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Wang Y.,Hunan Normal University | Wang Y.,Hunan Changling Petrochemical SandT Developing Co. | Wen X.,Hunan Normal University | Rong C.,Hunan Normal University | And 5 more authors.
Journal of Molecular Catalysis A: Chemical | Year: 2016

This paper first discloses that two heteroleptic 8-quinolinolato iron(III) complexes (Qa1Qb2FeIII, Qa2Qb1FeIII) could be synthesized conveniently via the coordination of FeCl2·6H2O with 2 equivalents of 5,7-dichloro-8-hydroxyquinoline (Qb) or 5-chloro-8-hydroxyquinoline (Qa) under N2 and then 1 equivalent of Qa or Qb under air. In comparison with the two homoleptic counterparts (Qa3FeIII and Qb3FeIII), the proposed heteroleptic Q3FeIII complexes possessed similar coordination features to the Qb3FeIII one but showed similar catalysis performances to the Qa3FeIII one in the oxygenation of cyclohexane to cyclohexanol and cyclohexanone by hydrogen peroxide (H2O2) in acetonitrile. More importantly, both heteroleptic Q3FeIII complexes showed a better accelerating effect on this reaction and provided a slightly higher conversion than the Qa3FeIII and especially Qb3FeIII ones. Furthermore, this predominance in catalytic activity was more strikingly apparent upon both-catalyzed oxygenations of benzene, toluene, ethylbenzene or thioanisole by H2O2. This should be due to a structurally distorted effect of the heteroleptic Q3FeIII complexes that is induced by the different in ligand environment, as supported by DFT B3LYP/6-311G (d) calculation. Based the present reaction and UV-vis spectral characterization results, a free radical mechanism for the present catalysis system was proposed. © 2015 Elsevier B.V. All rights reserved.

Liao X.,Sinopec | Liao X.,Shanxi Institute of Coal CAS Chemistry | Liao X.,Hunan Changling Petrochemical SandT Developing Co. | Wang S.-G.,Shanxi Institute of Coal CAS Chemistry | And 4 more authors.
Fuel Processing Technology | Year: 2012

Three kinds of SO 3H-functionalized Brønsted-acidic ionic liquids with different acidities were applied to the etherification of glycerol with tert-butyl alcohol. High conversion and good selectivity were obtained under mild conditions. Among the ionic liquids investigated, those having a HSO 4 - anion afforded the highest glycerol conversion and those having a F 3CSO 3 - anion afforded the largest head product selectivity for glycerol etherification. The minimum-energy geometries and experimental results show that acidities and catalytic activities of ionic liquids are not only related to their structures but also to their immiscibility. © 2011 Elsevier B.V.

Liao X.,Sinopec | Liao X.,Shanxi Institute of Coal CAS Chemistry | Liao X.,Hunan Changling Petrochemical SandT Developing Co. | Li K.,Shanxi Institute of Coal CAS Chemistry | And 6 more authors.
Journal of Industrial and Engineering Chemistry | Year: 2012

SiO 2 supported ruthenium catalysts with and without modifiers were prepared, characterized and tested for glycerol hydrogenation. Addition of K, Cu and Mo affects the reducibility and acidity of the Ru/SiO 2 catalyst. Characterization data shows that Cu and Mo-modified Ru/SiO 2 have stronger acidity. On the contrary, K element on a passive effect on the acidity of Ru based catalyst had been observed. A comparison with the pure Ru/SiO 2 indicates the Cu-promoted specimen has better selective to the desired products, acetol, 1,2-propanediol and ethyl glycol, although the reactivity is slightly lower. © 2011 The Korean Society of Industrial and Engineering Chemistry.

Zou J.,Hunan Changling Petrochemical SandT Developing Co. | Xiang M.,Hunan Changling Petrochemical SandT Developing Co. | Hou B.,Shanxi Institute of Coal CAS Chemistry | Wu D.,Shanxi Institute of Coal CAS Chemistry | Sun Y.,Shanxi Institute of Coal CAS Chemistry
Journal of Natural Gas Chemistry | Year: 2011

A novel synthesis route to obtain highly dispersed molybdenum carbides in porous silica is described. The synthesis was carried out by a single-step heat treatment of molybdenum-containing and methyl-modified silica (Mo-M-SiO 2) in argon atmosphere at 973 K. Mo-M-SiO 2 precursor was facilely obtained via a one-pot synthesis route, using (NH 4) 6Mo 7O 24·4H 2O (AHM) as molybdenum sources and polymethylhydrosiloxane (PMHS) as silica sources at the initial synthetic step. The optimal C/Mo molar ratio in reaction system for complete carburization of molybdenum species was 7. The carburization process of molybdenum species followed a nontopotactic route involving a MoO 2 intermediate phase, which was evidenced by XRD, N 2 adsorption-desorption and in situ XPS. Formation mechanism of Mo-M-SiO 2 precursor was also proposed by observation of the reaction between AHM and PMHS with TEM. Furthermore, by adding TEOS into silica sources and adjusting TEOS/PMHS mass ratio, crystal phase of molybdenum carbides transferred from β-Mo 2C to α-MoC 1-x, and SiO 2 structure changed from microporous to micro/mesoporous. Catalytic performances of samples were tested using CO hydrogenation as a probe reaction. The supported molybdenum carbides exhibited high selectivity for higher alcohol synthesis compared with bulk β-Mo 2C and αMoC 1-x. © 2011 CAS/DICP.

Shen N.,Shanxi Institute of Coal CAS Chemistry | Shen N.,Hunan Changling Petrochemical SandT Developing Co. | Xiang X.,Shanxi Institute of Coal CAS Chemistry | She X.,Hunan Changling Petrochemical SandT Developing Co. | And 2 more authors.
Applied Surface Science | Year: 2012

Cu-doped α-FeOOH nanowires with diameters of 30-40 nm and lengths up to 1 μm were synthesized by a convenient hydrothermal method under mild conditions. X-ray powder diffraction (XRD) and high-resolution TEM (HRTEM) studies indicated that nanowires were single-crystalline with an oriented growth along the [1 3 0] direction. The effects of Cu-dopant content on the morphologies and crystalline phases characterized by field emission scanning electron microscopy (FE-SEM), Mössbauer and Fourier transform infrared (FT-IR) spectroscopies were also investigated. Obtained results indicated that α-(Fe,Cu)OOH nanowires were formed up to x = 2.5, whereas α-(Fe,Cu) 2O 3 nanocubes alone were obtained at x = 10, where m(Fe:Cu) = 100:x. © 2012 Elsevier B.V.

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