Table of Content

10 March 2009, Volume 30 Issue 3

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高等学校化学学报2009年第30卷第3期目次

2009, 30(3):  0.  doi:

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下期目次预览

2009, 30(3):  0.  doi:

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综合评述

Analysis Laboratory Based on a Microfluidic Chip

LIN Bing-Cheng^*, QIN Jian-Hua^*

2009, 30(3):  433-445.  doi:

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This article provides an overview of the recent achievements of analysis laboratory on a microfluidic chip and their applications in molecular, cell and organism level based on the works mainly carried out in the authors laboratory. The chip fabrication capabilities have been extended into design and fabricate chips with higher degree of complexity in different materials, quartz, glass, PMMA, PDMS, and hydrogel etc. Various functional units such as sampling, separation, micro pumps/valves, droplet, membrane, SPE, PCR reaction, cell culture, sorting and lysis etc. were prepared and integrated. And these devices with higher degree of complexity and functional units have been demonstrated for a wide range of biomedical applications. Microfluidic devices built for drug metabolites and drug screening in cell and organism level were described in this review.


研究论文

Solvothermal Synthesis and Characterization of One-dimensional Chained Indium-Sulfate


TIAN Zhen-Fen¹, SONG Tian-You^1,2*, FAN Yong¹, HUANG Liang-Liang¹, WANG Li^1*

2009, 30(3):  446-449.  doi:

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A one-dimensional chained indium-sulfate (C₆H₂₂N₄)_0.5[In(OH)](SO₄)₂(1) was synthesized under solvothermal condition using triethylenetetramine(TETA) as the templated agent and characterized by IR spectroscopy, TG, ICP and elemental analyses, powder and single crystal X-ray diffraction analyses. Compound 1 crystallized in the monoclinic system, space group P2(1)/c with a=1.05240(3) nm, b=1.36802(4) nm, c=0.75295(2) nm, β=101.558(2)°, V=1.06204(5) nm³, Z=4, R₁ =0.0368, wR₂=0.0897, GOF=1.068. Its structure is built up by InO₄(OH)₂ octahedra and SO₄ tetrahedra by sharing their vertices to generate an one-dimensional anionic Tancoite-type chain. The one-dimensional chains are extended into three-dimensional supramolecular structure through the hydrogen bond interactions among the N atoms of TETA cations and O atoms of the anionic chains.


Thermal Stability and Optical Performance of CePO₄ Nanowires

YANG Ru^*, LI Yu-Shu, ZHONG Xu-Feng, LI Min

2009, 30(3):  450-455.  doi:

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The hexagonal and monoclinic monazite CePO₄ nanowires with a narrow range of diameter distribution and large aspect ratio were synthesized mildly through hydrothermal process at 150 ℃ using CeCl₃·7H₂O and H₃PO₄ as the raw materials. The crystal structure, micro-morphology, and photoluminescence of the nanowires were characterized by XRD, TEM, HRTEM, and UV spectrophotometer. The results indicate that the diameter of hexagonal CePO₄ nanowires is approximately 40 nm, the length is 3 μm, while the diameter of monoclinic(monazite) CePO₄ nanowires is approximately 50 nm, the length can reach 20 μm and the nanowires are of high purity, homogeneity and well crystallinty. The crystalline phase of CePO₄ nanowires can be controlled simply by changing the hydrothermal reaction time. The crystalline phase of CePO₄ nanowires changes from hexagonal to monoclinic monazite while the reaction time increases. With the increase of calcining temperature, the width of CePO₄ nanowires increases, and the samples remain 1D morphology even after calcined at 1000 ℃, indicating the good thermal stability of the nanowires. The intensity of UV excited emission decreases while the calcining temperature increases.

Novel Complicated Titanate Consisted of Three Sublattices

XU Yue-Hua^1*, JIANG Hai-Ying¹, FU Shuang¹, LI Ji-Xue¹, NAKAYAMA Noriaki², WANG Dan³, XU Jia-Ning¹, SONG Tian-You¹, FENG Shou-Hua¹


2009, 30(3):  456-459.  doi:

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A novel multisublattice compound, [Ni(OH)_1.115(H₂O)_0.885]_1.22(Ti_1.73O₄)·1.65H₂O, was hydrothermally synthesized with K_0.81Li_0.27Ti_1.73O₄ as the precursor. This compound was characterized by XRD, IR, TG-DTA and TEM. In this compound, the TiO₂ layers and Ni(OH)₂ layers alternately stack together along the c direction, and three sublattices were formed. One is TiO₂ sublattice, which is orthorhombic with possible space group Pmmm, the lattice parameters are a=0.3875 nm, b=0.2976 nm, c=2.288 nm and α=β=γ=90°. The other two are Ni(OH)₂ sublattices which have the same dimensions and symmetry, the lattice parameters are a=b=0.3140 nm, c=2.288 nm, α=β=90° and γ=120°. TiO₂ sublattice and Ni(OH)₂ sublattice are incommensurate in two dimensions in the ab plane. This result confirms that it is possible to design and synthesize more complicated misfit layered compounds based on the layered compounds by the soft chemical method.


Production Mechanism Study of Singlet Oxygen in Copper Ion-Catalyzed Curcumin Using Fluorimetric Method and Its Determination in the Presence of Superoxide Anion Radical

LÜ Qing-Luan, ZHANG Miao, YUE Ning-Ning, GONG Bin, WANG Huai-You^*

2009, 30(3):  460-464.  doi:

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The production mechanism of singlet oxygen(¹O₂) in the curcumin catalyzed by copper ion was studied using 1,3-diphenylisobenzofuran(DPBF) as a selective fluorescence probe. The absorption spectrum of curcumin(CUR) binding to copper ion demonstrated the formation of copper ion-CUR complexes. This complexes were further oxidized by H₂O₂ giving rise to singlet oxygen, which was similar to Haber-Weiss reaction. That the metal ions catalyzed curcumin to produce ¹O₂ was tested. Except for Cu²⁺ and Cu⁺-CUR systems, no detectable ¹O₂ was produced in other metal ion-CUR systems. A new method was found for determining ¹O₂ in the curcumin system by catalysis of Cu²⁺. A linear relationship was obtained between ΔI_F and the concentration of ¹O₂ in the range of 1.37×10^-8—3.66×10^-7 mol/L. The detection limit was 4.12×10^-9 mol/L.

