.375 g/cm3, m = 0.294 mm-1, F(000) = 960, R = 0.0492 and wR = 0.0768 for 3932 unique reflections with 1897 observed ones (I > 2s(I)). X-ray analysis reveals that there exist both intra-and intermolecular hydrogen bonds in the crystal lattice.展开更多
The title compounds, C7H4I2O2 1 and C13H7I2N2O3 2, have been synthesized and characterized by single-crystal X-ray diffraction. Compound 1 crystallizes in monoclinic, space group P21/c with a = 9.802(2), b = 13.867...The title compounds, C7H4I2O2 1 and C13H7I2N2O3 2, have been synthesized and characterized by single-crystal X-ray diffraction. Compound 1 crystallizes in monoclinic, space group P21/c with a = 9.802(2), b = 13.867(3), c = 7.364(2) A, β = 109.74(3)°, V= 942.1(3) A^3, Dc= 2.636 g/cm^3, C7H4I2O2, Mr= 373.90, F(000) = 672, μ = 6.627 mm^-1, Z = 4, R = 0.0459 and wR = 0.1018 for 1805 observed reflections (I 〉 2 σ(I)). Compound 2 belongs to the monoclinic system, space group P21/n with a = 9.015(2), b = 12.024(2), c = 14.072(3) A, β = 103.91(3)°, V = 1480.6(5) A^3, Dc= 2.216 g/cm^3, C13H7I2N2O3, Mr= 494.01, F(000) = 920, p = 4.255 mm^-1, Z = 4, R = 0.0777 and wR = 0.1757 for 2896 observed reflections (I 〉 2σ(I)). Compounds 1 and 2 were assayed for antibacterial activities against three Gram positive bacterial strains (B. subtilis, S. aureus and S. faecalis) and three Gram negative bacterial strains (E. coli, P. aeruginosa and E. cloacae) by MTr method. Fortunately, compound 2 is found to show potent antibacterial activity against these six bacterial strains.展开更多
The title compound N-(2,6-difluorobenzoyl)-N'-[5-(4-trifluoromethylphenyl)-1,3,4-thiadiazol-2-yl]urea(C17H9F5N4O2S,Mr = 428.34) has been synthesized by the reaction of 2-amino-5-(4-trifluoromethylphenyl)-1,3,...The title compound N-(2,6-difluorobenzoyl)-N'-[5-(4-trifluoromethylphenyl)-1,3,4-thiadiazol-2-yl]urea(C17H9F5N4O2S,Mr = 428.34) has been synthesized by the reaction of 2-amino-5-(4-trifluoromethylphenyl)-1,3,4-thiadiazole with 2,6-difluorobenzoyl isocyanate,and its crystal structure was determined by single-crystal X-ray diffraction.The crystal belongs to monoclinic,space group P21/n with a = 10.7316(13),b = 10.5617(13),c = 16.037(2) ,β = 106.408(2)°,V = 1743.6(4) 3,Z = 4,Dc = 1.632 g/cm3,μ = 0.260 mm-1,F(000) = 864,the final R = 0.0599 and wR = 0.1420 for 3467 observed reflections with I〉 2σ(I).The urea group,which adopts a planar configuration mediated by the intramolecular N-H...O hydrogen bond,is nearly coplanar with the thiadiazole and 4-trifluoromethylbenzene rings.The title compound was found to exhibit good fungicidal activity against Rhizoctonia solani and Botrytis cinerea.展开更多
The title complex (C50H44C14O8) was synthesized and structurally determined by single-crystal X-ray diffraction method. It crystallizes in monoclinic, space group P21/n with a = 19.7768(4), b =10.2085(2), c = 21...The title complex (C50H44C14O8) was synthesized and structurally determined by single-crystal X-ray diffraction method. It crystallizes in monoclinic, space group P21/n with a = 19.7768(4), b =10.2085(2), c = 21.2721(4)A,β= 97.153(1)°, V = 4261.23(14)A^3, Z = 4, Mr = 914.65, F(000) = 1904, Dc = 1.426 g/cm^3,μ = 0.336, the final R = 0.0550 and wR = 0.1647. The compound was structurally characterized by IR and ^1H NMR. The molecules are stacked through C-H...π interactions and intermolecular C-H...O hydrogen bonds.展开更多
