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1.
Arterioscler Thromb Vasc Biol ; 36(5): 810-816, 2016 05.
Artigo em Inglês | MEDLINE | ID: mdl-26988589

RESUMO

OBJECTIVE: Increased plasma concentrations of angiotensin II (Ang II) have been implicated in many cardiovascular diseases, such as atherosclerosis, aortic aneurysms, and myocardial infarction, in humans. However, it is not known whether high levels of plasma Ang II affect coronary plaque stability and subsequent myocardial infarction. This study was designed to examine whether elevated plasma Ang II can directly induce coronary events, such as acute coronary syndrome. APPROACH AND RESULTS: To examine the above hypothesis, we infused Ang II (100 ng/min per kg [low group] and 200 ng/min per kg [high group]) or saline vehicle via osmotic minipumps into Watanabe heritable hyperlipidemic rabbits, a model of human familial hypercholesterolemia and atherosclerosis. Infusion of Ang II resulted in mortality rates of 50% and 92% in the low- and high-Ang II groups, respectively, whereas there were no deaths in the vehicle group. Pathological analysis revealed that Ang II-infused Watanabe heritable hyperlipidemic rabbits that died showed myocardial infarction. Furthermore, Ang II-infused Watanabe heritable hyperlipidemic rabbits exhibited coronary plaque erosion and rupture that were associated with thrombosis. CONCLUSIONS: These findings suggest that increased blood levels of Ang II can destabilize coronary plaques and trigger the thrombosis, which possibly induces myocardial infarction. The model described in this study provides a novel means for the study of human acute coronary syndrome.


Assuntos
Angiotensina II/toxicidade , Doença da Artéria Coronariana/patologia , Vasos Coronários/efeitos dos fármacos , Hiperlipoproteinemia Tipo II/complicações , Infarto do Miocárdio/induzido quimicamente , Placa Aterosclerótica , Angiotensina II/administração & dosagem , Angiotensina II/sangue , Animais , Doença da Artéria Coronariana/genética , Vasos Coronários/patologia , Modelos Animais de Doenças , Predisposição Genética para Doença , Hereditariedade , Hiperlipoproteinemia Tipo II/genética , Bombas de Infusão Implantáveis , Infusões Subcutâneas , Infarto do Miocárdio/genética , Infarto do Miocárdio/patologia , Fenótipo , Coelhos , Fatores de Tempo
2.
Spectrochim Acta A Mol Biomol Spectrosc ; 291: 122369, 2023 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36657289

RESUMO

The development of multifunctional fluorescent chemosensors for the detection of multiple targets remains challenging but of great importance. In this paper, one novel coordination polymer (CP), denoted as [Cd2(edda)(phen)2]∙H2O (compound 1, H4edda = 5,5' (ethane-1,2-diylbis(oxy)) diisophthalic acid, phen = 1,10-phenanthroline) is successfully designed and prepared under hydrothermal conditions. Structural analysis indicates that compound 1 possesses a one-dimensional (1D) double chain structure, then self-assembles into a three-dimensional (3D) supramolecular framework via π…π interactions between phen molecules. Interestingly, compound 1 is found to be tolerant in wide range of acidic to alkaline aqueous solutions (pH = 2-13). Fluorescent spectral investigations reveal that compound 1 exhibits highly selective and sensitive fluorescence responses toward MnO4-, Cr(VI) ions, acetylacetone (acac) and ascorbic acid (AA) by fluorescence quenching in the aqueous phase. The detection limits are in the very low range, reaching µM level for the detection of MnO4-, Cr(VI) ions, nM for AA and ppm for acac detection. The distinguished multi-responsive performance suggests compound 1 to be a potential multifunctional probe. Furthermore, the possible quenching mechanisms have also been systematically investigated in this work.

