CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
 
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2015 Vol.31 No.1
 Published: 01 January 2015

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Chemical Research in Chinese Universities Vol.31 No.1 February 2015
2015 Vol. 31 (1): 0-0 [Abstract] ( 8 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi:

Letter
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LIU Yang, LI Dongze, ZHANG Ying, LIU Zhihui, XIE Renguo
Greener Gd-doped ZnAgInS3 Quantum Dots for Fluorescent and Magnetic Resonance Imaging Applications
2015 Vol. 31 (1): 1-3 [Abstract] ( 12 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4344-7

Articles
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LIU Yabing, DUAN Weijie, CUI Xiaobing, XU Jiqing
Hydrothermal Syntheses and Characterization of Two 1D Chain Complexes and Tetra-capped Keggin Clusters
2015 Vol. 31 (1): 4-8 [Abstract] ( 11 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4325-x

Two new compounds, [Ni(en)2]{[Ni(en)2]2[MoVI6MoV2VIV8O40(SiO4)]}[(NH2)2(C2H4)2NH]·2H2O(1) and [Ni(en)2]{[Ni(en)2]2[MoVI5MoV3VIV8O40(VO4)]}(en)·H2O(2)(en=ethylenediamine), have been hydrothermally synthesized and characterized by elemental analysis, infrared(IR), X-ray photoelectron spectroscopy(XPS), electron spin-resonance(ESR) and thermogravimetric(TG) analysis and single-crystal X-ray diffraction(XRD) analysis. Both the compounds exhibit a 1D chain composed of bi-supporting tetra-capped Keggin clusters and nickle coordination fragments. The 1D chains are further assembled into a 3D supramolecular network with different packing modes via hydrogen bonds. The magnetic susceptibility of compound 1 demonstrates the presence of antiferromagnetic interactions.

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YANG Yu, XU Wenyan, HU Yanjing, WANG Lei, HUANG Keke
Multi-component Hydrogen-bonding Organic Salts Formed from 1-Methylpiperazine with Aromatic Carboxylic Acids: Synthons Cooperation and Crystal Structures
2015 Vol. 31 (1): 9-15 [Abstract] ( 16 ) [HTML 1KB] [PDF 0KB] ( 6 )   
doi: 10.1007/s40242-015-4304-2

1-Methylpiperazine was employed to crystallize with 2,4-dihydroxybenzoic acid and 1,8-naphthalene acid, affording two multi-component hydrogen-bonding salts [(C5H14N2)2+·(C7H5O4)2-·H2O](1) and [(C5H14N2)2+(C12H6O4)2ˉ·2H2O](2). These two forms of salts are both monoclinic systems with space group P21/c(14). The lattice parameters of salts 1 and 2 are a=1.32666(10) nm, b=0.90527(7) nm, c=1.67107(13) nm, β=103.125(1)° and a=1.4950(2) nm, b=0.75242(15) nm, c=1.6563(3) nm, β=92.834(2)°, respectively. Expected classical hydrogen bonds N―H…O and O―H…O appear in the chargetransfer salts, and asymmetric units of these two forms both contain water molecules which play a significant role in building novel supramolecular architectures. Robust hydrogen-bond interactions between 1-methylpiperazine and aromatic acid provide sufficient driving force to direct the two crystals to three-dimensional structures. Weak interactions C―H…O emerging in salts 1 and 2 further enhance their crystal structures. As a consequence, hydrogen-bonding interactions in these compounds afford diverse 3D net supramolecular architectures. Thermal stability of these compounds was investigated by thermogravimetric analysis(TGA).

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Mouna SMIDA, Hager LITAIEM, Mohamed DAMMAK, Santiago GARCIA-GRANDA
Structure, Thermal Behavior and Characterization of a New Hybrid Iron Fluoride FeF4(2,2'-bipyridine)(H2O)2
2015 Vol. 31 (1): 16-20 [Abstract] ( 14 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4171-x

New crystal of FeF4(2,2'-bipyridine)(H2O)2 was prepared by hydrothermal synthesis. Crystalline structure determination is performed from single crystal X-ray diffraction data. The unit cell is monoclinic space group P21/n, with cell parameters a=0.9046(5) nm, b=0.7502(5) nm, c=1.9539(5) nm, β=93.307(5)°, V=1.3238(12) nm3 and Z=4. The structure of FeF4(2,2'-bipyridine)(H2O)2 is built up from FeF4N2 octahedra coordinated by two nitrogen atoms of the 2,2'-bipyridine molecules, and four fluorine atoms as well as uncoordinated H2O molecules. Thermal analysis of the title compound showed that the decomposition introduced four steps. IR spectra confirmed the presence of 2,2'-bipyridine molecules. The optical absorption was measured at the corresponding lmax using UV-Vis diffuse reflectance spectrum.