Six new transition metal complexes, [Zn(HBTC)(PYTPY)]n·n PYTPY(1), [Cu(HBTC)(PYTPY)]n·n PYTPY(2), [Co(HBTC)(PYTPY)]n·n DMF(3), [Mn(HBTC)(PYTPY)]n·n DMF(4), [Cd(HBTC)(PYTP...Six new transition metal complexes, [Zn(HBTC)(PYTPY)]n·n PYTPY(1), [Cu(HBTC)(PYTPY)]n·n PYTPY(2), [Co(HBTC)(PYTPY)]n·n DMF(3), [Mn(HBTC)(PYTPY)]n·n DMF(4), [Cd(HBTC)(PYTPY)(H2O)]n·2nH2O(5), and [Co(HBTC)(PYTPY)(H2O)2](6),(H3BTC = 1,3,5-benzenetricarboxylic acid, PYTPY = 4'-(4-pyridyl)-2,2':6',2''-terpyridine, DMF = N,N?-dimethylformamide), have been synthesized and characterized by elemental analysis, IR and X-ray single-crystal diffraction. Complexes 1~5 all feature one-dimensional chain structures, and complex 6 exhibits a zero-dimensional structure. Complexes 1~5 present three-dimensional(3D) supramolecular frameworks via π-π stacking interactions, whenas 6 has also a 3D supramolecular structure assembled by hydrogen bonding. Meanwhile, complexes 1 ~ 6 exhibit the thermal stabilities and photoluminescent properties.展开更多
The title compound (C29H50O2, Mr = 430.69) was isolated from the algae Halimeda xishaensis collected from the South China Sea. Its crystal structure was determined by single-crystal X-ray diffraction for the first tim...The title compound (C29H50O2, Mr = 430.69) was isolated from the algae Halimeda xishaensis collected from the South China Sea. Its crystal structure was determined by single-crystal X-ray diffraction for the first time. The crystal belongs to orthorhombic, space group P212121 with a = 8.1560(13), b = 10.7861(18), c = 29.973(5) ? V = 2636.8(8) 3, Z = 4, Dc = 1.085 g/cm3, F(000) = 960, (Mo-K? = 4.533 mm-1, ?= 0.71073 ? S = 1.061, (?max = 0.382 and (?min = 0.244 e/?. The structure was refined to R = 0.0561 and wR = 0.1553 for 2711 observed reflections with I > 2(I). X-ray diffraction analysis reveals that the title compound has two ?OH groups, and the side chain is saturated. There exist two intermolecular hydrogen bonds between three molecules.展开更多
A new ID coordination polymer, [Cda(L1)2(L2)2].H2O (1, H2L1 = 4-(carboxy- methoxy)benzoic acid and L2 = 2-(4-fluorophenyl)-I H-imidazo[4,5-f][1,10]phenanthroline), has been hydrothermally synthesized and cha...A new ID coordination polymer, [Cda(L1)2(L2)2].H2O (1, H2L1 = 4-(carboxy- methoxy)benzoic acid and L2 = 2-(4-fluorophenyl)-I H-imidazo[4,5-f][1,10]phenanthroline), has been hydrothermally synthesized and characterized by elemental analysis and single-crystal X-ray diffraction. It crystallizes in triclinic, space group P1 with a = 9.985(5), b = 10.768(5), c = 12.512(5) A, a = 68.959(5), β = 80.354(5), γ = 79.663(5)°, V= 1227.4(10) A3, Z = 1, C56H36Cd2F2N8O11, Mr = 1259.73, Dc = 1.704 g/cm3, F(000) = 630, μ(MoKa) = 0.949 mm-1, R = 0.0261 and wR = 0.0655. The L1 anions link the neighboring Cd(II) atoms to form a 1D double chain structure. The L2 ligands are alternately located on both sides of the double chains. More interestingly, the lateral L2 ligands from adjacent double chains are paired to furnish strong π-π interactions, yielding a 2D supramolecular layer. N-H...O, O-H...N and O-H...O hydrogen bonds further stabilize the structure of 1. The luminescent property of 1 was studied in solid state at room temperature.展开更多
A new metal-organic framework based on bbi and PHBA(bbi = 1,1'-(1, 4-butanediyl)bis(imidazole), PHBA = p-hydroxybenzoic acid), namely, [Cd(bbi)(PHBA)2]n(1) has been synthesized by the conventional method....A new metal-organic framework based on bbi and PHBA(bbi = 1,1'-(1, 4-butanediyl)bis(imidazole), PHBA = p-hydroxybenzoic acid), namely, [Cd(bbi)(PHBA)2]n(1) has been synthesized by the conventional method. Compound 1 displays a two-dimensional(2D) layer structure possessing the left-and right-handed helical chains and stabilized by intermolecular hydrogen-bonding to form a three-dimensional(3D) supramolecular structure. Topologically, the 2D layer belongs to well-known(4,4) network topology. The structure has been determined by single-crystal X-ray diffraction analyses, and further characterized by infrared spectra(IR), elemental analyses and powder X-ray diffraction. In addition, the thermal behavior and luminescent properties of [Cd(bbi)(PHBA)2]n have been investigated in detail.展开更多