3.
Spectrochim Acta A Mol Biomol Spectrosc ; 286: 121952, 2023 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-36228487

RESUMO

One novel cadmium(II)-coordination polymer [Cd3L2(datrz)(H2O)3] (CP 1) is controllably synthesized by surmising the astute combination of semi-rigid tricarboxylate acid 4-(2',3'-dicarboxylphenoxy) benzoic acid (H3L) and auxiliary ligand 3,5-diamino-1,2,4-triazole (datrz). Structure analysis shows that CP 1 has a two-dimensional (2D) layer structure with a 5-nodal (43) (44·62) (45·64·8) (45·6) (47·66·82) topology. Further investigations reveal that CP 1 shows superordinary water stability and good thermal stability. The fluorescent explorations suggest that the as-synthesized CP 1 could emit blue light centered at 485 nm, attributing to ligand-based emission. In terms of sensing investigations, CP 1 could act as a fluorescent sensor for detecting hypochlorite (ClO-) and acetylacetone (acac) through fluorescence turn-off process in aqueous solution, and the detection limit could reach 0.18 µM and 0.056 µM, respectively. Further research reveals that it is more likely the N-H···O-Cl hydrogen bonds between -NH2 groups of the triazole ligands and O atoms of ClO- plays the key role in the system, which may serve as a bridge for the energy transfer, leading to fluorescence quenching of the chemosensor. While the photoinduced electron transfer (PET) combined with inner filter effect (IFT) should be responsible for the turn-off fluorescence of CP 1 triggered by acac.


Assuntos
Ácido Hipocloroso , Água , Água/química , Cádmio/análise , Ligantes
4.
Spectrochim Acta A Mol Biomol Spectrosc ; 297: 122708, 2023 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-37043837

RESUMO

A water-stable ZnII-based coordination polymer (CP) with excellent photophysical behavior, namely [Zn2L(atez)(H2O)2] (compound 1; H3L = 4-(2',3'-dicarboxylphenoxy); atez = 5-aminotetrazole), was successfully prepared by the solvothermal reaction of Zn ions with a π-conjugated and semi-rigid multicarboxylate ligand H3L in the presence of N-containing linker atez. Compound 1 displays a hierarchically pillared three-dimensional (3D) (3,4,5)-connected (4·62) (42·64) (43·64·83) net which is based on two-dimensional (2D) multicarboxylate- ZnII layers strutted by the atez ligands. Sensing investigations of compound 1 reveal that this material can selectively and sensitively detect nitroaromatic compounds in water suspension through fluorescence quenching effect. In particular, it is worth noting that it shows highly specific detection of nitrobenzene (NB) and 2,4,6-trinitrophenol (TNP) with remarkable quenching constants (KSV = 7.5 × 104 M-1 for NB and KSV = 1.9 × 105 M-1 for TNP) and low limit of detection (LOD = 0.93 µM for NB and LOD = 0.36 µM for TNP). Investigations reveal that the probable mechanisms for such sensing processes are the concurrent presence of fluorescence resonance energy transfer (FRET) as well as photoinduced electron transfer (PET) between the CP and nitroaromatic molecules. This work not only offers an effective route to improve the application of fluorescent CPs but also provide one novel probable fluorescence probe for nitroaromatic compounds.

5.
Artigo em Inglês | MEDLINE | ID: mdl-36612382

RESUMO

A self-built house collapsed in Changsha City, Hunan Province, on 29 April 2022, causing 53 people to be trapped and 39 people to go missing. The tragedy caused a huge loss of life, so the stability of self-built houses has a non-negligible impaction on public safety. This report presents causes of the incident, rescue operations, cause analysis, and the analytic hierarchy process (AHP). The main conclusions about the reasons for the collapse include: (a) reckless heightening, (b) unreasonable structure, (c) adverse geological conditions, (d) architectural vulnerabilities, (e) negligence of competent authorities, and (f) lack of security awareness. This paper provides a reference for avoiding similar security incidents in the future.