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ZHAO Yueming, SONG Lina, LI Lingxia, LI Xiao'ou, SHI Qinghong, HONG Xin, GUO Jia, FANG Ling, HE Chengyan, LI Hongjun, ZHAO Haifeng
Mass Spectrometric Analysis Revealing Phosphorylation Modifications of Periostin
2015 Vol. 31 (1): 21-24 [Abstract] ( 1 ) [HTML 1KB] [PDF 0KB] ( 1 )   
doi: 10.1007/s40242-014-4317-2

Human periostin was over-expressed in HEK293T cells, which was enriched by nickel ion affinity resin, and further purified by gel electrophoresis. Phosphopeptides contained in the tryptic digestion of the purified periostin were enriched by TiO2 affinity chromatography, and then analyzed by liquid chromatography-tandem mass spectrometry(LC-MS/MS). LC-MS/MS analysis reveals three phosphorylation modification sites of periostin at IKVIEGpSLQPIIK(682―694), pSLHEKLKQDK(498―507) and p[TT]VLYEC*C*PGYM*R(73―85). The established method could be a great help to profiling the phosphorylation status of periostin under different physiological environments, such as inflammatory and tumor micro-environments.

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LIU Chunyu, WANG Shaoyan, FU Cuicui, LI Haibo, XU Shuping, XU Weiqing
Preparation of Surface-enhanced Raman Scattering(SERS)-active Optical Fiber Sensor by Laser-induced Ag Deposition and Its Application in Bioidentification of Biotin/Avidin
2015 Vol. 31 (1): 25-30 [Abstract] ( 7 ) [HTML 1KB] [PDF 0KB] ( 5 )   
doi: 10.1007/s40242-015-4294-0

A surface-enhanced Raman scattering(SERS) optical fiber sensor was prepared by the laser-induced deposition of Ag nanoparticle membrane on a silica optical fiber tip, which was applied to the real time SERS spectral monitoring on the biorecognition of biotin/avidin. The bioidentification of biotin/avidin was carried out through a indirect method, in which the bioidentification is based on the SERS response signal of a labeled dye(Atto610) after its fluorescence has been quenched totally by the deposited Ag nanoparticle membrane. By SERS monitoring the bioidentification process of biotin/avidin, it has been found that this recognition process is finished in 40 min. The lowest detection concentration of biotin is 1.0×10-7 mg/mL. This research is promising in the application of immunoassays on line and in vivo.

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GE Shun, ZHAO Ying, SUI Beibei, SHANGGUAN Guoqiang
Studies on the Interaction of Novel Organogermanium Sesquioxides with DNA
2015 Vol. 31 (1): 31-37 [Abstract] ( 2 ) [HTML 1KB] [PDF 0KB] ( 1 )   
doi: 10.1007/s40242-015-4198-z

The affinity and mode of interaction of four novel organogermanium sesquioxides with calf thymus DNA(CT-DNA) and two synthetic oligonucleotides, d(AT)22d(AT)22 and d(GC)22d(GC)22, were investigated by a combination of absorption spectroscopy, DNA thermal denaturalization method, viscosity method, fluorometric technique, and competitive binding study with ethidium bromide(EB). The results show that the organogermanium compounds can interact with DNA by intercalation, the binding ability of the compounds to CT-DNA and the synthetic oligonucleotides was found to be modest(in comparison to the proven intercalators), with binding constants on the order of 103―105 L/mol, respectively. Generally, the binding of the organogermanium sesquioxides with naphthalene moiety to DNA is stronger than that of the compounds with anthraquinone moiety. And the compounds with anthraquinone moiety have preference for binding to AT-rich duplexes, whereas the compounds with naphthalene moiety have a little preference for binding to GC-rich duplexes. DNA may be the primary effect target.