Contents

New Two-photon Fluorescence Probe for Nuclear DNA Imaging

LIU Xin¹, LIU Heng^1*, JIA Peng-Fei¹, ZHANG Bo¹, WANG Jun-Jie², ZHAO Ning², ZHANG Yuan-Hong², YU Xiao-Qiang^2*

2009, 30(3):  465-467.  doi:

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A new two-photon fluorescence DNA probe, BMVEC, with bigger σ×Φ(1437 GM) was synthesized. The absorption titration shows that there is an interaction between BMVEC and DNA because the probe can intercalate the grooves in the double helix of DNA, which enhances its two-photon fluorescent intensity. Meanwhile the double-staining results in cancer cells by means of TPM demonstrate the exclusive nucleic labeling ability of BMVEC, and the positions and amounts of nuclei labeled by BMVEC are wholly the identical as those by DAPI. Moreover, the incident power of BMVEC is lower than that of DAPI. The results indicate that BMVEC can act as the two-photon fluorescent probe of DNA.

研究论文

Studies on Chemical Constituents of Leaves of Actinidia kolomikta Planch(Ⅱ)


LU Juan¹, LI Xu-Wen¹, GUI Ming-Yu¹, LIU Gui-Ying¹, ZHU Na¹, YU Ai-Min¹, OKUYAMA Toru², MASAKI Baba², JIN Yong-Ri^1*


2009, 30(3):  468-473.  doi:

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Four new acetylated flavonoids, 4'-methoxyl-quercetin-7-(4"-O-acetylrhamnosly)-3-O-β-D-glucopyranoside(1), kaempferide-7-O-(3"-O-acetylrhamnosyl)-3-O-rutinoside(2), kaempferol-7-O-(4"-O-acetylrhamnosyl)-3-O-rutinoside(3), 4'-methoxyl-quercetin-7-(4"-O-acetylrhamnosyl)-3-O-rutinoside(4) were isolated from the extracts of the leaves of Actinidia Kolomikta(Rupr.et Maxim.) Planch. Their structures were elucidated by application of chemical and spectroscopic analysis including HRESI-MS, ¹H-¹H COSY, HMQC and HMBC.


Preparation and Effects of Resveratrol Bovine Serum Albumin Nanoparticles on Proliferation of Human Ovarian Carcinoma Cell SKOV3

GUO Li-Yuan, YAO Jing-Ping, SUI Li-Hua^*

2009, 30(3):  474-477.  doi:

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Resveratrol bovine serum albumin nanoparticles(RES-BSANP) were synthesized by desolvation. HPLC and Atomic force microscopy(AFM) were employed to study the shape, mean size and particle distribution of RES-BSANP. MTT was used to detect the effects of RES and RES-BSANP on the growth rate of cell SKOV3 at various concentration of them, and flow cytometry(FCM) was applied to assaying the cell cycle and cell apoptosis of cells SKOV3. The results show that RES-BSANP are slick and uniformity, the average diameter of RES-BSANP is about 400—500 nm, drug loading is about 4.077 mg/12 mg, entrapment efficiency is 33.97％. MTT test shows the growth of SKOV3 can be significantly inhibited by RES and RES-BSANP in dose-dependence manner, while RES-BSANP is superior to RES at concentrations of 60, 100, 200 μmol/L(P<0.05). FCM test shows RES-BSANP make cells SKOV3 be in S phase and the apoptosis of cells SKOV3 more significant compared with RES. Therefore, RES-BSANP appears to be a very promising drug for anti-proliferation on human ovarian carcinoma.

Simple One-pot Synthesis of Triazine-porphyrins

XIAO Shen-Chu, ZHENG Liang-Bin, XIE Wen-Zhong, LIN Wei-Ying, LI Qing-Hong, GUO Can-Cheng^*


2009, 30(3):  478-482.  doi:

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A series of substituted triazine-tetraphenylporphyrins were synthesized from the reaction of 5-[4-(3,5-dichloro-triazine-1-oxygen)]phenyl-10,15,20-triphenylporphyrin with amines or alcohols. A new simple one-pot synthetic method from the reaction of the tetraphenylporphyrin with hydroxyl group and 2,4,6-trichloro-1,3,5-triazine and other nucleophiles was studied. The researches show that amines or alcohols substitute selectively the one of two chlorine atoms in 5-[4-(3,5-dichloro-triazine-1-oxygen)]phenyl-10,15,20-triphenylporphyrin under different conditions to yield the substituted triazine-tetraphenylporphyrins. The structures of the substituted triazine-tetraphenylporphyrins depend on the nucleophilicity, stereochemistry of the nucleophiles and the reaction temperatures. Seven new triazine-porphyrin compounds were synthesized from the reaction of 5-(4-hydroxyl)phenyl-10,15,20-triphenylporphyrin with 2,4,6-trichlorotriazine, amines or alcohols. Their structures were charactered with ¹H NMR, MS, UV-Vis and elemental analysis. 三嗪卟啉

Expression, Purification and Spectral Characterization of Recombinant Human Cytoglobin


TIAN Su-Yan¹, LI Lian-Zhi^1*, LI Hai-Li¹, XUE Ze-Chun¹, DU Wei-Hong²


2009, 30(3):  483-488.  doi:

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Cytoglobin(Cygb) is a recently discovered hemeprotein belonging to the globin superfamily toge-ther with hemoglobin, myoglobin and neuroglobin. It is distributed in almost all human tissues. Human cytoglobin is composed of 190 amino acid residues, displays a hexacoordination His-Fe-His in the absence of external ligands. In almost all the published literatures, Cygb was expressed in inclusion bodies and purified from this form. Herein, we expressed and purified recombinant human Cygb in soluble form and in inclusion bodies form, and comparely studied their spectral features and thermal stability. The soluble form protein was purified by ammonium sulfate precipitation, Hiprep 16/10 Q FF anion exchange column, Hiload 16/60 superdex 75 size exclusion chromatography and CM Sepharose Fast Flow cation exchange column. The inclusion bodies form protein was purified by dissolving in 6 mol/L guanidinium chloride, renatured with haemin solution and chromatography. ESI-MS results indicate that the molecular weight of the two forms of Cygb is diffe-rence with 153.0. The UV-Vis absorption spectra, fluorescence spectra and circular dichroism spectra show that the heme conformations in the two form cytoglobin proteins are different, and there exists difference between the two forms in their thermal stability.


