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SCIENCE CHINA Chemistry
2016, 59 No. 3 pp. 251-382
Published: 17 February 2016

Nowadays, separation of trivalent lanthanides and actinides is considered to be a key issue in the advanced spent nuclear fuel reprocessing. In this work, a series of possible extraction complexes of Am3+ and Eu3+ with the traditional organophosphorus ligand HDEHP (di-(2-ethylhexyl) phosphoric acid) in nitric acid solution have been systematically explored by using scalar-relativistic density functional theory (DFT). Based on our calculations, HDEHP can coordinate with M3+ (M=Eu, Am) cations in the form of hydrogen-bonded dimers HL2- (L=DEHP–), and these dimers prefer to act as bidentate ligands in all the studied complexes. According to thermodynamic analysis, the HL2- dimer shows comparable affinity for Eu(III) and Am(III). The 1:3 type complexes M(HL2)3 seem to be more stable in the organic phase than the 1:1, 1:2 type nitrate complexes due to the higher lipophilicity of the former (see the article by Juan Luo, Congzhi Wang, Jianhui Lan, Qunyan Wu, Yuliang Zhao, Zhifang Chai, Changming Nie & Weiqun Shi on pages 324–331).


 
   
 
 
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New frontiers of N-heterocyclic carbene catalysis Hot!
Jiean Chen, Yong Huang
2016 Vol. 59 (3): 251-254 [Abstract] ( 135 ) [ PDF (1290 KB)   ] ( 167 )  [Supporting InformationDOI: 10.1007/s11426-015-5514-7
Received: 2015-08-08; Accepted: 2015-08-29; Published Online: 2015-11-25
 REVIEWS
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Nanoprobes in biomedical detection Hot!
Yawei Zhao, Changling Zou, Hongkang Zhao, Lina Zhao

Environmental problems caused by the development of nanotechnology have threatened human health. Investigating the biomedical effects of nanomaterials can help to solve these environmental safety issues. In studies on the biomedical effects of nanomaterials, several types of novel nanoscale probes that allow reliable, sensitive, accurate and rapid biomedical detection have emerged. We summarize recent developments in three categories of these nanoprobes, including noble metal nanocluster probes, carbon-based nanostructured probes, and unnatural amino acid-based probes. Besides reviewing the utility of different nanoprobes in cell imaging and protein detection, we also discuss the molecular mechanism of nanoprobe detection. Perspectives of novel nanoprobe design based on molecular details of biomedical detection are presented.

2016 Vol. 59 (3): 255-263 [Abstract] ( 168 ) [ PDF (2891 KB)   ] ( 135 )  [Supporting InformationDOI: 10.1007/s11426-015-5535-2
Received: 2015-07-29; Accepted: 2015-08-28; Published Online: 2015-12-17
 ARTICLES
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A novel preparation method of sulfonic functionalized silica: CH3SO3H as the sulfonic source and Al as the bridge
Naiwang Liu, Jiajia Yao, Li Shi

A novel approach is designed to optimize the synthesis of sulfonic-functionalized silica material. Results from 29Si and 27Al NMR suggest that the Al acts as the bridging atom connecting the methanesulfonate and silica matrix. Further pyridine-FTIR spectra followed by catalytic activity tests demonstrate that compared with previous methods, our new approach results in higher Lewis acid site concentration, higher thermal stability and superior catalytic activity. Moreover, the whole catalysis preparation procedure is environmentally friendly. Specifically, the silica matrix is synthesized through hydrolysis of tetraethylorthosilicate employing formic acid as hydro-catalyst, in which no surfactant species or precursors were involved.

2016 Vol. 59 (3): 264-270 [Abstract] ( 126 ) [ PDF (805 KB)   ] ( 74 )  [Supporting InformationDOI: 10.1007/s11426-015-5479-6
Received: 2015-05-12; Accepted: 2015-06-25; Published Online: 2015-11-10
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Bio-inspired multifunctional metallic glass Hot!
Yaxu He, Yun Peng, Zhou Li, Jiang Ma, Xiyao Zhang, Kesong Liu, Weihua Wang, Lei Jiang