A new ligand 2,5-di(pyridin-4-yl)benzaldehyde (L) was synthesized by the reaction of pyridin-4-yl-boronic acid with 2,5-dibromobenzaldehyde. Two novel CdII coordination polymers, [CdL(BDC)].DMF (1) and [CdL(B...A new ligand 2,5-di(pyridin-4-yl)benzaldehyde (L) was synthesized by the reaction of pyridin-4-yl-boronic acid with 2,5-dibromobenzaldehyde. Two novel CdII coordination polymers, [CdL(BDC)].DMF (1) and [CdL(BPDC)].4H2O (2) (BDC = 1,4-benzenedicarboxylate, BPDC = 4,4′-biphenyldicarboxylate), have been constructed based on the mixed ligands of L and dicaboxylic acid via solvothermal synthesis, and characterized by IR, microanalysis, TGA, single and power X-ray diffraction, and their fluorescence properties were also investigated. 1 crystallizes in orthorhombic space group Pcca with a = 15.8236(3), b = 16.0038(3), c = 20.2207(3) A, V = 5120.64(16) A3, Z = 8, Mr = 633.83, Dc = 1.644 g/cm3, F(000) = 2528, GOOF = 1.130, the final R = 0.0568 and wR = 0.1513 for 4108 observed reflections with I〉 2σ(I). 2 crystallizes in orthorhombic space group Pbcn with a = 29.1148(1), b = 16.0120(6), c = 16.7097(7) A, V = 7789.8(5) A3, Z = 8, Mr = 675.88, Dc = 1.153 g/cm3,/7(000) = 2712, GOOF = 1.088, the final R = 0.0670 and wR = 0.1805 for 6047 observed reflections with I〉 2σ(I). The dinuclear Cd2(CO2)4 unit is linked by BDC in 1 to form a 2D sheet that is further pillared by L to create a 3D metal-organic framework, which possesses a parallelogram channel with diagonal distances of-13.3 × 17.6 A along the b direction. 2 is structurally similar to 1, but has larger diagonal distances of-14.0 × 26.7 A. due to the elongated auxiliary ligand BPDC compared with the BDC ligand in 1. They are both thermally stable and exhibit strong photoluminescence in the visible region.展开更多
A series of lanthanide binuclear complexes, Ln2(L)6(H2O)4·2H2O(Ln=Sm(Ⅲ), Gd(Ⅲ), Er(Ⅲ), Yb(Ⅲ), HL=4-quinolinea-carboxylic acid, were synthesized by reactions of corresponding rare earth salts with...A series of lanthanide binuclear complexes, Ln2(L)6(H2O)4·2H2O(Ln=Sm(Ⅲ), Gd(Ⅲ), Er(Ⅲ), Yb(Ⅲ), HL=4-quinolinea-carboxylic acid, were synthesized by reactions of corresponding rare earth salts with 4-quinolineacarboxylic acid at room temperature and were characterized by elemental analysis, IR spectroscopy, and single-crystal X-ray diffraction.X-ray diffraction analyses showed that they exhibited the same binuclear architecture and crystallized in monoclinic system and P21/c space group.In four complexes, each metal center adopted nine-coordinated mode coordinated by nine O atoms from two H2O molecules and three carboxyls of three ligands, and HL showed three different coordination modes.The variable-temperature magnetic susceptibility showed that complex Gd2(L)6(H2O)4·2H2O performed very weak antiferromagnetic property at low temperature and exchange was almost paramagnetic at high temperature.Complexes Er2(L)6(H2O)4·2H2O and Yb2(L)6(H2O)4·2H2O performed dominating antiferromagnetic coupling.展开更多