Assuntos
Choque , Humanos , Cidades , China , Previsões
6.
Artigo em Inglês | MEDLINE | ID: mdl-36554884

RESUMO

This paper summarizes the cause of the debris flow impact train accident by investigating the local geological condition, meteorological data and field investigation that happened in Guizhou, China on 4 June 2022. The result showed that the major reason is the continuous heavy rain in the surrounding area, which led to a small landslide at the upper right of the tunnel entrance. Besides, the construction of the Jianrong Expressway in the upper reaches increased the catchment area, which makes the water content of the upper soil increase while the shear strength decreases. Such large-scale catastrophic accidents significantly threaten the local environment and public safety. Therefore, it is urgent to pay special attention to the changes in geological conditions along the line, especially the adverse effects of construction, to improve the early risk warning and post-accident treatment ability.


Assuntos
Acidentes , Solo , China
7.
Spectrochim Acta A Mol Biomol Spectrosc ; 242: 118750, 2020 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-32731144

RESUMO

Simultaneous high sensitivity detection of biomolecules is important for research in medicine, living cells and environmental samples. In this work, a water stable coordination polymer, [Cd2(bptc)(4,4'-bpy)(H2O)3]ˑH2O 1 (H4bptc = 2,3,3',4'-biphenyl tetracarboxylic acid, 4,4'-bpy = 4,4'-bipyridine), was designed and successfully synthesized as a luminescent sensor for simultaneous recognition of Ascorbic Acid (AA) and L-Tryptophan (L-Trp) based on luminescent -OFF and -ON, respectively. Importantly, the proposed sensing system showed an excellent performance with high KSV values of 4.85 × 104 M-1, 9.60 × 107 M-1 and low limit of detection (LOD) of 0.28 nM, 63 nM, respectively. In addition, the probable mechanisms are also discussed. The luminescent quenching behavior by AA can be mainly attributed to the static resonance energy transfer between complex 1 and the analytes. Whereas the enhancing effect of L-Trp comes from the intrinsic strong luminescence for L-Trp itself and photo-competitive mechanism between CP 1 sensor and L-Trp, supposedly. In addition, the repeatability of both systems were also investigated.


Assuntos
Ácido Ascórbico , Triptofano , Limite de Detecção , Luminescência , Polímeros
8.
Spectrochim Acta A Mol Biomol Spectrosc ; 229: 117915, 2020 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-31887675

RESUMO

A series of isostructural lanthanide coordination polymers (Ln-CPs), [Ln(Hbptc)(H2O)4]·H2O [Ln = Er (1), Pr (2), Dy (3), Sm (4), Gd (5), Nd (6) and Tb(7); H4bptc = 2,3,3',4'-biphenyl tetracarboxylic acid] have been isolated based on an unsymmetrical tetracarboxylic acid. Single-crystal X-ray diffraction analysis reveals that all CPs featured a two dimensional (2D) layer with (6, 6, 6)-connected 63 topology. Luminescent spectra demonstrate that CPs 1-7 exhibit impressive UV-visible luminescence in the solid state at room temperature. More significantly, a single-component white-light material with International Commission on Illumination (CIE) coordinates of (0.335, 0.334) for 4 (Sm-CP), very closing to the pure white-light of (0.333, 0.333) was obtained by finely tuning of the excitation wavelength. In addition, the luminescent detection for anions of 7 is investigated. Fluorescence measurements show that 7 can detect oxoanion pollutants Cr2O72-, CrO42-, and MnO4- anions in aqueous solutions with high selectivity and sensitivity, which suggests that the Tb-CP is a promising functional luminescence probe for toxic oxoanions. The possible mechanisms of the quenching effect were also discussed in detail.