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WANG Hui, WANG Jiayuan, WU Xiaopeng, SHEN Haiyan, LUO Ying, DAI Haofu, MEI Wenli
HPLC-ESI-MS Analysis of Flavonoids Obtained from Tissue Culture of Dracaena cambodiana
2015 Vol. 31 (1): 38-43 [Abstract] ( 11 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4184-5

Dragon's blood is a traditional medicine and used in many countries with different cultures because of its various therapeutic properties. The main bioactive constituents of dragon's blood are flavonoids, which exhibit va-rious pharmaceutical activities, such as haemostatic, analgesic, anticoagulant, and antimicrobial activities and so on, and have attracted the attention of researchers on the development of new drugs. However, the formation process of dragon's blood in nature is very slow, which cannot meet the demand of pharmaceutical uses. Dracaena cambodiana (D. cambodiana) is one of the resource plants of dragon's blood. During the course of tissue culture of D. cambodiana, 6-benzylaminopurine was added in the medium, then red secretion was discovered in the cultured medium. Twelve compounds(112), including 11 flavonoids, were determined via the analysis of constituents of the cultured medium by high performance liquid chromatography-electrospray ionization-mass spectrometry(HPLC-ESI-MS) and the results were compared with that of the standards isolated from dragon's blood. Among compounds 112, 4,4'-dihydroxy-2-methoxydihydrochalcone(5), 4,4'-dihydroxy-2,6-dimethoxydihydrochalcone(6) and (2S)-7,3'-dihydroxy-4'-methoxyflavane(9) were major compounds of the red secretion, with contents of 15.70, 7.10 and 57.23 mg/L, respectively. Therefore, it is promising that flavonoids from dragon's blood can be obtained from the tissue culture of its resource plants for the purpose of drug development.

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ZHAO Yanyan, WANG Liheng, GUO Zhimou, CHI Xiaofei, MA Xiaochi, QI Yan, FANG Shinong, LI Xiuling, LIANG Xinmiao
Enhanced Multi-phosphopeptide Enrichment and Nano LC-ESI-qTOF-MS Detection Strategy Using Click OEG-CD Matrix
2015 Vol. 31 (1): 44-52 [Abstract] ( 6 ) [HTML 1KB] [PDF 0KB] ( 5 )   
doi: 10.1007/s40242-014-4179-7

Detection and determination of multi-phosphopeptides from protein digestion products are difficult due to the low abundance and ion-suppression effect arised from the existence of their high-abundance counterparts. Click OEG-CD[olio(ethylene glycol)(OEG) linked β-cyclodextrin(CD)] matrix has shown excellent performance in phosphopeptide enrichment. However, few multi-phosphopeptides were detected previously. In this investigation, an improved method aiming at enhancing the enrichment selectivity and mass spectrometry(MS) detection of multi-phosphopeptide was developed via optimizing the sample loading amount on per mg of matrix. Mass spectra were obtained on a Nano liquid chromatography-electrospray ionization-quadrupole time of flight-mass spectrometry (LC-ESI-qTOF-MS). The enrichment selectivity of double-phosphopeptide could be enhanced with the increase of loading amount on per mg of matrix when taking the mixture of mono-, double-, and non-phosphopeptides as probe. Furthermore, the multi-phosphopeptide enrichment selectivity was enhanced under the condition of optimized loading amount when taking the product of typtic digestion α-casein as test sample. When the loading amount was 573 pmol/mg matrix, up to 20 α-casein phosphopeptide signals(including 15 multi-phosphopeptides) were detected. The result is much better than that of our previous report. The reduction of ion-suppression effect arised from the existence of high-abundance non-or mono-phosphopeptides and the stronger interactions between multi-phosphopepides and the matrix were contributed to the result. The study could be helpful to the better utilization of Click OEG-CD matrix in the enrichment of multi-phosphopeptide from complex biosamples in the subsequent investigation.

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CHENG Xu, LI Xiaolong, WAN Weili, HAO Wenmei, HAI Li, WU Yong
Indole-tolerant Oxidation of 1,2-Diarylalkynes to 1,2-Diketone Derivatives
2015 Vol. 31 (1): 53-59 [Abstract] ( 7 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4373-2

A new indole-tolerant oxidation condition for the synthesis of 1,2-diketone derivatives from the corresponding 1,2-diarylalkynes was described. By screening a series of oxidation systems on alkynes linked with indole and different substituted aromatic ring, the DMSO/PdCl2/CuCl2 system afforded moderate to good yields despite the existence of electron-rich indole ring.

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SU Ran, LÜ Lei, ZHENG Songzhi, JIN Yinghua, AN Shengji
Synthesis and Characterization of Novel Azo-containing or Azoxy-containing Schiff Bases and Their Antiproliferative and Cytotoxic Activities
2015 Vol. 31 (1): 60-64 [Abstract] ( 7 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4355-4

A series of novel Schiff base derivatives was designed and synthesized from 3,3'-azobenzaldehyde and 3,3'-azoxybenzaldehyde. The newly synthesized compounds were characterized by FTIR, 1H NMR, MS and elemental analysis and tested for their in vitro antiproliferative activities against HeLa cell lines. At the same time, the impact on the antitumor activity of the sulfanilamido, benzamido, phenolic hydroxyl or thiourea groups was investigated and discussed. Compounds 4, 6 and 10 were found to exhibit strong cytotoxic activity.