Dynamic Observation of Cellular Localization of Fluorescein Isothiocyanate Labeled Recombinant Ganoderma Lucidum Immunoregulatory Protein(rLz-8) in NB4 APL Cell

LIANG Chong-Yang¹, XU Wei-Qing², CAO Yan-Xin², LIU Li-Xia³, ZHANG Shu-Qin¹, LIU Zhi-Yi¹, LI Hong-Rui¹, LI Bai-Zhi¹, SUN Fei^1*


2009, 30(3):  489-492.  doi:

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NB4 APL cell was induced apoptosis by Recombinant Ganoderma lucidum immunoregulatory protein(rLz-8) for the first time in this study. The dynamic cellular localization of FITC-rLz-8 was observed by laser scanning confocal microscope LSCM: identifying the receptors of cell membrane, entering into cell, gathering on nucleus finally. Annexin V-FITC kit was used for measuring apoptosis of NB4 by rLz-8. Results show that the effects of the dose group(0.5 μg/mL) is close to the one of positive control(As₂O₃). All data show that apoptosis inducing activity of rLz-8 in HL60 cells and changes of cell morphology and Ca²⁺ level in cytosol are probably interrelate with rLz-8's subcellular localization.

Synthesis and DNA-cleaving Function of Cyclotriphosphazene Polydentate Ligands


WANG Le¹, YE Yong^1*, ZHONG Shang-Bin¹, ZHANG Di¹, ZHAO Yu-Fen^1,2*

2009, 30(3):  493-496.  doi:

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A series of multinuclear cyclotriphosphazene ligands were synthesized and used as artificial nuclease enzyme model. All of these new compounds were confirmed by MS, ¹H NMR, ³¹P NMR, ¹³C NMR and IR. Preliminary studies on the cleavage of pUC19 DNA in the presence of metal complexes were performed. The results strongly suggest that the pUC19 DNA can be cleaved efficiently by these ligands. The effect of DNA cleavage with ligand 5b was also studied under different cleavage time.

Multi-walled Carbon Nanotubes Exposure Induces Oxidative Stress and Depolarizes Mitochondrial Membrane Potential in Cultured A549 Cells


YE She-Fang^1*, ZHONG Li-Ming¹, WU Yi-Hui¹, ZHANG Qi-Qing^1,2*


2009, 30(3):  497-501.  doi:

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The present study was undertaken to determinate the cytotoxicity exhibited via multi-walled carbon nanotubes(MWCNTs) in human A549 lung epithelial cells as a model system. Cell mortality was measured by methyl thiazolyl tetrazolium(MTT) assays. The morphological changes of A549 cells were examined by Hoechst 33342 staining. The level of reactive oxygen species(ROS) was detected by means of flow cytometry analysis with a redox-sensitive fluorescent probe 2',7'-dichlorfluorescein-diacetate(DCFH-DA).The mitochondria membrane potential was observed by a confocal laser-scanning microscope with JC-1 fluorescence. The heme oxygenase-1(HO-1) protein expression was analyzed by immunofluorescence and Western blotting. The result reveal that treatment of A549 cells with MWCNTs lead to loss of cell viability, ROS production, glutathione depletion and decline in mitochondrial membrane potential. MWCNTs were potent toward inducing cellular heme oxygenase-1(HO-1) expression, a sensitive biomarker for oxidative stress. Our observations suggest that MWCNTs exert toxicity by increasing oxidative stress, decreasing the mitochondrial membrane potential in cultured A549 cells.

New Method for the Preparation of Acetylenic Retinoids

LI Zhi-Zhang¹, GU Zheng², ZHANG Rong², WU Yun-Dong², WANG Xiao-Yong¹, JIANG Hai-Ming¹, XIANG Jian-Nan^2*

2009, 30(3):  502-505.  doi:

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Acetylenic RAs is a kind of important drug for treating cancer. In this paper, a novel acetylenic retinoids was synthesized and a directly copper-free Sonogashira coupling between iodoaryl acid and phenylacetylene was developed. In the absence of Cu(Ⅰ), the catalytic coupling of haloaryl carboxylic acids or unactivated aryl bromides with terminal alkynes were shown to occur in the presence of 10 multiple piperidine at 85 ℃ within 20 min with PdCl₂(PPh₃)₂ as catalyst in good yields. The overall yield was 72%. Due to the fact that the reaction is simple and the yield is high, it is applicable to synthesis of other acetylenic RAs.

Preparation and Characterization of Quantum Dots-anti-GSH Human scFvs Bioconjugations


XU Jun-Jie¹, WANG Shi-Wen¹, ZHAO Hong⁴, CHEN Gui-Qiu⁵, HUO Rui¹, TIAN Li¹, DUAN Yu-Jing¹, LI Min-Jie³, YANG Bai³, WEI Jing-Yan^1,2*


2009, 30(3):  506-509.  doi:

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In order to generate catalytic antibodies with glutathione peroxidase(GPX) activity, the clone B3 that bound specifically to glutathione(GSH) was selected from the phage display antibody library[human synthetic VH+VL single-chain Fv fragment(scFv) library] and the expression vector of scFv-B3 was constructed in previous study. The expression vector pPELB-B3 constructed was transformed into the Escherichia coli Rosetta to express the human anti-GSH single chain fragments variable(scFvs) antibodies. The scFv-B3 was purified by Ni2+-immobilized metal affinity chromatography(IMAC). 3-Mercaptopropyl acid-stabilized CdTe quantum dots synthesized in aqueous solution were used to conjugate with scFvs. Spectra analysis show that the fluorescent of QD-scFvs undergo a blue-shift in the emission peak, which suggest that the scFvs have been effectively bound to the scFvs, via covalent conjugation. It is also suggested by the result of the simple new method of dot blot. The results of membrane dot indicate that the QD-scFvs can specifically recognize the GSH. The status of the QD-scFvs acting on the MCF-7 cells was observed under fluorescence microscope. The results show that QD-scFvs can enter the cytoplasm across the membrane.