A new Cd(II) coordination polymer, [Cd05(nba)(bib)0.5]2n (1, Hnba = 4-nitrobenzoicacid, bib = 1,4-bis(imidazol-l-yl)-butane), was synthesized at room temperature condition andcharacterized by IR spectra, ele...A new Cd(II) coordination polymer, [Cd05(nba)(bib)0.5]2n (1, Hnba = 4-nitrobenzoicacid, bib = 1,4-bis(imidazol-l-yl)-butane), was synthesized at room temperature condition andcharacterized by IR spectra, elemental analyses, single-crystal and powder X-ray diffractions.Complex 1 belongs to the monoclinic system, C2/c space group, with a = 26.0600(14), b = 6.7889(4),c = 16.5825(9)A, β= 118.8120(10)°, V= 2570.6(2) A3, Z= 4. It shows one-dimensional chains andis further linked by π-π stacking interactions to yield a three-dimensional supramolecular structure.Thermal stability and luminescence of 1 were investigated.展开更多
A novel cobalt complex,[Co2(bptc)(bix)1.5](1,H4bptc=3,3',4,4'-biphenyltetra-carboxylic acid,bix = 1,4-bis(imidazol-1-ylmethyl)benzene),has been hydrothermally prepared and characterized by IR spectroscopy,el...A novel cobalt complex,[Co2(bptc)(bix)1.5](1,H4bptc=3,3',4,4'-biphenyltetra-carboxylic acid,bix = 1,4-bis(imidazol-1-ylmethyl)benzene),has been hydrothermally prepared and characterized by IR spectroscopy,elemental analysis and single-crystal X-ray diffraction.The crystal is of triclinic system,space group P1 with a=10.770(7),b=12.245(8),c=13.514(9),α=102.829(8),β=107.734(8),γ=98.833(9)°,C37H27N6O8Co2,Mr=801.51,V=1607.5(18)3,Dc=1.656g/cm3,F(000)=818,μ=1.100mm-1,Z=2,the final R = 0.0694 and wR = 0.1543 for 3034 observed reflections(I2σ(I)).In the title complex,the two Co(Ⅱ) ions are in different coordination environments with distorted octahedral and trigonal bipyramidal geometries,respectively.The Co atoms are linked together through hexadentate bptc ligands,giving rise to 2D layers which are bridged by the bix ligands into a 3-D supramolecular network.Magnetic susceptibilities of 1 reveal weak antiferromagnetic exchange interactions between the adjacent Co(Ⅱ) ions.展开更多
A new Cu(Ⅱ) complex [Cu(4-cba)(1,10-phen)(H2O)2](NO3) (4-Hcba = 4-cyanobenzoic acid) has been synthesized by solvothermal reaction in an ethanol/water mixed solution at 100 ℃ and structurally characteriz...A new Cu(Ⅱ) complex [Cu(4-cba)(1,10-phen)(H2O)2](NO3) (4-Hcba = 4-cyanobenzoic acid) has been synthesized by solvothermal reaction in an ethanol/water mixed solution at 100 ℃ and structurally characterized by single-crystal X-ray diffraction. Crystallographic data: C20H16CuN4O7, Mr= 487.91, triclinic, space group PI, a = 7.8420(2), b = 9.1070(2), c = 15.1140(6) A, a = 76.889(9), β = 81.332(11), γ = 74.844( 11)°, V = 1009.89(5) A^3, Z = 2, Dc = 1.605 g/cm^3, F(000) = 498, μ = 1.134 mm^-1, the final R = 0.0379 and wR = 0.0865 for 2977 observed reflections with 1 〉 2σ(Ⅰ). The Cu(Ⅱ) atom is coordinated by two terminal water molecules, one chelating 1,10-phen molecule and one monodentate 4-cba ligand to form a slightly distorted square pyramid. The title complex molecules are connected through hydrogen bonds and π-π stacking interactions to generate a 2D layered network. The thermogravimetric analysis of the title complex has also been discussed.展开更多
文摘The structures,mechanical properties and electronic structures of M metals(M=Ti,V,Cr,Mn and Fe)dopedβ-Si_(3)N_(4) were investigated by First-principles calculations within CASTEP.The calculated lattice parameters ofβ-Si_(3)N_(4) were consistent with previous date.The cohesive energy and formation enthalpy show that initialβ-Si_(3)N_(4) has the highest structural stability.The calculated elastic constant and the Voigt-Reuss-Hill approximation indicate that elastic moduli ofβ-Si_(3)N_(4) are slightly reduced by M doping.Based on Poisson’s and Pugh’s ratio,β-Si_(3)N_(4) is a ductile material and the toughness ofβ-Si_(3)N_(4) increases with M doping,and Fe doping exhibited the best toughness.The results of density of states,charge distributions and overlapping populations indicate thatβ-Si_(3)N_(4) has the strong covalent and ionic bond strength between N and Si.