As a novel class of metallic materials, bulk metallic glasses (BMGs) have attracted a great deal of attention owing to their technological promise for practical engineering applications. In nature, biological materials exhibit inherent multifunctional integration, which provides some inspiration for scientists and engineers to construct multifunctional artificial materials. In this contribution, inspired by superhydrophobic self-cleaning lotus leaves, multifunctional bulk metallic glasses (BMG) materials have been fabricated through the thermoplastic forming-based process followed by the SiO2/soot deposition. To mimic the microscale papillae of the lotus leaf, the BMG micropillar with a hemispherical top was first fabricated using micro-patterned silicon templates based on thermoplastic forming. The deposited randomly distributed SiO2/soot nanostructures covered on BMG micropillars are similar to the branch-like nanostructures on papillae of the lotus leaf. Micro-nanoscale hierarchical structures endow BMG replica with superhydrophobicity, a low adhesion towards water, and self-cleaning, similar to the natural lotus leaf. Furthermore, on the basis of the observation of the morphology of BMG replica in the Si mould, the formation mechanism of BMG replica was proposed in this work. The BMG materials with multifunction integration would extend their practical engineering applications and we expect this method could be widely adopted for the fabrication of other multifunctional BMG surfaces.

2016 Vol. 59 (3): 271-276 [Abstract] ( 160 ) [ PDF (1892 KB)   ] ( 130 )  [Supporting InformationDOI: 10.1007/s11426-015-5496-5
Received: 2015-06-10; Accepted: 2015-06-24; Published Online: 2015-11-03
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Synthesis and photocatalytic activity of ZnO-Au25 nanocomposites Hot!
Junjie Hu, Hai Yuan, Peng Li, Jian Wang, Qiankun Liu, Hui Wang, Qilin Wang, Xiaoyou Yuan

ZnO-Au25 nanocomposites were synthesized by doping Au25 nanoclusters into the porous ZnO nanospheres. It was notable that the ultrasmall Au25 nanoclusters possessed uniform sizes and fine dispersibility on the porous ZnO supports. A considerable correlation between the loading of Au25 nanoclusters and the photocatalytic activity was found. Compared with the pure ZnO nanospheres, the ZnO-Au25 nanocomposites exhibited more efficient photocatalytic activity in terms of degradation of Rhodamine B (RhB) in an aqueous solution. In addition, the possible photocatalytic mechanisms are discussed in this work. This strategy may be helpful for preparing other novel hybrid nanocomposites with well-defined structures and superior performances.

2016 Vol. 59 (3): 277-281 [Abstract] ( 126 ) [ PDF (3064 KB)   ] ( 121 )  [Supporting InformationDOI: 10.1007/s11426-015-5487-6
Received: 2015-06-05; Accepted: 2015-06-26; Published Online: 2015-12-02
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Preparation and properties of physically and chemically cross-linked hybrid hydrophobic association hydrogels with good mechanical strength
Guoqing Jiang, Li Huang, Bo Li, Quan Zhou, Zhiying Li

To correct the defects of hydrophobic association hydrogels (HA-gels), new physically and chemically cross-linked hybrid hydrophobic association hydrogels (hybrid HA-gels) were prepared by radical copolymerization of acrylamide (AM), octylphenol polyoxyethylene (n) acrylate (OPnAC, n stands for the number of ethoxy group, and is 10 and 21) and N,N'-methylene-bisacrylamide (MBA). On the basis of the statistical molecular theory of rubber elastic, the Mooney-Rivlin model and using the tensile true stress (σtrue) tested at room temperature, the number of network strands per unit volume (ν0) and the number-average molar mass of a network strand (Mc) were evaluated for hybrid HA-gels. For the hydrogels, the effect of the content of MBA and OP10AC on their tensile mechanical properties was studied by using ν0 and Mc; also, the effect of the compositions and temperature on their swelling behavior in distilled water was discussed in detail. In addition, hybrid HA-gels including a small quantity of MBA possessed the capabilities of secondary self-healing and remolding. In contrast with HA-gels prepared by the same compositions besides MBA, hybrid HA-gels showed good mechanical strength and long-term thermal stability in distilled water in the range of 25 to 80 ℃. Furthermore, hybrid HA-gels also avoided the self-deswelling behavior of HA-gels. The results show that the application fields of HA-gels will be greatly broadened after introducing a chemical cross-linking network.