Synthesis of Isatin Derivatives and Their Inhibition Against AHAS

TAN Hai-Zhong, LI Hui-Dong, WANG Jian-Guo*, LI Wen-Ming, LI Yong-Hong, LI Zheng-Ming^*


2009, 30(3):  510-512.  doi:

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Based on the crystal structure of AHAS enzyme, bio-rational drug design was used to discover some novel AHAS inhibitors via computational virtual screening. Some isatin derivatives as AHAS inhibitors were designed, synthesized and evaluated. The preliminary results show that the isatin compounds exhibit conside-rate inhibition both in vivo and in vitro against AHAS. Compound 13 show an inhibition of 85% at 100 μg/mL concentration in vitro and compound 7 show an inhibition of 84.7% of rape root length at 100 μg/mL concentration. This discovery provides meaningful information for further design and synthesis of novel compounds with enhanced activity.


Electrochemical Synthesis of 2-Alkylidene-5-hydroxymethyltetrahedrofunans

ZHANG Cheng-Liang¹, LEI Ze^1,2, LIU Fu-Chu¹, ZHU Zheng-Hui¹, JIANG Ming-Zhong¹, ZHU Hong-You^1,2*

2009, 30(3):  513-516.  doi:

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The structural unit of 2-alkylidene-5-hydroxymethyltetrahydrofunan exists in some natural compounds such as the macrotetrolide antibiotics and the ocean natural products Sarcodictyin and Eleutherobin. These natural compounds usually show outstanding biological activities. In this work we decribed a totally new method for the constructing of this structural unit by employing indirect electrolysis, namely, using KI and NaI as the indirect electrolyte, water as solvent and reagent, the γ-alkylation products of β-Ketoesters as the starting material. Thirteen kinds of 2-alkylidene-5-hydroxymethyltetrahydrofunans were synthesized in high yields and good selectivity. The success of this method has not only provided a “clean technology” of indirect electrolysis but also prompted a simple, effective and environmental friendly green synthesis.

Proteomics Investigation of Mouse Hepatocarcinoma Cell Lines with Different Lymph Node Metastasis Capacities


SUN Ming-Zhong¹, LIU Shu-Qing², TANG Jian-Wu^3*

2009, 30(3):  517-524.  doi:

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Two mouse hepatocarcinoma ascites syngeneic cell lines, a Hca-F with lymph node metastasis rate of 75% and a Hca-P with low lymph node metastasis rate of 25%were established and well maintained in our laboratory. The different expressed proteins between the two cell lines were separated and compared with fluorescent two-dimensional difference gel electrophoresis(2D DIGE), the expression levels of differentially expressed proteins were quantified by DeCyder software and protein identifications of interested protein spots were performed via the high performance liquid chromatography-nano electrospray HPLC-nESI-MS/MS approach. Among the total 116 protein spots obtained by the 2D DIGE, 62 protein spots were observed up-regulated in Hca-F and 54 protein spots up-regulated in Hca-P cell lines, respectively. 109 unique proteins were identified from all the 116 different expressed protein spots. Part of the identified protein candidates have been reported to be associated with the occurrence, invasion and metastasis of a variety of tumors. However, most of the proteins identified in current were for the first time revealed to be involved in the mouse hepatocarcinoma due to the lymphatic metastasis.

Rapid Glycosylated Functionalization of Single-walled Carbon Nanotubes for Lectin Recognition


FU Qun, WU Ming-Hong^*, JIAO Zheng, WANG De-Qing

2009, 30(3):  525-529.  doi:

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Single-walled carbon nanotube(SWNT) was functionalized with N-n-octadecyl-D-maltonamide(NOMA), a simple sugar-containing amphipathic compound, by a method of noncovalent adsorption to form a NOMA-SWNT nanocomposite. The spectroscopic and morphology results show that NOMA could be rapidly and effectively adsorbed on the surface of SWNT without changing the native structure of NOMA and the structure properties of SWNT. Moreover, it was shown that the dispersion ability of SWNT in aqueous solution had a significant improvement after coating with NOMA. Field effect transistor(FET) devices with a NOMA-SWNT bundle as the conducting channel have been developed to detect maltose-Concanavalin A(Con A) interaction. Obvious changes in the Carbon nanotube field effect transistor(CNTFET) characteristics have been detected after NOMA functionalization and after Con A adsorption to the NOMA coating layer, which demenstrates the possobility of noncovalent glycosylated functionalization of SWNTs with simple molecue NOMA and sugar-lectin recognition detection by CNTFET. The presented method for functionalization of SWNT had several advantages, such as rapid and facile CNT functionalization, good hydrophilicity and biocompatibility, versatile detection of receptor via various glycoligand molecule, etc., and could be used for bio-functionalized materials, detection of carbohydrate-protein interactions and diagnose processes of deleterious disease.

Biomimetic Synthesis of Needle-shaped Nano-CaCO₃ Particles with L-Histidine as the Template


XIAO Yu-Peng¹, ZHAO Xu¹, ZHAO Li-Na¹, WU Xiao-Xia², LEI Hong¹, REN Su-Xia¹, WANG Zi-Chen^1*

2009, 30(3):  530-533.  doi:

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Based on the theory of biomimetic synthesis, well dispersed needle-shaped nano-CaCO₃ particles with an average width of 80 nm and a ratio of diameter to length about 1∶12 were synthesized via a simple precipitation reaction of Na₂CO₃ with CaCl₂ in the presence of L-histidine. The products were characterized by field emission scanning electron microscopy(FESEM), X-ray diffraction(XRD), fourier transform infrared spectroscopy(FTIR) and whiteness meter. The results show that needle-shaped nano-CaCO₃ crystals are obtained in the presence of L-histidine. Whereas, only cubic micron CaCO₃ crystals were obtained without L-histidine. Due to its nano-size, high oil-absorbed value and high whiteness, the needle-shaped nano-CaCO₃ particle was expected to be used as the filler for high-grade paper products, such as carbon paper, handkerchief paper, printing paper, etc.