9.
Ying Yong Sheng Tai Xue Bao ; 29(11): 3587-3595, 2018 Nov.
Artigo em Chinês | MEDLINE | ID: mdl-30460805

RESUMO

Reproductive isolation, the key process to prevent interspecific hybridization and keep the completeness and independence of species, is crucial to the formation and maintenance of biodiversity. The forming steps, methods and intensities of reproductive isolation between different species are not completely the same. Literatures on reproductive isolation between species provide valuable evidence for speciation and its maintenance. Flowering phenology, flowering-visiting insects, and pollen-stigma compatibility were observed for Ligularia virgaurea and L. sagitta, two species of weeds sympatrically distributed in eastern Qinghai-Tibet Plateau. The characteristics of reproductive isolation mechanism of both species and its role in reproductive isolation were also studied. The results showed that the flowering period of L. virgaurea was 20 d earlier than that of L. sagitta. Although the full-blooming period separated, there was a roughly 10 d overlap between the two species. Meanwhile, the pollens and stigmas of the two species were both viability in the overlapped 10 d. L. virgaurea and L. sagitta shared the same types of pollinating insects, which was a generalized pollination type. Besides, the flower-visiting behavior towards the two species from the pollinators was similar, along with the interleaved access between the two species. There was no complete time isolation and no complete pollinator isolation between the two species, but the stigma had poor compatibility towards heterogenic pollen. The germination of pollen on stigma and growth of the pollen tube was hampered. Furthermore, the rejection of pollen-stigma was likely to be an important prezygotic reproductive isolation between L. virgaurea and L. sagitta, thus avoiding the natural hybridization and maintaining the diversity and genetic stability of the two species.


Assuntos
Asteraceae/fisiologia , Isolamento Reprodutivo , Simpatria , Animais , China , Flores , Polinização , Tibet
10.
Spectrochim Acta A Mol Biomol Spectrosc ; 161: 138-43, 2016 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-26971022

RESUMO

A new 3-D Zn(2+) coordination polymer (CP) [(CH3)2NH2]3[Zn6(ox)4.5(trz)6]⋅4H2O (ox=oxalate; trz=1,2,4-triazolate) 1 was obtained by a simple solvothermal self-assembly. The crystal structural analysis demonstrates that the trz molecules link the Zn(2+) ions into a two-dimensional (2-D) layer network, which is based on the trinuclear Zn3(trz)6 clusters. The ox molecules serve as the linkers to propagate the 2-D layers into a three-dimensional (3-D) network of 1. The thermogravimetry (TG) behavior, photoluminescence property, and the sensing ability of 1 are investigated. The sensing experiment on nitrobenzene (NB) reveals that 1 can serve as a fluorescence probe to detect NB at the ppm concentration.

11.
Artigo em Inglês | MEDLINE | ID: mdl-27236205

RESUMO

By utilizing the hydrothermal in situ acylation of organic acids with N2H4, three acylhydrazidate-coordinated compounds [Mn(L1)2(H2O)2] (L1=2,3-quinolinedicarboxylhydrazidate; HL1=2,3-dihydropyridazino[4,5-b] quinoline-1,4-dione) 1, [Mn2(ox)(L2)2(H2O)6]·2H2O (L2=benzimidazolate-5,6-dicarboxylhydrazide; HL2=6,7-dihydro-1H-imidazo[4,5-g]phthalazine-5,8-dione; ox=oxalate) 2, and [Cd(HL3)(bpy)] (L3=4,5-di(3'-carboxylphenyl)phthalhydrazidate; H3L3=6,7-dihydro-1H-imidazo[4,5-g]phthalazine-5,8-dione; bpy=2,2'-bipyridine) 3, as well as two acylhydrazide molecules L4 (L4=oxepino[2,3,4-de:7,6,5-d'e']diphthalazine-4,10(5H,9H)-dione) 4 and L5 (L5=4,5-dibromophthalhydrazide; L5=6,7-dibromo-2,3-dihydrophthalazine-1,4-dione) 5 were obtained. X-ray single-crystal diffraction analysis reveals that (i) 1 only possesses a mononuclear structure, but it self-assembles into a 2-D supramolecular network via the NhydrazineH⋯Nhydrazine and OwH⋯Ohydroxylimino interactions; (ii) 2 exhibits a dinuclear structure. Ox acts as the linker, while L2 just serves as a terminal ligand; (iii) In 3, L3 acts as a 3-connected node to propagate the 7-coordinated Cd(2+) centers into a 1-D double-chain structure; (iv) 4 is a special acylhydrazide molecule. Two OH groups for the intermediates 3,3'-biphthalhydrazide further lose one water molecule to form 4; (v) 5 is a common monoacylhydrazide molecule. Via the NhydrazineH⋯Ohydrazine, OhydroxyliminoH⋯Oacylamino and the π⋯π interactions, it self-assembles into a 2-D supramolecular network. The photoluminescence analysis reveals that 4 emits light with the maxima at 510nm.