2016 Vol. 59 (3): 282-292 [Abstract] ( 147 ) [ PDF (2599 KB)   ] ( 81 )  [Supporting InformationDOI: 10.1007/s11426-015-5509-4
Received: 2015-06-11; Accepted: 2015-08-04; Published Online: 2015-11-23
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Gelation capability of cysteine-modified cyclo(L-Lys-L-Lys)s dominated by Fmoc and Trt protecting groups
Huimin Geng, Qianying Zong, Jie You, Lin Ye, Aiying Zhang, Ziqiang Shao, Zengguo Feng

A series of symmetrical peptidomimetics (3-8) based on cysteine-modified cyclo(L-Lys-L-Lys)s were synthesized, and their gelation capability in organic solvents was dominated by fluorenylmethyloxycarbonyl (Fmoc) and triphenylmethyl (Trt) protecting groups and the exchange of thiol-to-disulfide as well. The peptidomimetics holding Trt (3 and 4) showed no gel performance, while the Fmoc groups promoted 5 and 6 to give rise to thermo-reversible organogels in a number of organic solvents. The self-assembled fibrillar networks were distinctly evidenced in the organogels by transmission electron microscopy (TEM) and scanning electron microscopy (SEM) observations. Fourier transform infrared spectroscopy (FT-IR) and fluorescence analyses revealed that the hydrogen bonding and p-p stacking play as major driving forces for the self-assembly of these organogelators. A b-turn secondary structure was deduced for the organogel of 6 by virtue of X-ray diffraction, FT-IR and circular dichroism (CD) measurements, and an interdigitated bilayer structure was also presented.

2016 Vol. 59 (3): 293-302 [Abstract] ( 127 ) [ PDF (2694 KB)   ] ( 72 )  [Supporting InformationDOI: 10.1007/s11426-015-5477-8
Received: 2015-05-18; Accepted: 2015-06-18; Published Online: 2015-10-13
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Radiation induced graft polymerization of multi-walled carbon nanotubes for superhydrophobic composite membrane preparation Hot!
Bowu Zhang, Siyuan Xie, Rongmao Wei, Hongjuan Ma, Ming Yu, Linfan Li, Jingye Li

Highly soluble multi-walled carbon nanotubes (MWNTs) were prepared by radiation-induced free radical graft polymerization of vinyl acetate (VAc) onto pristine MWNT surfaces. High resolution transmission electron microscopy (HR-TEM), Fourier transform infrared (FTIR) spectroscopy, and micro-Raman spectroscopy were used to confirm that poly(vinyl acetate) (PVAc) had been successfully grafted onto the surface of the MWNTs. The effects of experimental parameters on the degree of grafting (DG) of PVAc were also investigated, including adsorbed dose, dose rate, initial monomer concentration, and solvents. The grafted MWNTs (MWNTs-g-PVAc) exhibited good solubility in common organic solvents at high mass fraction. In addition, a superhydrophobic composite membrane could be readily fabricated by vacuum filtration of MWNTs-g-PVAc onto a supporting membrane, as was confirmed by water contact angle testing and visualization by scanning electron microscopy.

2016 Vol. 59 (3): 303-309 [Abstract] ( 177 ) [ PDF (4099 KB)   ] ( 189 )  [Supporting InformationDOI: 10.1007/s11426-015-5472-0
Received: 2015-05-07; Accepted: 2015-05-27; Published Online: 2015-09-16
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Virus-like supramolecular assemblies formed by cooperation of base pairing interaction and peptidic association
Meiwen Cao, Ningning Wang, Peng Zhou, Yawei Sun, Jiqian Wang, Shengjie Wang, Hai Xu

A peptide nucleic acid (PNA)-peptide conjugated molecule, T'3(AKAE)2, was designed to have both a PNA segment for oligo-nucleotide binding and an ionic self-complementary peptide sequence for self-association. T'3(AKAE)2 could co-assemble with oligoadenines (d(A)x) to form virus-like supramolecular structures whose morphology showed dependence on the chain length and rigidity of the d(A)x molecules. Smaller nanospheres with diameters of 13.0±2.0 nm were produced in the case of d(A)6. Wormlike aggregates with lengths of 20-50 nm and diameters of 15.0±2.5 nm were found in the cases of d(A)12, d(A)18, d(A)24 and d(A)30. And larger spherical aggregates with diameters of 18±5 nm came into presence in the cases of d(A)36 and d(A)42. These nanostructures were suggested to be formed under a cooperative effect of base pair recognition and peptidic association. The study provides insights into the programmed assembly of a multi-components system as well as control of the size and shape of the co-assembled structures, which is of great significance in developing gene/drug delivery systems.