Liquid-phase Preparation of DME Slurry Catalysts Using Pseudo-boehmite as Aluminum Source

GAO Zhi-Hua, HUANG Wei^*, LI Jun-Fang, YIN Li-Hua, XIE Ke-Chang


2009, 30(3):  534-538.  doi:

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Al-based slurry catalysts using pseudo-boehmite as aluminum source were prepared by a complete liquid-phase technology and the catalyst precursors were modified by different drying control chemical additives(DCCAs). The catalysts were characterized by means of X-ray diffraction, N₂ adsorption, X-ray photoelectron spectroscopy and H₂ temperature-programmed reduction. The performance of the catalysts was evaluated in a slurry reactor for the synthesis of dimethyl ether(DME) from syngas. The results indicate that using pseudo-boehmite as aluminum source there takes place a strong interaction between copper and aluminum, which induce the formation of CuAl₂O₄ and decrease the amount of reducible Cu₂O. Consequently, the catalyst activity is decreased. Further study shows that the DCCA influences significantly on catalyst's property. When the catalyst precursors are modified by glycerol as DCCA, the catalysts surface area and mean pore size are increased. The active component of the catalyst is dispersed uniformly and the formation of CuAl₂O₄ is suppressed, meanwhile, the reducible Cu₂O is increased. Therefore, the catalyst shows the highest space time yield and selectivity of dimethyl ether.

In situ FTIR Study on Photo-catalytic Degradation of Trichloroethylene over TiO2


JIANG Chuan-Rui1, ZHENG Chun-Li1, LI Xin-Yong1,2*, WANG Li-Yuan1, ZHANG Wen-Shuang1, CHEN Guo-Hua2

2009, 30(3):  539-543.  doi:

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Photo-degradation and gas-phase photocatalytic degradation on TiO2 of trichloroethy-lene were stu-died by in situ infrared spectroscopy. The results show that UV/TiO2 has a higher degradation capacity than UV on trichloroethylene. In the photocatalytic degradation process, dichloroacetyl chloride, carbon dioxide, carbon monoxide, water, hydrogen chloride and phosgene were detected. Base on the in situ FTIR spectra in different stages, the reaction mechanism of trichloroethylene photocatalysis on TiO2 was proposed: trichloroethylene was oxidized by hydroxyl radical and other free radical and formed to dichloroacetyl chloride. Finally, dichloroacetyl chloride was converted further to carbon dioxide, carbon monoxide, water, hydrogen chloride and phosgene.


Preparation and Gases Permeation Properties of Carbon Nanotubes Composite Membrane Supported by Porous Substrate


MI Wan-Liang^*, SU Qing-Quan

2009, 30(3):  544-548.  doi:

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Vertically aligned carbon nanotube(CNT) arrays were grown on porous Al₂O₃ substrate by improved floating catalysis method. Gaps among CNTs were sealed by polystyrene using spin-coating method, and then, the sample was prepared into carbon nanotube composite membrane. H₂ and CO₂ permeation through the prepared carbon nanotube membrane were studied. Experimental results show that the ideal selectivity of H₂/CO₂ increases with the decreasing of carbon nanotube diameter, it is higher than Knudsen limit in the membrane with smaller diameter carbon nanotubes, the ideal selectivity reaches to 6.25, gaining preferable separation results. Permeance of both gases slightly decreases when permeation temperature increases.

Effect of Anionic Dispersant on Rheological Properties of Acid-bentonite

LIANG Hu-Nan^1,2,3, LONG Zhu^1*, PI Cheng-Zhong², YANG Shu-Hui¹, ZHOU Xiao-Fan²

2009, 30(3):  549-552.  doi:

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The effect of anionic dispersant(sodium polyacrylate) on rheological properties for 10%(mass fraction) acid-bentonite dispersion were studied. The results show that, among dispersion containing dispersant dosage of 0.2%, 0.4%, 0.6% and 0.8%, respectively, the dispersion containing 0.4% dispersant has the lowest shear stress, apparent viscosity and yield stress. In range of studying shear rate, dispersion containing 0.4% dispersant exhibited dilatant characteristic and others transformed rheology from pseudoplastic to dilatant characteristic. The result also show that the rheograms fitting Herschel-Bulkley model are well. The mechanism of rheological properties on acid-bentonite dispersion was also discussed.

Electrochemistry of Microperoxidase-11(MP-11) on Glassy Carbon Electrode Modified with Chitosan


WANG Kun-Qi^1,3,4, MA Zhong-Su^1*, LU Tian-Hong³, XING Wei³, ZHU Lin³, LÜ Qiang¹, XING Shen-Yang²

2009, 30(3):  553-556.  doi:

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In this paper, microperoxidase-11(MP-11) was immobilized on glassy carbon electrode surface modified with chitosan by physical adsorption. The direct electrochemistry and the electrocatalytic behaviours to O₂ and the H₂O₂ of MP-11 on glassy carbon electrode modified with chitosan were characterized by cyclic voltammetry. The results indicate that MP-11 on modified electrode displays a quasi-reversible electrochemical process coupled with proton transfer in the phosphate buffer solutions(pH=7.12). Direct electrochemical reaction of MP-11 on modified electrode has been realized. MP-11 on modified electrode can catalyze reduction for O₂ and H₂O₂. Both of the catalytic reductions are surface-controlled electrochemical process. The response current of MP-11 on modified electrode to H₂O₂ is linear with hydrogen peroxide concentration. In a word, the electrode modified by chitosan as a matrix material can be used in the biofuell cell and biosensor in the future.

Preparation and Performance of Solid-state Electrochromic Devices Based on Polyaniline


CHEN Li-Xian², LU Yan-Ting², WENG Shao-Huang², ZHOU Jian-Zhang^1*, LIN Zhong-Hua¹


2009, 30(3):  557-562.  doi:

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In this paper, by polymeric electrolyte(PMMA-PC-EC-LiClO₄), we introduced CeO₂-TiO₂ composite as the complementary electrode of a new solid-state dual-type polyaniline electrochromic device(ECD). The electrochromic performance of the dual-type ECD was characterized using in situ UV-Vis spectroscopy. Compared to single-type ECD(ITOPANIPEITO), the dual-type ECD showed better electrochromic performance such as less response time, longer cyclic lifetime. Also, the composition of the electrolyte was found to influence the cyclic stability of PANI. The optimized dual-type ECD exhibited reversible electrochromic behavior from yellow at bleached state(-1.5 V) to blue at colored state(1.0 V PANI vs. CeO₂-TiO₂) with good cyclic stability. The transmittance of the ECD at 700 nm changed from 42.19% to 13.35% with a coloration efficiency of 152.1 cm²/C.