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CHEN Zhanguo, LIU Yali, HU Junli, LIU De'e
Aminobromination of Ethyl α-Cyanocinnamate Derivatives with 1,3-Dibromo-5,5-dimethylhydantoin(DBDMH) as Nitrogen and Halogen Sources
2015 Vol. 31 (1): 65-70 [Abstract] ( 3 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4341-x

1,3-Dibromo-5,5-dimethylhydantoin(DBDMH) was found to be a new and efficient nitrogen/halogen source for the aminobromination of ethyl α-cyanocinnamate derivatives catalyzed by K3PO4. The reaction afforded the aminobrominated products in high yields at room temperature, and the full regiospecificity of all the products were achieved. A possible pathway involving a Michael addition for this aminobromination was suggested.

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TANG Xiaobin, LI Zhenghui, LI Yonghong, LIU Wei, YU Peng, LI Lixin, GUO Yu, YANG Cheng
Synthesis and Biological Evaluation of Novel Saccharin Derivatives Containing 1,2,3-Triazole Moiety
2015 Vol. 31 (1): 71-77 [Abstract] ( 5 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-4309-x

A series of novel saccharin derivatives containing 1,2,3-triazole moiety was synthesized in satisfactory yields. The structures of all the compounds were elucidated and confirmed by Fourier transform infrared(FTIR) spectroscopy, 1H and 13C nuclear magnetic resonance(1H NMR, 13C NMR) spectroscopy, and high resolution mass spectrometry(HRMS). The bioassays indicated that most of the title compounds displayed some extent herbicidal activities at 100 μg/mL.

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JIA Xuedong, LIU Xiujun, WANG Jian, WANG Minghua, GUO Huiyuan, LIU Mingliang
Synthesis and Antitumor Activity of Capecitabine Derivatives
2015 Vol. 31 (1): 78-83 [Abstract] ( 8 ) [HTML 1KB] [PDF 0KB] ( 4 )   
doi: 10.1007/s40242-015-4282-4

A series of capecitabine derivatives with a Boc group at the N4-position was synthesized and their in vitro antitumor activities against HepG2(liver hepatocellular carcinoma) were primarily evaluated. Some compounds were chosen for further evaluation of their in vivo efficacy on nude mice xenografted human hepatoma HepG2. The results showed that compounds 3 and 6 had considerable in vivo activity against HepG2, with tumor growth inhibition rates of 70% and 64% on day 21, respectively, and 56% and 55% on day 35, respectively, which are roughly comparable to capecitabine(74% and 59% on days 21 and 35, respectively).

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JI Baoming, DENG Dongsheng, WANG Weizhou, WANG Ke, HE Mengli
Structural Study on Four co-Crystals of N-Containing Heteroaromatics with Iodofluorobenzene
2015 Vol. 31 (1): 84-90 [Abstract] ( 6 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4145-z

N-Containing heteroaromatics 1,2,4,5-tetra(pyridin-3-yl)benzene[1,2,4,5-T(3-PY)B] and 1,2,4,5-tetra-(pyridin-4-yl)benzene[1,2,4,5-T(4-PY)B] were each co-crystallized with 1,2-diiodo-tetrafluoro-benzene(1,2-DITFB), or 1,4-diiodo-tetrafluoro-benzene(1,4-DITFB), respectively, generating four co-crystals, namely, (1,2-DITFB)4·[1,2,4,5-T(3-PY)B](1), (1,2-DITFB)4·[1,2,4,5-T(4-PY)B](2), (1,4-DITFB)2·[1,2,4,5-T(3-PY)B]·CHCl3(3), and (1,4-DITFB)·[1,2,4,5-T(4-PY)B]·2CHCl3(4). This study takes aim at providing an insight into the relative importance of fundamental solid state halogen bonding interactions(i.e., halogen…N, halogen…halogen, and halogen…π) in systems. The effects of the donor and acceptor on supramolecular assembly and the crystal structure determined interactions were discussed. The N…I halogen bonds are the main directing interactions responsible for the observed structures. In compounds 1 and 2, the donors exhibited lower-than-expected supramolecular connectivity. In spite of this, co-crystal 2 exhibits polymeric structures consisting of infinite one-dimensional(1D) double-zigzag chains of alternating electron donor and acceptor. The basic structure of co-crystals 3 and 4 is also infinite 1D chain. Therefore, the 1D halogen bonded supramolecular assemblies can be obtained by matching the appropriate donor and acceptor.