2016 Vol. 59 (3): 310-315 [Abstract] ( 170 ) [ PDF (3210 KB)   ] ( 60 )  [Supporting InformationDOI: 10.1007/s11426-015-5495-6
Received: 2015-06-16; Accepted: 2015-08-03; Published Online: 2015-11-02
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Polymorph selection in the crystallization of hard-core Yukawa system
Wenze Ouyang, Zhiwei Sun, Jun Zhong, Hongwei Zhou, Shenghua Xu

Colloid-colloid interactions in charge-stabilized dispersions can to some extent be represented by the hard-core Yukawa model. The crystallization process and polymorph selection of hard-core Yukawa model are studied by means of smart Monte Carlo simulations in the region of face-centered-cubic (fcc) phase. The contact value of hard-core Yukawa potential and the volume fraction of the colloids are fixed, while the Debye screening length can be varied. In the early stage of the crystallization, the precursors with relatively ordered liquid structure have been observed. Although the crystal structure of thermodynamically stable phase is fcc, the system crystallizes into a mixture of fcc and hexagonal close-packed (hcp) structures under small Debye screening length since the colloidal particles act as effective hard spheres. In the intermediate range of Debye screening length, the system crystallizes into a mixture of fcc, hcp, and body-centered-cubic (bcc). The existence of metastable hcp and bcc structures can be interpreted as a manifestation of the Ostwald's step rule. Until the Debye screening length is large enough, the crystal structure obtained is almost a complete fcc suggesting the system eventually reaches to a thermodynamically stable state.

2016 Vol. 59 (3): 316-323 [Abstract] ( 114 ) [ PDF (2143 KB)   ] ( 83 )  [Supporting InformationDOI: 10.1007/s11426-015-5473-z
Received: 2015-05-05; Accepted: 2015-06-08; Published Online: 2015-09-21
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Theoretical studies on the complexation of Eu(III) and Am(III) with HDEHP: structure, bonding nature and stability Hot!
Juan Luo, Congzhi Wang, Jianhui Lan, Qunyan Wu, Yuliang Zhao, Zhifang Chai, Changming Nie, Weiqun Shi

Separation of trivalent lanthanides (Ln(III)) and actinides (An(III)) is a key issue in the advanced spent nuclear fuel reprocessing. In the well-known trivalent actinide lanthanide separation by phosphorus reagent extraction from aqueous komplexes (TALSPEAK) process, the organophosphorus ligand HDEHP (di-(2-ethylhexyl) phosphoric acid) has been used as an efficient reagent for the partitioning of Ln(III) from An(III) with the combination of a holdback reagent in aqueous lactate buffer solution. In this work, the structural and electronic properties of Eu3+ and Am3+ complexes with HDEHP in nitric acid solution have been systematically explored by using scalar-relativistic density functional theory (DFT). It was found that HDEHP can coordinate with M(III) (M=Eu, Am) cations in the form of hydrogen-bonded dimers HL2- (L=DEHP), and the metal ions prefer to coordinate with the phosphoryl oxygen atom of the ligand. For all the extraction complexes, the metal-ligand bonds are mainly ionic in nature. Although Eu(III) complexes have higher interaction energies, the HL2- dimer shows comparable affinity for Eu(III) and Am(III) according to thermodynamic analysis, which may be attributed to the higher stabilities of Eu(III) nonahydrate. It is expected that this work could provide insightful information on the complexation of An(III) and Ln(III) with HDEHP at the molecular level.

2016 Vol. 59 (3): 324-331 [Abstract] ( 172 ) [ PDF (1595 KB)   ] ( 122 )  [Supporting InformationDOI: 10.1007/s11426-015-5489-4
Received: 2015-05-22; Accepted: 2015-06-24; Published Online: 2015-10-29
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Platinum nanoparticles supported MoS2 nanosheet for simultaneous detection of dopamine and uric acid
Jie Chao, Xiaoyan Han, Haofan Sun, Shao Su, Lixing Weng, Lianhui Wang