文摘In the traditional process, m-phenylenediamine reacts with fuming sulfuric acid at high temperature to get intermediates, and then after dehydration occurs intramolecular rearrangement to get 2,4-diaminobenzenesulfonic acid. Traditional methods need to consume a lot of fuming sulfuric acid or concentrated sulfuric acid, resulting in high industrial large-scale production cost, more waste, and posing a serious environmental pollution risk. In this thesis, three different sulfonation reagents were used for the sulfonation reaction of m-phenylenediamine, and the reaction mechanisms and crystal structures of the three pathways were investigated. The three routes are: 1) one-step synthesis of monosulfonated compound 1 from raw material and sulfur trioxide (SO<sub>3</sub>);2) rapid reaction of raw material and chlorosulfonic acid to synthesize bisulfonated compound 2;3) direct eutectic crystallization of raw material and ordinary sulfuric acid to obtain compound 3. The crystal structure of the compounds synthesized by three paths was analyzed by X-ray single crystal diffraction, and compound 1 was characterized by NMR, Fourier infrared spectra, UV-visible spectrum and Mass spectrometry. The one-step synthesis of SO<sub>3</sub> as a sulfonation reagent has the advantages of mild reaction conditions, simple operation and low cost.
基金funding from the National Natural Science Foundation of China (No.51872173)Taishan Scholar Foundation of Shandong Province (No.tsqn201812068)+2 种基金Youth Innovation Technology Project of Higher School in Shandong Province (No.2019KJA013)Science and Technology Special Project of Qingdao City (No.20-3-4-3-nsh)the Opening Fund of State Key Laboratory of Heavy Oil Processing (No.SKLOP202002006)。
文摘In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and experimental data have shown that the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure has a stronger light absorption capacity and larger specific surface area than pure g-C_(3)N_(4) NCs and g-C_(3)N_(4) nanosheets(NSs),and the presence of the co-catalysts 1T'-MoS_(2) can effectively inhibit the photoinduced carrier recombination.As a result,the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure with an optimum 1T'-MoS_(2) loading of 9 wt%displays a hydrogen evolution rate of 1949 mmol h^(-1) g^(-1),162.4,1.2,1.5,1.6 and 1.2 times than pure g-C_(3)N_(4) NCs(12 mmol h^(-1) g^(-1)),Pt/g-C_(3)N_(4) NCs(1615 mmol h^(-1) g^(-1))and Pt/g-C_(3)N_(4) nanosheets(NSs,1297 mmol h^(-1) g^(-1)),1T'-MoS_(2)/g-C_(3)N_(4) nanosheets(1216 mmol h^(-1) g^(-1))and 2H-MoS_(2)/g-C_(3)N_(4) nanocages(1573 mmol h^(-1) g^(-1)),respectively,and exhibits excellent cycle stability.Therefore,1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure is a suitable photocatalyst for green H_(2) production.
文摘The crystal structure of 2(1-phenyl-3-methyl-5-chloro-1H-pyrazol-4-yl)-3-(1- naphthoylamido)-4-thiazolidinone (C24H19ClN4O2S, Mr = 462.94) has been determined by single- crystal X-ray diffraction method. The crystal belongs to monoclinic, space group P21/c with a = 11.623(5), b = 11.579(5), c = 16.619(7) ? b = 90.112(8), V = 2237(2) 3, Z = 4, Dc = 1.375 g/cm3, m = 0.294 mm-1, F(000) = 960, R = 0.0492 and wR = 0.0768 for 3932 unique reflections with 1897 observed ones (I > 2s(I)). X-ray analysis reveals that there exist both intra-and intermolecular hydrogen bonds in the crystal lattice.
基金supported by the National Natural Science Foundation of China (No 30772627)
文摘The title compounds, C7H4I2O2 1 and C13H7I2N2O3 2, have been synthesized and characterized by single-crystal X-ray diffraction. Compound 1 crystallizes in monoclinic, space group P21/c with a = 9.802(2), b = 13.867(3), c = 7.364(2) A, β = 109.74(3)°, V= 942.1(3) A^3, Dc= 2.636 g/cm^3, C7H4I2O2, Mr= 373.90, F(000) = 672, μ = 6.627 mm^-1, Z = 4, R = 0.0459 and wR = 0.1018 for 1805 observed reflections (I 〉 2 σ(I)). Compound 2 belongs to the monoclinic system, space group P21/n with a = 9.015(2), b = 12.024(2), c = 14.072(3) A, β = 103.91(3)°, V = 1480.6(5) A^3, Dc= 2.216 g/cm^3, C13H7I2N2O3, Mr= 494.01, F(000) = 920, p = 4.255 mm^-1, Z = 4, R = 0.0777 and wR = 0.1757 for 2896 observed reflections (I 〉 2σ(I)). Compounds 1 and 2 were assayed for antibacterial activities against three Gram positive bacterial strains (B. subtilis, S. aureus and S. faecalis) and three Gram negative bacterial strains (E. coli, P. aeruginosa and E. cloacae) by MTr method. Fortunately, compound 2 is found to show potent antibacterial activity against these six bacterial strains.