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GONG Jinsong, WANG Yue, ZHANG D, an, LI Heng, ZHANG Xiaomei, ZHANG Rongxian, LU Zhenming, XU Zhenghong, SHI Jinsong
A Surfactant-stable Bacillus pumilus K9 α-Keratinase and Its Potential Application in Detergent Industry
2015 Vol. 31 (1): 91-97 [Abstract] ( 4 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4351-8

An α-keratinase producing strain was isolated with wool as the sole carbon and nitrogen source and identified as Bacillus pumilus K9. The major amino acids liberated from the keratin degradation of wool by B. pumilus K9 were glutamic acid and leucine. The α-keratinase was purified to electrophoretic homogeneity with a molecular weight of 32000. The purified enzyme exhibits an optimum activity at 60 ℃ and pH=9.0. It was stable at pH values between 8 and 11. Bacillas pumilus keratinase displays a high activity towards casein, keratin, wool and feather, which indicates its wide application range. The keratinase was completely inhibited by phenylmethyl-sulfonyl fluoride(PMSF) and β-mercaptoethanol, and moderately inhibited by ethylemediamine-tetraacetic acid(EDTA), sugges-ting it is a metallo-cysteine keratinase. This enzyme could remain stable that could even be promoted in the presence of surfactants, including sodium dodecyl sulfate(SDS), Tween and Triton. And Tween 40 and Triton X-100 could substantially enhance the activity of the enzyme by 54% and 35%, respectively. It may indicate the prominent feature of the keratinase to tolerate surfactants. The enzymatic properties distinguish this keratinase from others in the literature. Furthermore, this enzyme is extremely stable in the presence of a commercially available detergent with 1% concentration. Detergents ARIEL, Bluemoon and WhiteCat can enhance the activity of the keratinase by 43.56%, 15.22%, and 22.48%, respectively.

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YU Xiaoxiao, HAO Weiwei, XIE Guiqiu, WANG Yingwu, GAO Renjun
Clone, Purification and Characterization of Thermostable Aminopeptidase ST1737 from Sulfolobus tokodaii
2015 Vol. 31 (1): 98-102 [Abstract] ( 1 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-014-4314-5

The aminopeptidase gene from thermophilic archaea Sulfolobustokodaii was cloned and expressed in Escherichia coli BL21 codon-plus(DE3). To overexpress the aminopeptidase, the vector pET32a was constructed, in which the target gene was fused with the genes of histidine-tag and thioredoxin(Trx). The expressed protein was purified using Ni2+-column affinity chromatography and ion exchange chromatography and cleft with enterokinase(EK) to obtain the purified aminopeptidase(ST1737). The biochemical and enzymic properties of the expressed ST1737 were characterized. The results show that its optimal pH and temperature are 8 and 80 ℃, respectively. The half-life of ST1737(0.2 mg/mL) is about 85 h at 90 ℃, indicating that the enzyme exhibits an excellent thermostability. The activity of ST1737 could still maintain over 85% after its treatment at 25 ℃ in different buffers with a pH range of from 6.0 to 10.5 for 24 h, demonstrating that ST1737 is stable in neutral or slight alkali environment. The enzyme shows a high activity for the substrates, such as unmodified peptide Asp-Ala, while the pNPC8 shows an optimal esterase substrate specificity. These results indicate that the enzyme is a bifunctional enzyme, and different from the aminopeptidase reported before.

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WU Yichao, DENG Xiuqing, MAO Yinchun, ZHANG Yan, LIU Jiaqin, RONG Li, XU Zhihong
Retention Mechanism of Phenolic Compounds in Subcritical Water Chromatography
2015 Vol. 31 (1): 103-106 [Abstract] ( 2 ) [HTML 1KB] [PDF 0KB] ( 1 )   
doi: 10.1007/s40242-015-4360-7

The transfer enthalpies and entropies of hydroxyl and nitryl in different mobile phase systems were compared by van't Hoff curve. Results suggest that the presence of acetonitrile and methanol in the mobile phase may decrease the interaction of solute and stationary phase with respect to subcritical water, thereby reducing the contribution of enthalpy to the retention. Retention mechanisms of phenolic compound appear to be more similar in subcritical water and water/methanol systems on the PRP-1 column. Hydrogen bond in subcritical water system plays a very important role in the retention of the phenols.