12.
Zhonghua Gan Zang Bing Za Zhi ; 13(11): 801-4, 2005 Nov.
Artigo em Chinês | MEDLINE | ID: mdl-16313719

RESUMO

OBJECTIVES: To establish a transplanted tumor producing HCV NS3 protein in mice and study the therapeutic effect of minigene vaccine based on invariant chain substitution. METHODS: SP2/0-NS3 cells expressing HCV NS3 antigen were injected subcutaneously into BALB/ c mice. After three days of inoculation, different therapeutical reagents were injected intramuscularly into different groups of mice. The boost immunization was carried out two weeks after the first immunization. The efficiency of HCV NS3 Th1 minigene vaccine was estimated after 60 days observation. RESULTS: For saline, pCI-neo, pHCV-NS3 and pHCV-NS3-Th1 treated groups, the induction period needed for tumor growth was 16.17+/-2.55, 14.40+/-1.82, 16.75+/-2.36, and 24.00+/-5.57 days (t =2.623, P =0.034 vs saline, t =3.713, P =0.010 vs pCI-neo and t =2.425, P =0.045 vs pHCV-NS3) respectively. The tumorigenesis rates were 100%, 100%, 57.1% (8/14, chi2 = 6.190, P = 0.013 vs saline and chi2 = 6.608, P = 0.010 vs pCI-neo) and 46.7% (7/15, chi2 = 9.707, P = 0.002 vs saline and chi2 = 10.311, P = 0.001 vs pCI-neo ) respectively. The survival rates were 0, 0, 50.0% (7/14, chi2 = 5.787, P = 0.016 vs saline and chi2 = 9.333, P = 0.002 vs pCI-neo) and 53.3% (8/15, chi2 = 6.651, P = 0.010 vs saline and chi2 = 10.311, P = 0.001 vs pCI-neo) respectively. The average tumor diameter of the pHCV-NS3-Th1 treated group was significantly smaller compared with the control groups and the pHCV-NS3 treated group (P =0.001). Moreover, the average survival time of tumor-bearing mice immunized with pHCV-NS3-Th1 was 6 days longer compared with the saline treated group, 12 days longer compared with the pCI-neo treated group (P =0.001), and 6 days compared with the pHCV-NS3 treated group. CONCLUSION: HCV NS3 Th1 epitope vaccine might be a potential biotherapy candidate against HCV infection.


Assuntos
Mieloma Múltiplo/metabolismo , Vacinas Sintéticas/uso terapêutico , Vacinas contra Hepatite Viral/uso terapêutico , Proteínas não Estruturais Virais/biossíntese , Animais , Feminino , Camundongos , Camundongos Endogâmicos BALB C , Mieloma Múltiplo/patologia , Transplante de Neoplasias , Distribuição Aleatória , Células Tumorais Cultivadas , Proteínas não Estruturais Virais/genética
14.
Dalton Trans ; 44(4): 1655-63, 2015 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-25436936

RESUMO

Under hydro(solvo)thermal conditions, two 4-(4-carboxyphenoxy)phthalate-based three-dimensional (3-D) coordination polymers: [Cd3(cpph)2(bpa)2(H2O)]·0.5H2O (cpph = 4-(4-carboxyphenoxy)phthalate, bpa = 1,2-bis(4-pyridyl)ethane) 1, and [H2(bpp)][Mn2(cpph)2(H2O)2] (bpp = 1,2-bis(4-piperidyl)propane) 2 were isolated. In both compounds, the cpph molecules extend the metal ions into a 3-D network: a (4,6)-connected net for 1 and a simple 6-connected net with a pcu topology for 2. The introduced bpa or bpp molecule stabilizes the 3-D metal-cpph architecture in the form of linker or guest molecule. The sensing ability of 1 was investigated, revealing that it can be used as a fluorescence probe to sense nitrobenzene at ppm concentrations.