基金supported by the Natural Science Foundation of Hubei Province (No. 2008CDB016)the Research Project for Innovative Research Team of Hubei University for Nationalities
文摘The title compound N-(2,6-difluorobenzoyl)-N'-[5-(4-trifluoromethylphenyl)-1,3,4-thiadiazol-2-yl]urea(C17H9F5N4O2S,Mr = 428.34) has been synthesized by the reaction of 2-amino-5-(4-trifluoromethylphenyl)-1,3,4-thiadiazole with 2,6-difluorobenzoyl isocyanate,and its crystal structure was determined by single-crystal X-ray diffraction.The crystal belongs to monoclinic,space group P21/n with a = 10.7316(13),b = 10.5617(13),c = 16.037(2) ,β = 106.408(2)°,V = 1743.6(4) 3,Z = 4,Dc = 1.632 g/cm3,μ = 0.260 mm-1,F(000) = 864,the final R = 0.0599 and wR = 0.1420 for 3467 observed reflections with I〉 2σ(I).The urea group,which adopts a planar configuration mediated by the intramolecular N-H...O hydrogen bond,is nearly coplanar with the thiadiazole and 4-trifluoromethylbenzene rings.The title compound was found to exhibit good fungicidal activity against Rhizoctonia solani and Botrytis cinerea.
基金the Scientific Research Fund Projects of China West Normal University(No.06B003)the Youth Fund Projects of Sichuan Educational Department(No.2006B039)
文摘The title complex (C50H44C14O8) was synthesized and structurally determined by single-crystal X-ray diffraction method. It crystallizes in monoclinic, space group P21/n with a = 19.7768(4), b =10.2085(2), c = 21.2721(4)A,β= 97.153(1)°, V = 4261.23(14)A^3, Z = 4, Mr = 914.65, F(000) = 1904, Dc = 1.426 g/cm^3,μ = 0.336, the final R = 0.0550 and wR = 0.1647. The compound was structurally characterized by IR and ^1H NMR. The molecules are stacked through C-H...π interactions and intermolecular C-H...O hydrogen bonds.
基金Supported by the National Natural Science Foundation of China(No.21576112)Natural Science Foundation of Jilin Province(20150623024TC-19,20170520147JH)the Science and Technology Development Plan of Siping City(2015049)
文摘Six new transition metal complexes, [Zn(HBTC)(PYTPY)]n·n PYTPY(1), [Cu(HBTC)(PYTPY)]n·n PYTPY(2), [Co(HBTC)(PYTPY)]n·n DMF(3), [Mn(HBTC)(PYTPY)]n·n DMF(4), [Cd(HBTC)(PYTPY)(H2O)]n·2nH2O(5), and [Co(HBTC)(PYTPY)(H2O)2](6),(H3BTC = 1,3,5-benzenetricarboxylic acid, PYTPY = 4'-(4-pyridyl)-2,2':6',2''-terpyridine, DMF = N,N?-dimethylformamide), have been synthesized and characterized by elemental analysis, IR and X-ray single-crystal diffraction. Complexes 1~5 all feature one-dimensional chain structures, and complex 6 exhibits a zero-dimensional structure. Complexes 1~5 present three-dimensional(3D) supramolecular frameworks via π-π stacking interactions, whenas 6 has also a 3D supramolecular structure assembled by hydrogen bonding. Meanwhile, complexes 1 ~ 6 exhibit the thermal stabilities and photoluminescent properties.
基金the 863 National Foundation of China (No. 2001AA628100) National Natural Science Foundation of China (No. 20002001) and Natural Science Foundation of Guangdong Province (No .000720)
文摘The title compound (C29H50O2, Mr = 430.69) was isolated from the algae Halimeda xishaensis collected from the South China Sea. Its crystal structure was determined by single-crystal X-ray diffraction for the first time. The crystal belongs to orthorhombic, space group P212121 with a = 8.1560(13), b = 10.7861(18), c = 29.973(5) ? V = 2636.8(8) 3, Z = 4, Dc = 1.085 g/cm3, F(000) = 960, (Mo-K? = 4.533 mm-1, ?= 0.71073 ? S = 1.061, (?max = 0.382 and (?min = 0.244 e/?. The structure was refined to R = 0.0561 and wR = 0.1553 for 2711 observed reflections with I > 2(I). X-ray diffraction analysis reveals that the title compound has two ?OH groups, and the side chain is saturated. There exist two intermolecular hydrogen bonds between three molecules.