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SHENG Liwen, ZHANG Tianlong, WANG Kang, TANG Hongsheng, LI Hua
Quantitative Analysis of Fe Content in Iron Ore via External Calibration in Conjunction with Internal Standardization Method Coupled with LIBS
2015 Vol. 31 (1): 107-111 [Abstract] ( 25 ) [HTML 1KB] [PDF 0KB] ( 4 )   
doi: 10.1007/s40242-014-4318-1

The external calibration in conjunction with internal standardization(ECIS) coupled with laser-induced breakdown spectroscopic(LIBS) technique was proposed to perform the quantitative analysis of Fe content in iron ore. The plasma temperature and the electron number density were calculated to prove that the plasma was under local thermodynamic equilibrium(LTE) conditions and to ensure that the integral intensities of Fe I lines were reasonable. In addition, the result of the quantitative analysis shows a content of (20.26±0.59)% by mass of Fe in the iron ore. It was determined by four calibration curves, drawn for four emission lines of Fe I(373.48, 373.71, 404.58 and 438.35 nm) normalized by Mn I line, base on the ECIS method which can eliminate the influence of matrix effect and improve the accuracy of quantitative analysis, compared with the standard addition method. Both the results of these two analytical methods were compared with that listed in the Standard Substance Certificate. The percentage content of Fe in the same sample of iron ore by the ECIS method was (20.17±0.08)% by mass, which shows a good performance to analyze the Fe content of iron ore in combination with LIBS.

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PAN Chengling, TANG Guodong, CAO Zhi, XU Jiqing, SHENG Shaoding
Structural and Theoretical Studies of a New CuI-CuI Complex Bearing Bulky Unsymmetrical Benzamidinate Ligand
2015 Vol. 31 (1): 112-116 [Abstract] ( 4 ) [HTML 1KB] [PDF 0KB] ( 1 )   
doi: 10.1007/s40242-015-4287-z

Density functional theory(DFT) calculations unambiguously verify that there is little or no direct metal-metal bonding in the dinuclear copper(I) benzamidinate complex [Cu2(LRR')2](2){LRR'=[PhC(NR)(NR')]-(R= 2,6-iPr2C6H3, R'=SiMe3)} with a short Cu-Cu distance[0.24454(4) nm].

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ZHANG Ying, PAN Yue, LIU Jia, WANG Guiling, CAO Dianxue
Synthesis and Electrochemical Studies of Carbon-modified LiNiPO4 as the Cathode Material of Li-ion Batteries
2015 Vol. 31 (1): 117-122 [Abstract] ( 5 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4261-9

Well-crystallized olivine LiNiPO4 and carbon-modified LiNiPO4(LiNiPO4/C) were synthesized by a combined solvothermal and solid state reaction method using water-benzyl alcohol two-phase solvent. The structure and morphology of the prepared LiNiPO4 were systematically characterized by powder X-ray diffraction, scanning electron microscopy and transmission electron microscopy. The LiNiPO4 particles are up to around 2 μm in diameter while the particle size of LiNiPO4/C is about 100—200 nm. At a current rate of 0.05 C(1.00 C=167 mA/g, corresponding to one Li+ intercalation/deintercalation), LiNiPO4 and LiNiPO4/C presented a high initial specific capacity of 157 and 220 mA·h/g, respectively. The capacity of LiNiPO4/C is 72% larger than that of LiNiPO4 at 0.1 C. The LiNiPO4/C cathode exhibits a superior electrochemical performance in comparison with LiNiPO4, revealing that carbon modifying is an effective method to improve the ionic diffusion and electronic conductivity of cathode material LiNiPO4. Furthermore, lithium ion diffusion coefficients of LiNiPO4 and LiNiPO4/C are 1.80×10-15 and 1.91×10-14 cm2/s, respectively, calculated via the data from electrochemical impedance spectra.

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ZHANG Hui, SHANG Yan, CHEN Qingguo, HAN Baozhong
Theoretical Studies on Dielectric Breakdown Strength Increasing Mechanism of SF6 and Its Potential Alternative Gases
2015 Vol. 31 (1): 123-129 [Abstract] ( 4 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-014-4255-z

A theoretical investigation on the dielectric insulation mechanism of sulfur hexafluoride(SF6) and its potential alternative gases at the atomic and molecular levels was made. The electronic structures of the molecules of them were calculated at the B3LYP/6-311+G(d,p) level. The HOMO-LUMO energy gaps, ionization potentials, electron affinities, and dipole moments of the studied molecules at the ground state were obtained. The 11 isomerization reactions, with the harmonic vibration frequencies of the equilibrium geometries and the minimum energy path by the intrinsic reaction coordinate theory, were also obtained at the same level. The results show that the insulation gas, with the larger HOMO-LUMO energy gap, the higher ionization potential and the stronger electron affinity, can increase the dielectric breakdown strength efficiently, which is in good agreement with the available experimental finding. We suggested that the molecule with isomerization reaction occurring can dissipate the energy of hot electrons availably, which is favorable to the dielectric breakdown strength increasing for the SF6 potential alternative gas.