15.
Chempluschem ; 80(12): 1732-1740, 2015 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31973329

RESUMO

5-(3',4'-Dicarboxylphenoxy)isophthalic acid (H4 L1) and 5-(2',3'-dicarboxylphenoxy)isophthalic acid (H4 L2) were reacted with Cd2+ salt with/without the assistance of N-donor ligands, creating five 3D CdII coordination polymers [Cd2 (L1)(H2 O)5 ]⋅H2 O (1), [Cd2 (L1)(bpe)(H2 O)] (bpe=1,2-bis(4-pyridyl)ethene; 2), [Cd2 (L1)(bpa)(H2 O)] (bpa=1,2-bis(4-pyridyl)ethane; 3), [Cd2 (L1)(bpp)] (bpp=1,3-bis(4-pyridyl)propane; 4), and [Cd2 (L2)(bpp)2 (H2 O)2 ]⋅H2 O (5). Crystal-structure analysis reveals 1) in 1, phthalate moieties for L1 link Cd1 centers into a 1D slightly helical chain; Cd2 centers act as bridges, linking 1D helical chains into a 3D network with a (3,5)-connected topology; 2) in 2-4, although Cd2+ centers were further modified by the introduction of organic bases, L1 molecules still link Cd2+ centers into 3D networks, which can all be simplified as pcu topology; 3) in 2-4, phthalate moieties first link Cd2+ centers into an oligomer, in which carboxylate-bridged discrete or rod-shaped secondary building units (SBUs) are found (tetranuclear SBU in 2 and 3, rod-shaped SBU in 4); and 4) in 5, L2 molecules link Cd2+ centers into a 2D (4,4) net; introduced bpp molecules serve as pillar linkers, extending Cd2+ -L2 layers into a 3D network of 5. The sensing abilities of 2-5 for nitrobenzene (NB) were investigated. Results revealed that they could all serve as fluorescence probes to sense NB at ppm concentrations.

16.
Dalton Trans ; 44(11): 5095-105, 2015 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-25669175

RESUMO

Under ambient conditions, reactions of CdCl2/Cd(CH3COO)2, SCN(-) and various organic amine molecules in strongly acidic solutions afforded the five new thiocyanatocadmates [H2(abpy)][CdCl2(SCN)2] (abpy = azobispyridine) 1, [H(apy)][Cd(SCN)3] (apy = 4-aminopyridine) 2, [H(ba)]2[CdCl2(SCN)2] (ba = tert-butylamine) 3, [H2(tmen)][Cd3Cl6(SCN)2] (tmen = N,N,N',N'-tetramethylethylenediamine) 4, and [H(dba)]2[Cd2(CH3COO)2(SCN)4] (dba = dibutylamine) 5. In compound 2 only, the CH3COO(-) ions in Cd(CH3COO)2 were completely displaced by SCN(-), producing a chained thiocyanatocadmate [Cd(SCN)3](-). In the other four compounds, the Cl(-) or CH3COO(-) ions appeared in the final inorganic anion frameworks. In compound 1, the Cl(-) ions doubly bridge the Cd(2+) centers, forming a one-dimensional (1-D) infinite chain, and the SCN(-) group exists in a terminal form, whereas in compound 3, the reverse situation is observed. Due to a trans-mode arrangement for two terminal Cl(-) or SCN(-) ions around each Cd(2+) center, the inorganic anion chains in compounds 1 and 3 both show a linear shape. In compound 4, Cd(2+) and Cl(-) first aggregate to form a 1-D endless chain with a composition of Cd3Cl6, which can be described as a linear arrangement of the open double cubanes. SCN(-) serves as the second connector, propagating the Cd3Cl6 chain into a three-dimensional (3-D) network with the occluded H2(tmen)(2+) cations. In compound 5, the SCN(-) groups doubly bridge the Cd(2+) centers, forming a 1-D zigzag-shape chain. The formation of the zigzag chain likely derives from chelation of the CH3COO(-) group to the Cd(2+) center. The thermal behavior and the photoluminescence properties of the title compounds were also investigated.