基金Supported by Jilin Province Science and Technology Development projects (No. 201105085)
文摘A new ID coordination polymer, [Cda(L1)2(L2)2].H2O (1, H2L1 = 4-(carboxy- methoxy)benzoic acid and L2 = 2-(4-fluorophenyl)-I H-imidazo[4,5-f][1,10]phenanthroline), has been hydrothermally synthesized and characterized by elemental analysis and single-crystal X-ray diffraction. It crystallizes in triclinic, space group P1 with a = 9.985(5), b = 10.768(5), c = 12.512(5) A, a = 68.959(5), β = 80.354(5), γ = 79.663(5)°, V= 1227.4(10) A3, Z = 1, C56H36Cd2F2N8O11, Mr = 1259.73, Dc = 1.704 g/cm3, F(000) = 630, μ(MoKa) = 0.949 mm-1, R = 0.0261 and wR = 0.0655. The L1 anions link the neighboring Cd(II) atoms to form a 1D double chain structure. The L2 ligands are alternately located on both sides of the double chains. More interestingly, the lateral L2 ligands from adjacent double chains are paired to furnish strong π-π interactions, yielding a 2D supramolecular layer. N-H...O, O-H...N and O-H...O hydrogen bonds further stabilize the structure of 1. The luminescent property of 1 was studied in solid state at room temperature.
基金Supported by the Science and Technology Development Plan of Jilin Province(20150520006JH)Science and Technology Research Project of Education Department of Jilin Province(2016219)Science and Technology Development Plan of Siping City(2013055)
文摘A new metal-organic framework based on bbi and PHBA(bbi = 1,1'-(1, 4-butanediyl)bis(imidazole), PHBA = p-hydroxybenzoic acid), namely, [Cd(bbi)(PHBA)2]n(1) has been synthesized by the conventional method. Compound 1 displays a two-dimensional(2D) layer structure possessing the left-and right-handed helical chains and stabilized by intermolecular hydrogen-bonding to form a three-dimensional(3D) supramolecular structure. Topologically, the 2D layer belongs to well-known(4,4) network topology. The structure has been determined by single-crystal X-ray diffraction analyses, and further characterized by infrared spectra(IR), elemental analyses and powder X-ray diffraction. In addition, the thermal behavior and luminescent properties of [Cd(bbi)(PHBA)2]n have been investigated in detail.
基金supported by NSFC-21025103 and 20971085"973" Programs (2007CB209701 and 2009CB930403)+1 种基金Shanghai Science and Technology Committee (10DJ1400100)the key project of State Education Ministry
文摘A new ligand 2,5-di(pyridin-4-yl)benzaldehyde (L) was synthesized by the reaction of pyridin-4-yl-boronic acid with 2,5-dibromobenzaldehyde. Two novel CdII coordination polymers, [CdL(BDC)].DMF (1) and [CdL(BPDC)].4H2O (2) (BDC = 1,4-benzenedicarboxylate, BPDC = 4,4′-biphenyldicarboxylate), have been constructed based on the mixed ligands of L and dicaboxylic acid via solvothermal synthesis, and characterized by IR, microanalysis, TGA, single and power X-ray diffraction, and their fluorescence properties were also investigated. 1 crystallizes in orthorhombic space group Pcca with a = 15.8236(3), b = 16.0038(3), c = 20.2207(3) A, V = 5120.64(16) A3, Z = 8, Mr = 633.83, Dc = 1.644 g/cm3, F(000) = 2528, GOOF = 1.130, the final R = 0.0568 and wR = 0.1513 for 4108 observed reflections with I〉 2σ(I). 2 crystallizes in orthorhombic space group Pbcn with a = 29.1148(1), b = 16.0120(6), c = 16.7097(7) A, V = 7789.8(5) A3, Z = 8, Mr = 675.88, Dc = 1.153 g/cm3,/7(000) = 2712, GOOF = 1.088, the final R = 0.0670 and wR = 0.1805 for 6047 observed reflections with I〉 2σ(I). The dinuclear Cd2(CO2)4 unit is linked by BDC in 1 to form a 2D sheet that is further pillared by L to create a 3D metal-organic framework, which possesses a parallelogram channel with diagonal distances of-13.3 × 17.6 A along the b direction. 2 is structurally similar to 1, but has larger diagonal distances of-14.0 × 26.7 A. due to the elongated auxiliary ligand BPDC compared with the BDC ligand in 1. They are both thermally stable and exhibit strong photoluminescence in the visible region.