Volumetric Properties of Binary System C₆H₆-DMF at 293.15 K

HOU Hai-Yun^1*, PENG San-Jun², WANG Xiao-Xian¹, GENG Xin-Peng¹

2009, 30(3):  563-567.  doi:

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The densities of binary solution C₆H₆-DMF(benzene-N,N-dimethylformamide) at 293.15 K were measured by use of the Anton Paar vibrating-tube densimeter, the molar fractions of benzene for the binary solution is from 0 to 1. The apparent molar volumes of C₆H₆ and DMF in the binary system C₆H₆-DMF were separately calculated from the density data, and the optimized dependences between apparent molar volumes and molar fractions and mass fractions were also determined, respectively, by the nonlinear least-square Regression, and further more, the standard partial molar volumes and the molar volumes of C6H6 and DMF were also obtained from the functions limits. At the same time, the excess molar volumes for the binary solution were calculated and were fitted by the fourth-order Redlich-Kister equation well, so the Redlich-Kister coefficients and the excess molar volume extremum were obtained.

Water and Salts Molecular Simulation of Diffusion Process in Reverse Osmosis Membrane


LIU Qing-Zhi^1*, YANG Deng-Feng¹, HU Yang-Dong²

2009, 30(3):  568-572.  doi:

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In this paper, we used molecular dynamic simulation method to study the diffusion process and diffusion coefficient of small molecules in reverse osmosis membrane, and made an analysis and discussion of relationship between the membranous structure monomer and the diffusion coefficients of small molecules in membrane. Among the eight kinds of membranes, diffusion coefficent of water changed obviously in different membranes and the changing direction was in accordance with experimental values. In eight kinds of membranes we simulated, the diffusion coefficient value of Na⁺ and Cl^- had much difference. The movement of NaCl molecule was restricted by the ions which moves slowly. Diffusion process of salt molecule in the membrane was only restricted by the membrane species, without relationship with salt molecules itself. Movement of molecule of water was not affected by the kinds of salt molecules in the same membrane.

Two Photon Absorption Property of a PPV Oligomer with Central Biphenyl Bridge and Peripheral Carbazole Substituents


JIN Jia-Ke, SONG Xue-Liang, LI Han-Ying, WANG Mang, SUN Jing-Zhi^*

2009, 30(3):  573-576.  doi:

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The effect of cruciform structure on the two photon absorption action cross-section of fluorescence chromophore was reported. 1,4-Di(9'-ethyl-carbazolyl)- 3'-vinylbenzene(R1) is a classic two photon absorption(TPA) chromophore with D-π-D structure. By linking two TPA chains with a biphenyl bridge, the obtained cruciform molecule(1) exhibits evidently larger two photon absorption action cross-section(σ') than its single-chain counterpart. For example, in 10^-4 mol/L toluene solution, cruciform 1 shows a σ' value of 491.0×10^-50 cm⁴·s, while the σ' value of R1 is only 137.5×10^-50 cm⁴·s. The amplification of σ' was ascribed to the cruciform structure, which rendered the TPA chromophores with cross dipole arrangement and curbed the fluorescence quenching in concentrated solutions.

Structure-Property Investigation on TDNAZ·HNO₃ and DNAZ·HCl

GAO Rong^1,2, MA Hai-Xia^1*, YAN Biao¹, SONG Ji-Rong¹, WANG Ying-Hui¹

2009, 30(3):  577-582.  doi:

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1,3,3-Trinitroazetidine(TNAZ) is one of famous insensitive and high energetic materials, which can be synthesized by 3,3-dinitroazetidine(DNAZ). N-Tertiarybutyl-3,3-dinitroazetidine nitrate(TDNAZ·HNO₃) and 3,3-dinitroazetidine hydrochloride(DNAZ·HCl) were synthesized during the process of synthesizing DNAZ. Single crystals suitable for X-ray measurement were obtained. TDNAZ·HNO₃ crystallizes in the orthorhombic system, space group Pnma with unit cell parameters a=1.2697(3) nm, b=0.8179(2) nm, c=1.1621(3) nm, V=1.2067 nm³ , Z=4. DNAZ·HCl crystallizes in the orthorhombic system, space group Cmc2₁ with unit cell parameters a=0.6681(2) nm, b=1.0441(2) nm, c=0.9971(2) nm, V=0.6955 nm³, Z=4. The Density-Functional Theory(DFT) method was used to calculate the geometry and frequencies of the two intermediates. The geometry, Hishfeld charges of atoms, Mayer bond orders, frontier orbital energy and the main atomic orbital percentage were calculated. The corresponding reaction mechanism was explained based on the molecular and electronic structural information. The thermal stability was also compared by their thermal behavior.

Density Functional Study of the Properties of CO Adsorption on SnO₂(110) Surface


XUE Yan-Bing^1,2*, TANG Zhen-An¹

2009, 30(3):  583-587.  doi:

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Based on density functional theory in the generalized gradient approximation, together with the total energy plane-wave Pseudopotential, adopted a six-layers periodic slab model, four modes of CO adsorption on SnO₂ (110) surface were calculated and the surface property modifications due to CO adsorption were investigated. The results indicate that the most stable adsorption mode is associated to the CO with the C-end oriented to the five-coordinated Sn ion, and this adsorption mode improves the relaxation of the surface. The distribution of the electronic states of surface has no remarkable change after CO adsorption, but the Fermi level has 1.06 eV shift to a high-energy direction. Adsorption resulted in a 0.07 electron transfer from CO molecule to the surface, which causes the decrease of the surface resistance. The present results favor the surface conduc-tance model of the sensitive mechanism of gas sensors.

Theoretical Investigations of Electric Field Effect on the Hydrogen Bonding and Electron Transport in DNA Base Pairs


XU Zhong¹, LI Ning¹, CUI Yan-Ping¹, LIU Hong-Mei², WANG Hong-Bo¹, YE Yuan-Feng², ZHAO Jian-Wei^2*

2009, 30(3):  588-592.  doi:

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The theoretical investigations on the molecular geometry and electronic structure of the DNA base pairs A-T were carried out at B3LYP/6-31+G**//HF/6-31+G** level, with the influence of external electric field. The results show that the electric field affects hydrogen bonding and the binding energy. In addition, the electron transport calculation has also been performed by density functional method with non-equili-brium Green's function formalism. Slight molecular rectification has been observed and the favorite direction for electron transfer is from T to A.