17.
Dalton Trans ; 43(41): 15617-27, 2014 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-25208479

RESUMO

By employing two types of hydrothermal in situ ligand reactions (acylation of N2H4 with aromatic polycarboxylic acids, reduction of 3-nitrophthalhydrazide by N2H4), three new acylhydrazidate-extended Zn(2+) coordination polymers [Zn2(3-apth)(atrz)2] (3-apth = 3-aminophthalhydrazidate; atrz = 3-amino-1,2,4-triazolate) 1, [Zn2(4-apth)(atez)2] (4-apth = 4-aminophthalhydrazidate; atez = 5-aminotetrazolate) 2, and [Zn(3-cppth)(H2O)] (3-cppth = 4-(3-carboxyphenoxy)phthalhydrazidate) 3 were obtained. X-ray single-crystal diffraction analysis revealed that (i) compound 1 possesses a 3-D structure. The triazolate molecules link the Zn(2+) ions to form a 2-D layer with a (6,3) topology. Then the acylhydrazidate molecule acts as the second linker, extending the (6,3) nets into a 3-D network of compound 1; (ii) compound 2 also exhibits a 3-D structure. The acylhydrazidate molecules first link the Zn(2+) ions into a 1-D infinite chain. The tetrazolate molecules propagate further the chains into a 3-D (4,4)-connected net (symbol: (4·6(4)·8)2(4(2)·6(2)·8(2))); (iii) compound 3 only shows a 1-D chain structure. The photoluminescence analysis indicates that the three title compounds all emit light, especially compound 2 which emits extremely strong blue light. The side group on the phthalhydrazidate molecule plays a crucial role in the emission behaviors of compounds 1-3. At 77 K, the activated compound 2 can adsorb N2 with a capacity of ca. 41.0 cm(3) g(-1).

18.
Dalton Trans ; 43(30): 11646-57, 2014 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-24946299

RESUMO

Under hydrothermal conditions, the reactions of Ba(2+)/Zn(2+), aromatic polycarboxylic acids and N2H4 with or without oxalic acid were carried out, affording four new acylhydrazidate-extended metal-organic frameworks (MOFs) [Ba(pmdh)] (pmdh = pyromellitdihydrazidate) 1, [Ba(sdpth)(H2O)2]·0.5H2O (sdpth = 4,4'-sulfoyldiphthalhydrazidate) 2, [Ba2(cpth)2(H2O)2] (cpth = 4-carboxylphthalhydrazidate) 3 and [Zn2(pdh)2(ox)]·H2O (ox = oxalate, pdh = pyridine-2,3-dicarboxylhydrazidate) 4. The acylhydrazidate molecules pmdh, sdpth, cpth and pdh in compounds 1-4 derived from the hydrothermal in situ acylation of N2H4 with aromatic polycarboxylic acids. X-ray single-crystal diffraction analysis revealed that (i) in compound 1, the pmdh I molecules link the Ba(2+) ions into a two-dimensional (2D) layer with a (4,4) topology, and then the pmdh II molecules extend these layers into a three-dimensional (3D) network; (ii) in compound 2, the sdpth molecules link the Ba(2+) ions to form a one-dimensional (1D) square tube. Interestingly, the tubes are further linked into a 3D supramolecular network via the N-H···O interactions, creating synchronously big channels; (iii) in compound 3, the cpth I molecules link the Ba1 ions into a 3D network with a (10,3) topology. Ba2 and cpth II are distributed on the channels; (iv) in compound 4, Zn(2+) and pdh aggregate to form two types of Zn4(pdh)4 clusters. The ox molecules act as the secondary linkers, extending the Zn4(pdh)4 secondary building units (SBUs) into a 3D network with a 6(6) topology. The photoluminescence analysis indicates that compounds 3 and 4 emit green light with maxima at 495 nm for 3 (λ(ex) = 397 nm), and 522 nm for 4 (λ(ex) = 395 nm), respectively. At 77 K, the activated 2 and 4 can adsorb N2 in amounts of 58.31 cm(3) g(-1) for 2 and 38.38 cm(3) g(-1) for 4, respectively.

