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This work reports on the capability of the O2-activated Cu-ZSM-5 and Cu-MOR zeolites to selectively convert methane into methanol at a temperature of 398 K. A strong correlation between (i) the activity and (ii) the intensity of the 22 700 cm-1 UV-vis band, assigned to the bis(mu-oxo)dicopper core, is found (i) as a function of the reaction temperature, (ii) as a function of the Cu loading of the zeolite, and (iii) in comparison to other Cu materials. These three lines of evidence firmly support the key role of the bis(mu-oxo)dicopper core in this selective, low-temperature hydroxylation of methane.  相似文献   
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Several magnetic and optical processes contribute to the magneto-optical response of nickel thin films after excitation by a femtosecond laser pulse. We achieved a first complete identification by explicitly measuring the time-resolved Kerr ellipticity and rotation, as well as its temperature and magnetic field dependence in epitaxially grown (111) and (001) oriented Cu/Ni/Cu wedges. The first hundreds of femtoseconds the response is dominated by state filling effects. The true demagnetization takes approximately 0.5-1 ps. At the longer (sub-ns) time scales the spins are found to precess in their anisotropy field. Simple and transparent models are introduced to substantiate our interpretation.  相似文献   
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The high‐silica zeolite SSZ‐27 was synthesized using one of the isomers of the organic structure‐directing agent that is known to produce the large‐pore zeolite SSZ‐26 ( CON ). The structure of the as‐synthesized form was solved using multi‐crystal electron diffraction data. Data were collected on eighteen crystals, and to obtain a high‐quality and complete data set for structure refinement, hierarchical cluster analysis was employed to select the data sets most suitable for merging. The framework structure of SSZ‐27 can be described as a combination of two types of cavities, one of which is shaped like a heart. The cavities are connected through shared 8‐ring windows to create straight channels that are linked together in pairs to form a one‐dimensional channel system. Once the framework structure was known, molecular modelling was used to find the best fitting isomer, and this, in turn, was isolated to improve the synthesis conditions for SSZ‐27.  相似文献   
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A new germanosilicate zeolite named SCM-15 (Sinopec Composite Material No. 15), the first zeolite containing a 3-dimensional (3D) channel system with interconnected 12-, 12-, and 10-ring channels (pore sizes: 6.1×7.2, 6.1×7.4, and 5.2×5.9 Å), has been synthesized using neutral 4-pyrrolidinopyridine as organic structure-directing agents (OSDAs). Its structure has been determined by combining single-crystal electron diffraction (SCED) and synchrotron powder X-ray diffraction (SPXD) data. The unique open framework structure of SCM-15 is related to that of FOS-5 ( BEC ), ITQ-7 ( ISV ), PKU-16 ( POS ), ITQ-26 ( IWS ), ITQ-21, Beta polymorph B, and SU-78B, since all these framework structures can be constructed from similar chains which are connected through shared 4-ring or double 4-ring (d4r) units. Based on this relation, six topologically reasonable 3D large or extra-large pore hypothetical zeolites are predicted.  相似文献   
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The synthesis of the new potentially tridentate ligand 3,5-bis(dimethylaminomethyl)pyridine ( 3 ) is described. Coordination chemistry of this ligand has been investigated with PdII and PtII precursor compounds. Both a bidentate bridging bonding motif and a monodentate bonding mode is observed. The latter compounds incorporate 3 by coordination through the pyridinic N atom only. The former complexes contain ligand 3 bonded to 2 metal centres by bridging through coordination of one trialkyl N donor atom and the pyridinic N atom. The solid-state structure of a ligand bridged Pd dimer has been elucidated by single-crystal X-ray diffraction and corroborates with the solid-state IR data that suggested a trans-PdCl2 unit was present.  相似文献   
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The effect the catalytic chain transfer agent, bis[(difluoroboryl) dimethylglyoximato] cobalt(II) (COBF), on the course of the ab initio emulsion polymerization of methyl methacrylate, and the product properties in terms of the molecular weight distribution were investigated. The emulsion polymerization kinetics have been studied with varying surfactant, initiator, and COBF concentrations. The experimentally determined average number of radicals per particle strongly depends on the concentration of COBF and proves to be in good agreement with the results of model calculations. The apparent chain transfer constant, determined up to high conversion, is in excellent agreement with the predicted value based on a mathematical model based on COBF partitioning and the Mayo equation. The results of this work enhance the fundamental understanding of the influence a catalytic chain transfer agent has on the course of the emulsion polymerization and the control of the molecular weight distribution. © 2009 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 5078–5089, 2009  相似文献   
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