Polarization Dependence of Surface-enhanced Raman Spectroscopy on Single Fe₂O₃@Au Particle

SHEN Hong-Xia^1,2, YAO Jian-Lin^1*, ZOU Wen-Jun¹, GU Ren-Ao^1*

2009, 30(3):  593-595.  doi:

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The core-shell Fe₂O₃@Au particle with spindle morphology were synthesized by three steps. The mean size of the core-shell paricles was about 500 nm by 85 nm. The final single separated spindle particles were attached onto Si substrates. The thiophenol(TP) was served as probe molecule to investigate the pola-rized dependent surface-enhanced Raman scattering(SERS) from single particle. Dramatic variations in SERS intensity was observed when the single core-shell particle was oriented at different angles relative to the polarization of excitation laser. The maximum SERS intensity was detected for TP absorbed on the anisotropic particle which was in the polarization direction parallel to the long axis of the particle, while the minimum intensity was detected at the direction of the incident field that is perpendicular to the long axis of the particle. Our preliminary results provided useful way for obtaining deeper insight to the SERS mechanism.

Influence of Carbon Dioxide on the Polymerization Behavior of Sodium Silicate-acrylamide Solution and Products Properties


ZHAO Ren-Bao

2009, 30(3):  596-600.  doi:

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The polymerization behavior of acrylamide at its low concentration in sodium silicate solution under different pressure of carbon dioxide was studied. The microstructure and rheological properties of the synthetic products were characterized by environmental scanning electron microscope(ESEM), rheometer and laser particle sizer. A mixture is produced in experiments and will have larger storage modulus or viscoelasticity at a higher CO₂ concentration. It has a complex network structure formed by silicic acid gel embedded into polyacrylamide gel. After detaching from the mixture when exposed to ultrasonic wave, the silicate granules have a particle size distribution range of 280—900 nm, and their average size becomes smaller with the increase of exposure time. The mechanisms is that carbon dioxide helps increase both the diffusion velocity of AM molecule and also contact chance among the AM and initiator and crosslinking agent, which could enhance the molecule weight of the products.

Physical and Chemical Mechanism of Mechanical Mixing of Powder Styrene-butadiene Rubber Composites Filled with High Contents of Carbon Nanotubes


ZHOU Xiang-Wen^1,2*, ZHU Yue-Feng², XIONG Guo-Ping², LIANG Ji², YU Su-Yuan¹

2009, 30(3):  601-606.  doi:

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Carbon nanotubes(CNTs)/styrene-butadiene rubber(SBR) composite powders prepared by spray drying method was mechanically mixed with a two-roller open mixer. Influences of the mechanical mixing on the mechanical properties of the composites were investigated and the theoretical mechanism of such influences was analyzed. The results show that mechanical mixing effectively enhance the mechanical properties of CNTs/SBR composites particularly for those with high content of CNTs which are much better than those filled with the same content of carbon black. CNTs could be further dispersed homogeneously in the matrix through mechanical mixing. On the other hand, because of large shear force during the mixing process and the formed free functional groups, the interactions between CNTs and the rubber matrix such as physical absorption, hydrogen bonding and chemical bonding were improved that increased the combined rubber contents of the composites. Correspondingly CNTs could be more efficient in strengthening the SBR. Therefore the tensile and tear strengths of the composites were improved after the mechanical mixing. The strengthening effect of CNTs in SBR probably accorded with the “strong and weak bonding” mechanism.

Synchronistic Synthesis and Immobilization of Phenyl Porpherin on Crosslinked Polystyrene Microspheres


ZHANG Guo-Hai, GAO Bao-Jiao^*, WANG Rui-Xin, WANG Fei-Yu

2009, 30(3):  607-612.  doi:

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Synchronistic synthesis and immobilization of phenyl porpherin on crosslinked polystyrene microspheres(CPS) were realized successfully using benzaldehade, pyrrole and the microspheres HBA-CPS, on which hydroxyl benzaldehyde was bound, as the reactants and with Adler method, and the microspheres PP-CPS, on which phenyl porphyrin (PP) was immobilized, was prepared. In this investigation, the effects of the main factors on the process of synchronistic synthesis and immobilization of phenyl porpherin were studied. The coordination reaction between the microspheres PP-CPS and cobalt salt was also conducted, and the functional microspheres CoP-CPS, on which cobalt porphyrin (CoP) was immobilized, was obtained. The catalytic activity of CoP-CPS for the oxidation of ethyl benzene by dioxygen was examined. The experimental results show that the synchronistic synthesis and immobilization of phenyl porpherin on crosslinked polystyrene microspheres (CPS) can be carried out by the microspheres HBA-CPS, benzaldehade and pyrrole as reactants via the Adler reaction between solid phase and liquid phase. This is a new route to prepare immobilized porphyrin. In the process of the synchronistic synthesis and immobilization of porpherin, the acidity of the catalysts and the polarity of the solvents affect the synchronistic synthesis and immobilization of porpherin greatly. As the catalyst with a pK_a value in the region of 2.8—3.4 is used, the microspheres PP-CPS with a higher immobilization amount of porphyrin will be obtained. When the solvent with higher polarity is used, the obtained microspheres PP-CPS have a higher immobilization amount of porphyrin. The microspheres CoP-CPS have obvious catalytic activity in the oxidation reaction of ethyl benzene by dioxygen.

Lysine Immobilization Through Poly(ethylene glycol) Spacer for Bloodcompatible Polyurethane Surface


HU Xiao-Yang¹, ZHANG Yan-Xia¹, ZHANG Tao², YU Qian¹, CHEN Hong^1*

2009, 30(3):  613-617.  doi:

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A blood-compatible polyurethane surface was prepared by multiply steps surface modification. ε-Lysine was conjugated to polyurethane surface through PEG spacer via Schiff-base and reduce reaction. The results of water contact angle and XPS measurements suggest that both PEG and lysine are immobilized to the surface successfully. Protein adsorption and plasma clot lysis measurements were performed to investigate the bloodcompatibility of the modified surface. Comparing with the unmodified surface, ε-lysine modified surface reduced fibrinogen adsorption by 80%. It was shown in clot lysis experiment that the ε-lysine modified surface could break down the incipient fibrinous clot within 13 min. The results demonstrate that ε-lysine modified surface not only suppress non-specific protein adsorption, but also degrade fibrin in an evolving clot.