Herein, platinum nanoparticles-decorated molybdenum disulfide (PtNPs@MoS2) nanocomposite has been synthesized via a microwave-assisted hydrothermal method, which was characterized by transmission electron microscopy (TEM) and powder X-ray diffraction (XRD). This MoS2-based nanocomposite modified glass carbon electrode (PtNPs@MoS2/GCE) exhibited excellent electrocatalytic activity toward dopamine (DA) and uric acid (UA) due to their synergistic effect. Two well-defined oxidation peaks of DA and UA were obtained at PtNPs@MoS2/GCE with a large peak separation of 160 mV (DA-UA), suggesting that the modified electrode could individually or simultaneously analyze DA and AA. Under the optimal conditions, the peak currents of DA and UA were linearly dependent on their concentrations in the range of 0.5-150 and 5-1000 mmol/L with detection limit of 0.17 and 0.98 mmol/L, respectively. The proposed MoS2-based sensor can also be employed to examine DA and UA in real samples with satisfactory results. Therefore, the PtNPs@MoS2 nanocomposite might offer a good possibility for electrochemical sensing and other electrocatalytic applications.

2016 Vol. 59 (3): 332-337 [Abstract] ( 158 ) [ PDF (3912 KB)   ] ( 141 )  [Supporting InformationDOI: 10.1007/s11426-015-5492-9
Received: 2015-06-23; Accepted: 2015-07-27; Published Online: 2015-10-15
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Conformation preference and related intramolecular noncovalent interaction of selected short chain chlorinated paraffins
Yuzhen Sun, Wenxiao Pan, Jianjie Fu, Aiqian Zhang, Qinghua Zhang

Short chain chlorinated paraffins (SCCPs) are not only research focus of environmental issues but also interesting model molecules for organic chemistry which exhibit diverse conformation preference and intramolecular noncovalent interactions (NCIs). A systematic study was conducted to reveal the conformation preference and the related intramolecular NCIs in two C10-isomers of SCCPs, 5,5,6,6-tetrachlorodecane and 4,4,6,6-tetrachlorodecane. The overall conformation profile was determined on the basis of relative energies calculated at the MP2/6-311++G(d,p) level with the geometries optimized by B3LYP/6-311++G(d,p) method. Then, quantum theory of atoms in molecules (QTAIM) has been adopted to identify the NCIs in the selected conformers of the model molecules at both B3LYP/6-311++G(d,p) and M06-2X/aug-cc-pvdz level. Different chlorine substitution modes result in varied conformation preference. No obvious gauche effect can be observed for the SCCPs with chlorination on adjacent carbon atoms. The most stable conformer of 5,5,6,6-tetrachlorodecane (tTt) has its three dihedral angles in the T configuration, and there is no intramolecular NCIs found in this molecule. On the contrary, the chlorination on interval carbon atoms favors the adoption of gauche configuration for the H-C-C-Cl axis. Not only intramolecular H…Cl contacts but also H…H interactions have been identified as driving forces to compensate the instability from steric crowding of the gauche configuration. The gggg and g'g'g'g' conformers are the most popular ones, while the populations of tggg and tg'g'g' conformer are second to those of the gggg and g'g'g'g' conformers. Meanwhile, the M06-2X method with large basis sets is preferred for identification of subtle intramolecular NCIs in large molecules like SCCPs.

2016 Vol. 59 (3): 338-349 [Abstract] ( 168 ) [ PDF (1663 KB)   ] ( 60 )  [Supporting InformationDOI: 10.1007/s11426-015-5502-y
Received: 2015-07-25; Accepted: 2015-08-13; Published Online: 2015-12-24
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Efficient removal of chlorophenols from water with a magnetic reduced graphene oxide composite
Han Yan, Qing Du, Hu Yang, Aimin Li, Rongshi Cheng