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ZHANG Lingna, CAI Kun, ZHANG Feng, YUE Qunfeng
Adsorption of CO2 and H2 on Nitrogen-doped Porous Carbon from Ionic Liquid Precursor
2015 Vol. 31 (1): 130-137 [Abstract] ( 8 ) [HTML 1KB] [PDF 0KB] ( 7 )   
doi: 10.1007/s40242-015-4224-1

Nitrogen-doped mesoporous carbon material was prepared via a simple one-step thermolysis method via the carbonization of ionic liquid, 1-cyanomethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([MCNIm]+[Nf2T]-). The nanostructure of the resultant carbon material was characterized by X-ray diffraction(XRD) and transmission electron microscopy(TEM) and the types of N-containing groups of the carbon material were investigated by X-ray photoelectron spectroscopy(XPS). The N-content of the carbon material is 18.6%(mass fraction) based on the elemental analysis. The produced mesoporous carbon material was further used as the solid sorbent for H2 and CO2. The hydrogen uptake capacity and H2 isosteric heat of the carbon material were discussed. Furthermore, the nitrogen-containing carbon material as good sorbent shows relatively high adsorption and separation ability for CO2 from CH4, for which the heat of CO2 adsorption(Qst) is 31.8 kJ/mol. The mesoporous structure and nitrogen functionality make the carbon material with high adsorption capacity and selectivity for CO2 and ability to store H2, indicating that this kind of nitrogen-doped carbon material originated from ionic liquids is a promising sorbent material for high-performance separation and adsorption.

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CHEN Na, JIANG Yanqiu, CHENG Wenjing, LIN Kaifeng, XU Xianzhu
Synthesis of Submicrometer-sized Sn-MCM-41 Particles and Their Catalytic Performance in Baeyer-Villiger Oxidation
2015 Vol. 31 (1): 138-143 [Abstract] ( 11 ) [HTML 1KB] [PDF 0KB] ( 5 )   
doi: 10.1007/s40242-014-4204-x

Submicrometer-sized tin-containing MCM-41 particles with a size of several hundred nanometers(Sn-MCM-41/SMPs) were rapidly prepared with tin chloride as tin source and tetraethyl orthosilicate as silicon source via a dilute solution route in sodium hydroxide medium at room temperature. The characterization results show the highly ordered hexagonal mesopores and tetrahedral Sn species in Sn-MCM-41/SMPs. The material proved to be active and selective for Baeyer-Villiger oxidation of adamantanone with aqueous H2O2. Notably, Sn-MCM-41/ SMPs displayed a higher initial reaction rate and turnover number(TON) than common micrometer-sized Sn-MCM-41 large particles(Sn-MCM-41/LPs), mainly attributed to the accelerated diffusion of the reactants and enhanced accessibility to the catalytic Sn species via shorter mesopore channels in Sn-MCM-41/SMPs. Furthermore, Sn-MCM-41/SMPs could be reused without the loss of activity after five runs, indicating that Sn active sites in the submicrometer-sized particles are remarkably stable. The study shows that decreasing particle size of Sn-MCM-41 in submicrometer scale is an effective way to achieve catalysts for Baeyer-Villiger oxidations with improved catalytic performance.

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ZHANG Shengyu, LÜ Ying, LIN Xueyu, ZHANG Yuling, SU Xiaosi
Performance and Mechanisms of Fluoride Removal from Groundwater by Lanthanum-aluminum-loaded Hydrothermal Palygorskite Composite
2015 Vol. 31 (1): 144-148 [Abstract] ( 23 ) [HTML 1KB] [PDF 0KB] ( 7 )   
doi: 10.1007/s40242-015-4126-2