Modification of PTFE Fiber and Its Adsorption Property for Bilirubin

HAN Xiao-Yan^1,2, ZHANG Zheng-Pu^1*

2009, 30(3):  618-624.  doi:

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The adsorbent of bilirubin based on polytetrafluoroethylene(PTFE) fiber was prepared by ⁶⁰Co radiation-induced graft polymerization with GMA and by subsequent chemical modification of the epoxy group of PTFE-g-GMA fiber with PEI. The highest amino content on the PTFE-g-GMA-PEI fiber is 1.87 mmol /g. The effect of pH, ionic strength, temperature, BSA, initial bilirubin concentration and adsorption dynamics on the adsorption capacity of PTFE-g-GMA-PEI fiber for bilirubin were investigated in a batch system. Experimental data indicate that the adsorption capacity of the grafted fiber is greatly affected by the pH of the medium, and in near neutral solution of pH=6.5, the grafted fiber have the highest adsorption capacity(9.6 mg/g). The bilirubin adsorption on the PTFE-g-GMA-PEI fiber obeyed the Langmuir model. Besides, the PTFE-g-GMA-PEI fiber has the considerablely competitive ability to combine bilirubin with BSA.

Preparation and Property of Chitosan/Sodium Tripolyphosphate Microcapsules as Drug Carrier


YANG Wen-Jing, WANG Ting, HE Nong-Yue^*

2009, 30(3):  625-628.  doi:

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Chitosan/sodium tripolyphosphate(CS/TPP) nano-sized microcapsules were prepared with ionic gelation of CS with TPP. The obtained CS nano-sized microcapsules were characterized with the infrared spectra(IR), scanning electron microscope(SEM) and the particle size analyzer. The model protein, bovine serum albumin(BSA) as a model drug, was encapsulated into the CS/TPP nano-sized microcapsules. Infrared spectrum of CS/TPP nano-sized microcapsules indicated that CS was cross-linked with TPP. The average diameter of the obtained nano-sized microcapsules was around 430 nm, and a homogeneous size distribution and good dispersion were observed. BSA-loading efficiency of CS/TPP nano-sized microcapsules did not increase with the increase in concentration of CS. When mass fraction of CS was 0.25%, the highest BSA-loading efficiency of CS/TPP nano-sized microcapsules reached 79.74%, while BSA continually and smoothly released up to one week.

Synthesis and Fluorescent Properties of Dendrimer PAMAM(1G)-FCD

HAN Qiao-Rong^1,2, WANG Bing-Xiang², HE Xu-Min^1*, DING Ma-Tai¹, XIA Hai-Ping¹

2009, 30(3):  629-631.  doi:

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A dendrimer of PAMAM(1G)-FCD was synthesized. Its structure was characterized via IR, ¹H NMR, MALDI-TOF-MS, etc. The fluorescent properties of PAMAM(1G)-FCD, as well as the influence of Sn²⁺ on this dendrimer, were also studied systematically. The results show that the fluorescence of this dendrimer can be significantly enhanced by Sn²⁺. The UV spectra detected a new absorption peak at 360 nm with the addition of Sn²⁺ into the solution of PAMAM(1G)-FCD, suggesting that chemical reaction occured in the Sn²⁺ and PAMAM(1G)-FCD system. This hybrid material of metal-dendrimer holds promise as a scarce material to emit blue fluorescence.

Molecular Inclusion Complexation and Recognition Behavior of Amphiphilic Hyperbranched Polymer Carrying β-Cyclodextrin as Pendant Groups on Shell Layer

TIAN Wei, FAN Xiao-Dong^*, LIU Tao, LIU Yu-Yang, SUN Le, JIANG Min, HUANG Yi

2009, 30(3):  632-637.  doi:

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The molecular inclusion complexation and recognition behavior of amphiphilic hyperbranched polymers with β-cyclodextrin as pendant groups on the shell layer were determined by UV-Vis spectroscopy in bu-ffer solution(pH=11) at 25 ℃. The results indicate that these polymers posses double inclusion capabilities from both β-cyclodextrin and amphiphilic hyperbranched polymer, and also can form inclusion complexation with single-guest, including phenolphthalein, methyl orange, and 4-nitrophenol, respectively. Furthermore, these polymers possess much stronger inclusion capability than that of single β-cyclodextrin or amphiphilic hyperbranched polymer. On the other hand, these polymers show double recognition behavior when methyl orange solution is added dropwise into phenolphthalein solution containing polymers. The phenomenon can be attributed to the existence of the different cavities from both β-cyclodextrin and hyperbranched polymer. In addition, the double-guest inclusion behavior of these polymers was also studied via selecting a complex guests system of phenolphthalein and methyl orange.

Cation Exchange Reaction of Poly(lithium acrylate) with 1-Butyl-3-methylimidazolium Bromide


ZHANG Xiao-Meng¹, LI Jun^1*, LIU Zheng-Ping^2*, ZHANG Li-Xin¹

2009, 30(3):  638-642.  doi:

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A new kind of conducting random copolymer of lithium acrylate with 1-butyl-3-methylimidazolium acrylate[P(AALi-BmimAA)] was prepared by the cation exchange reaction of PAALi with 1-butyl-3-methylimidazolium bromine ionic liquid. As a result, well-ordered structure of poly(lithium acrylate)(PAALi) was destroyed by introducing the 1-butyl-3-methylimidazolium cation and the formed copolymers had lower T_g and more than PAALi. Thus, the ionic conductivity of copolymer became higher than PAALi. The highest ionic conductivity of copolymer is 1.44×10^-8 S/cm which is higher than that of PAALi in three orders of magnitude. After mixing with LiTFSI, the ionic conductivity of copolymer increased two orders of magnitude to 2.90×10^-6 S/cm again.