19.
Dalton Trans ; 42(47): 16547-55, 2013 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-24065053

RESUMO

By employing the hydrothermal in situ acylation of N2H4 with aromatic polycarboxylic acids, three new acylhydrazidate-containing complexes [Zn(N2H4)(dphkh)]·H2O (dphkh = 4,4'-diphthalhydrazidatoketone hydrazone) 1, [Zn(npth)2] (npth = naphthalhydrazidate) 2 and [Mn(mpdh)2(H2O)2]·2H2O 4, and two new acylhydrazide molecules [bpth]·0.5H2O (bpth = 3,3'-biphthalhydrazide) 3 and [(chpth)2] (chpth = 4-chloro-5-hydrazinophthalhydrazide) 5 were obtained. It is noteworthy that (i) compound 1 is a layered Zn(2+) coordination polymer with a mixed ligand of dphkh and N2H4. The nucleophilic addition of the keto spacer with N2H4 also occurred, forming the ketone hydrazone; (ii) compound 2 is a unique example of a npth-extended coordination polymer, exhibiting a double-chain structure; (iii) apart from the acylation of N2H4 with dcpha (dcpha = 4,5-dichlorophthalic acid), one Cl was substituted by N2H4, generating a new monoacylhydrazide molecule of compound 5. The solid-state photoluminescence analysis revealed that compounds 1 and 5 exhibit strong luminescence with the maximum at 490 nm for 1 and 535 nm for 5, whereas compounds 2 and 3 show weaker emissions with the peaks at 510 nm for 2 and 440 nm for 3.

20.
Dalton Trans ; 42(18): 6429-39, 2013 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-23467616

RESUMO

With diverse multi-dentate N-heterocyclic/diamine molecules as the cations, the reactions between Cd(2+) and SCN(-) in C2H5OH/H2O solution acidified by H2SO4 created five new thiocyanatocadmates [H2(bim)][Cd(SCN)2(H2O)2]SO4 (bim = 2,2'-biimidazole) 1, [H2(pympip)]2[Cd2(SCN)4(SO4)2(H2O)4]·2H2O (pympip = 1-(2-pyrimidyl)piperazine) 2, [H2(tdpy)]2[Cd3(SCN)10] (tdpy = 4,4'-thiodipyridine) 3, [H2(badpm)][Cd(SCN)4] (badpm = 4,4'-biaminodiphenylmethane) 4 and [H2(pdma)][Cd2(SCN)4(SO4)] (pdma = 1,4-phenylenedimethanamine) 5. It is noteworthy that (i) in compounds 1, 2 and 5, SO4(2-) was incorporated into the organically templated thiocyanatocadmate frameworks; (ii) compound is a rare example, in which two types of chained thiocyanatocadmates are found, and (iii) compound shows an interesting layer structure, constructed up from the ribboned thiocyanatocadmates by µ2-mode SO4(2-). Photoluminescence analysis revealed that compounds 1, 2 and 5 in solid state emit blue light with the maximum at 425 nm for 1, 405 nm for 2 and 445 nm for 5, respectively.

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