Lanthanum-aluminum loaded hydrothermal palygorskite(La-Al-HP) composite was prepared and selected as adsorbent for the fluoride removal from simulated groundwater. The adsorbent was characterized by scanning electron microscopy(SEM), Brunauer-Emmet-Teller(BET) analysis, X-ray diffraction(XRD) analysis and X-ray photoelectron spectroscopy(XPS). SEM visualization shows that the dense surface structure of raw HP appeared loose and presented micro canals after modification. The BET analysis also proved the specific surface area of La-Al-HP composite(95.58 m2/g) was higher than that of the raw HP(34.31 m2/g). Subsequently, the adsorption capacity of La-Al-HP composite was demonstrated in adsorption experiments. The kinetics of fluoride ion adsorption into La-Al-HP composite followed the pseudo-second order with a correlation coefficient of 0.997. The isotherm data was well fitted with the Langmuir model. The monolayer adsorption capacity of La-Al-HP composite was 1.30 mg/g. The XRD and XPS results reveal that the La3+ and Al3+ ions were loaded on the surface of modified HP and the fluoride ion was adsorbed onto the La-Al-HP composite. A large amount of La-Al-O composite oxide existing on the surface of La-Al-HP composite might be the immanent cause for the excellent adsorption capacity of fluoride ions.

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LI Wenzhao, MENG Wei, TIAN Pu
Impact of Stable Protein-protein Interaction on Protein Conformational Space
2015 Vol. 31 (1): 149-155 [Abstract] ( 1 ) [HTML 1KB] [PDF 0KB] ( 2 )   
doi: 10.1007/s40242-015-3402-5

Backbone dihedral angle based clustering approach was applied to investigate the effect of protein complexation on backbone conformational space and the effect on protein dynamics. Three representative enzyme-inhibitor complexes and their comprised proteins were used as models for small-and moderate-sized globular proteins to compare available backbone conformational space before and after complexation. Microsecond time scale molecular dynamic simulations were generated to ensure sufficient statistics. The result suggests that stable protein-protein interactions lead to redistribution of protein backbone mobility and restriction of the protein backbone conformational space, especially for short time scale motions. Surprisingly, these effects are found to be uncorrelated with protein-protein interaction surface. Consistent with many experimental and computational observations, our results indicate that both induced-fit and conformational selection models play roles in stable protein complexation process, with the dominant role being different for different protein complexes.

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HU Fang, WANG Yamin, LAI Xiaoyong, WU Yusheng, DU Fei, WANG Chunzhong
Facile Synthesis of Mesoporous Si-containing γ-Al2O3Nanofiber with Enhanced Thermal Stability
2015 Vol. 31 (1): 156-159 [Abstract] ( 8 ) [HTML 1KB] [PDF 0KB] ( 4 )   
doi: 10.1007/s40242-015-4322-0

Mesoporous γ-Al2O3 nanofiber was prepared via a simple reverse precipitation route using Si-containing Al(OH)3 and HNO3 as raw materials. The resultant Si-containing mesoporous γ-Al2O3 nanofiber exhibited high surface area of 320 m2/g, large pore volume of 1.17 cm3/g and large pore size of 10.5 nm. The introduction of Si element remarkably enhanced the thermal stability of mesoporous γ-Al2O3. The as-prepared nanofiber could maintain relative high surface area(110 m2/g) and pore volume(0.73 cm3/g) up to 1100 ℃. The effects of various experimental conditions, such as pH value, reaction temperature and aging temperature on the structural properties of the mesoporous γ-Al2O3 were also investigated.

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ZUO Huajiang, WEN Wanhua, WU Dingcai, FU Ruowen, TANG Chunyi
Antibacterial Activity of Polymeric Quaternary Ammonium Compounds Tuned by Incorporating Hydrophilic co-Monomer
2015 Vol. 31 (1): 160-166 [Abstract] ( 10 ) [HTML 1KB] [PDF 0KB] ( 3 )   
doi: 10.1007/s40242-015-4248-6

Copolymers of quaternary ammonium monomer(QAM) and hydrophilic co-monomer were successfully synthesized by free radical polymerization. It was discovered that the hydrophilic co-monomers with poor antibacterial activity significantly enhanced the activity of QAM substituted with a long alkyl chain[i.e., N,N-dimethyl-N-dodecyl methacrylate ammonium bromide(DMAEMA-DB)]. When a suitable molar ratio of DMAEMA-DB to co-monomer was selected, the activity of the copolymers was up to 123 times that of the homopolymer of DMAEMA-DB against S. aureus, and 282 times that of it against E. coli. But unlike DMAEMA-DB, the co-monomers might weaken the activity of QAM substituted with a short alkyl chain[i.e., N,N-dimethyl-N-butyl methacrylate ammonium bromide(DMAEMA-BB)]. Moreover, it was found that copolymers of DMAEMA-DB were much more biocidal than those of DMAEMA-BB. Therefore, it could be speculated that the long alkyl chain plays an important role in the antibacterial activity, and that the hydrophilic co-monomers are beneficial to polymeric guaternary ammonium compounds(PQACs) to exert the positive effect of the long alkyl chain to the greatest degree.

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