基金supported by the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality (05005011200602)Foundation of Natural Science of Beijing Municipality (2082004)
文摘A series of lanthanide binuclear complexes, Ln2(L)6(H2O)4·2H2O(Ln=Sm(Ⅲ), Gd(Ⅲ), Er(Ⅲ), Yb(Ⅲ), HL=4-quinolinea-carboxylic acid, were synthesized by reactions of corresponding rare earth salts with 4-quinolineacarboxylic acid at room temperature and were characterized by elemental analysis, IR spectroscopy, and single-crystal X-ray diffraction.X-ray diffraction analyses showed that they exhibited the same binuclear architecture and crystallized in monoclinic system and P21/c space group.In four complexes, each metal center adopted nine-coordinated mode coordinated by nine O atoms from two H2O molecules and three carboxyls of three ligands, and HL showed three different coordination modes.The variable-temperature magnetic susceptibility showed that complex Gd2(L)6(H2O)4·2H2O performed very weak antiferromagnetic property at low temperature and exchange was almost paramagnetic at high temperature.Complexes Er2(L)6(H2O)4·2H2O and Yb2(L)6(H2O)4·2H2O performed dominating antiferromagnetic coupling.
基金supported by the Science and Technology Development Project of Jilin Provincial Science&Technology Department(201205080)the Science and Technology Research Projects of the Education Office of Jilin Province(No.2013.384)
文摘A new Cd(II) coordination polymer, [Cd05(nba)(bib)0.5]2n (1, Hnba = 4-nitrobenzoicacid, bib = 1,4-bis(imidazol-l-yl)-butane), was synthesized at room temperature condition andcharacterized by IR spectra, elemental analyses, single-crystal and powder X-ray diffractions.Complex 1 belongs to the monoclinic system, C2/c space group, with a = 26.0600(14), b = 6.7889(4),c = 16.5825(9)A, β= 118.8120(10)°, V= 2570.6(2) A3, Z= 4. It shows one-dimensional chains andis further linked by π-π stacking interactions to yield a three-dimensional supramolecular structure.Thermal stability and luminescence of 1 were investigated.
基金supported by the National Natural Science Foundation of China (No 20971004)the Outstanding Youth Foundation of Education Commission of Anhui Province (No 2010SQRL108ZD)
文摘A novel cobalt complex,[Co2(bptc)(bix)1.5](1,H4bptc=3,3',4,4'-biphenyltetra-carboxylic acid,bix = 1,4-bis(imidazol-1-ylmethyl)benzene),has been hydrothermally prepared and characterized by IR spectroscopy,elemental analysis and single-crystal X-ray diffraction.The crystal is of triclinic system,space group P1 with a=10.770(7),b=12.245(8),c=13.514(9),α=102.829(8),β=107.734(8),γ=98.833(9)°,C37H27N6O8Co2,Mr=801.51,V=1607.5(18)3,Dc=1.656g/cm3,F(000)=818,μ=1.100mm-1,Z=2,the final R = 0.0694 and wR = 0.1543 for 3034 observed reflections(I2σ(I)).In the title complex,the two Co(Ⅱ) ions are in different coordination environments with distorted octahedral and trigonal bipyramidal geometries,respectively.The Co atoms are linked together through hexadentate bptc ligands,giving rise to 2D layers which are bridged by the bix ligands into a 3-D supramolecular network.Magnetic susceptibilities of 1 reveal weak antiferromagnetic exchange interactions between the adjacent Co(Ⅱ) ions.
基金This work was supported by the NSF for Distinguished Young Scientist of China (20425104) and the NSF of Fujian Province (A0420002, 2005I017)
文摘A new Cu(Ⅱ) complex [Cu(4-cba)(1,10-phen)(H2O)2](NO3) (4-Hcba = 4-cyanobenzoic acid) has been synthesized by solvothermal reaction in an ethanol/water mixed solution at 100 ℃ and structurally characterized by single-crystal X-ray diffraction. Crystallographic data: C20H16CuN4O7, Mr= 487.91, triclinic, space group PI, a = 7.8420(2), b = 9.1070(2), c = 15.1140(6) A, a = 76.889(9), β = 81.332(11), γ = 74.844( 11)°, V = 1009.89(5) A^3, Z = 2, Dc = 1.605 g/cm^3, F(000) = 498, μ = 1.134 mm^-1, the final R = 0.0379 and wR = 0.0865 for 2977 observed reflections with 1 〉 2σ(Ⅰ). The Cu(Ⅱ) atom is coordinated by two terminal water molecules, one chelating 1,10-phen molecule and one monodentate 4-cba ligand to form a slightly distorted square pyramid. The title complex molecules are connected through hydrogen bonds and π-π stacking interactions to generate a 2D layered network. The thermogravimetric analysis of the title complex has also been discussed.