A magnetic reduced graphene oxide composite (MRGO) was successfully prepared by a simple and green method. MRGO was then used as an adsorbent and found to exhibit enhanced removal efficiency for various chlorophenols (CPs) from water compared with its precursors, graphene oxide (GO) and reduced graphene oxide. The CPs were o-chlorophenol, p-chlorophenol, 2,4-dichlorophenol, and 2,4,6-trichlorophenol. Among them, 2,4,6-trichlorophenol, which exhibited the lowest water solubility and highest molecular weight, most easily bound to MRGO. The preferential interactions between MRGO and CPs were hydrophobic interactions (p-p stacking and hydrophobic effect). This result was confirmed by the equilibrium adsorption behavior in which isotherms were all well described by Freudlich model, indicating heterogeneous and multilayer adsorption. Therefore, CP adsorption was more favored under neutral and acidic conditions, and the decreased removal efficiency of MRGO at higher pH levels was due to the improved hydrophilicity of CPs for deprotonation effect. Moreover, MRGO showed fast removal of each CP, achieving adsorption equilibrium within 10.0 min, presented efficient separation from water under an external magnetic field, and was easily regenerated using dilute NaOH aqueous solution after reaching saturated adsorption. Adsorption capacity of the regenerated MRGO had almost no loss until after five cycles. In summary, MRGO was an efficient adsorbent for the removal of various CPs and had considerable application potential in water treatment.

2016 Vol. 59 (3): 350-359 [Abstract] ( 187 ) [ PDF (1977 KB)   ] ( 130 )  [Supporting InformationDOI: 10.1007/s11426-015-5482-y
Received: 2015-05-14; Accepted: 2015-06-18; Published Online: 2015-09-11
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CO2 solubility in aqueous solutions of N-methyldiethanolamine+piperazine by electrolyte NRTL model
Jicai Huang, Maoqiong Gong, Xueqiang Dong, Xiaodong Li, Jianfeng Wu

Accurate modeling of the solubility behavior of CO2 in the aqueous alkanolamine solutions is important to design and optimization of equipment and process. In this work, the thermodynamics of CO2 in aqueous solution of N-methyldiethanolamine (MDEA) and piperazine (PZ) is studied by the electrolyte non-random two liquids (NRTL) model. The chemical equilibrium constants are calculated from the free Gibbs energy of formation, and the Henry's constants of CO2 in MDEA and PZ are regressed to revise the value in the pure water. New experimental data from literatures are added to the regression process. Therefore, this model should provide a comprehensive thermodynamic representation for the quaternary system with broader ranges and more accurate predictions than previous work. Model results are compared to the experimental vapor-liquid equilibrium (VLE), speciation and heat of absorption data, which show that the model can predict the experimental data with reasonable accuracy.

2016 Vol. 59 (3): 360-369 [Abstract] ( 112 ) [ PDF (837 KB)   ] ( 106 )  [Supporting InformationDOI: 10.1007/s11426-015-5508-5
Received: 2015-05-30; Accepted: 2015-08-07; Published Online: 2015-11-16
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A novel method to anchor methanesulfonic acid in silica matrix
Naiwang Liu, Jiajia Yao, Li Shi

Methanesulfonic acid (MSA) was successfully immobilized in silica, leading to a novel and environmentally friendly solid acid catalyst SMSA. The most important feature of SMSA is that anhydrous formic acid is used to hydrolysis of tetraethylorthosilicate (TEOS). No water was added in the whole preparation. Therefore, MSA could be anchored in silica matrix more effectively instead of being dissolved in water. This new organic/inorganic hybrid catalyst was characterized by powder X-ray diffraction (XRD), energy dispersive spectrum (EDS), N2 adsorption-desorption analyzer, thermogravimetric analysis (TGA-DSC) and pyridine-FTIR. The catalytic activity was tested by alkylation of olefins and aromatics. High concentration acid sites, both Lewis and Brønsted, abundant porosity and large surface area enabled the highest activity for SMSA, among MCM-22, ZSM-5 and industrial acidity clay.

2016 Vol. 59 (3): 370-379 [Abstract] ( 136 ) [ PDF (2315 KB)   ] ( 103 )  [Supporting InformationDOI: 10.1007/s11426-015-5506-7
Received: 2015-05-26; Accepted: 2015-08-31; Published Online: 2015-12-28
 COMMUNICATIONS
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Metastasis-related genes in hepatocellular carcinoma cell-lines are clustered on chromosome territories predicted by transcriptome and proteome Hot!
Li Feng, Hong Li, Yang Zhang, Huali Shen, Hongxiu Yu, Fan Zhong, Lunxiu Qin, Fuchu He, Pengyuan Yang, Zhaoyou Tang
2016 Vol. 59 (3): 380-382 [Abstract] ( 116 ) [ PDF (510 KB)   ] ( 128 )  [Supporting InformationDOI: 10.1007/s11426-015-5478-7
Received: 2015-05-21; Accepted: 2015-07-22; Published Online: 2015-08-27
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