Characterization of Au3+ species in Au/C catalysts for the hydrochlorination reaction of acetylene

A set of Au/C catalysts for the gas phase hydrochlorination of acetylene to vinyl chloride monomer were prepared using a range of strong acids as impregnating solvents and varying the preparation drying temperature. The most active catalyst is the material prepared using aqua regia as solvent with an intermediate drying temperature of 140 °C. The effects of the catalyst preparation parameters on the catalytic activity are examined using XPS and TPR as analytical tools. In particular, the use of thermal reduction methods allows the determination of kinetic parameters for the reduction of Au3+ to Au0 by means of H2. These data support the existence of a redox cycle between Au3+/Au0 when carbon is used as support

Solid State Spectroscopic Studies of Molibdenum Oxo Species with Coordinated ONR Groups

A re-study of some complexes of Mo claimed to contain coordinated C-nitroso compds. demonstrated that these solids are complex and that π-coordination of RNO cannot be the sole structural component

Aberration corrected analytical electron microscopy studies of sol-immobilized Au + Pd, AuPd and PdAu catalysts used for benzyl alcohol oxidation and hydrogen peroxide production

In this study, a systematic series of AuPd bimetallic particles were prepared by colloidal synthesis methods, in order to gain better control over the particle size distribution and structure. Particles having random alloy structures, as well as 'designer' particles with Pd-shell/Au-core and Au-shell/Pd-core morphologies, have been prepared and immobilized on both activated carbon and TiO2 supports. Aberration corrected analytical electron microscopy (ACEAM) has been extensively used to characterize these sol-immobilized materials. In particular, state-of-the-art z-contrast STEM-HAADF imaging and STEM-XEDS spectrum imaging has been employed. These techniques have provided invaluable new (and often unexpected) information on the atomic structure, elemental distribution within particles, and compositional variations between particles for these controlled catalyst preparations. In addition, we have been able to compare their differing thermal stability, sintering and wetting behaviors on activated carbon and TiO2 supports. These sol immobilized materials have also been compared as catalysts for (i) benzyl alcohol oxidation and (ii) the direct production of H2O2 in an attempt to elucidate the optimum particle morphology/support combination for each reaction. \ua9 2011 The Royal Society of Chemistry

Evolution of active catalysts for the selective oxidative dehydrogenation of methanol on Fe2O3 surface doped with Mo oxide

Iron molybdate catalysts are used for the selective oxidation of methanol to formaldehyde. In this paper we have attempted to understand what determines high selectivity in this reaction system by doping haematite with surface layers of Mo by incipient wetness impregnation. This works well and the Mo appears to form finely dispersed layers. Even very low loadings of Mo have a marked effect on improving the selectivity to formaldehyde. Haematite itself is a very poor catalyst with high selectivity to combustion products, whereas, when only 0.25 monolayers of Mo are deposited on the surface, formaldehyde and CO selectivities are greatly enhanced and CO2 production is greatly diminished. However, even with as much as seven monolayers of Mo dosed on to the surface, these materials achieve much less selectivity to formaldehyde at high conversion than do the industrial catalysts. The reason for this is that the Mo forms a 'skin' of ferric molybdate on a core of iron oxide, but does not produce a pure Mo oxide monolayer on the surface, a situation which is essential for very high yields of formaldehyde

Some recent advances in gold-based catalysis facilitated by aberration corrected analytical electron microscopy

The recent availability of aberration corrected analytical electron microscopes (ACAEM) is revolutionizing our ability to characterize nanostructured catalyst materials. Some recent case studies are presented whereby the application of the high angle annular dark field (HAADF) imaging technique, coupled with STEM-XEDS analysis, has given us a more detailed and realistic view of the catalyst morphology. The examples chosen include supported Au catalysts for low temperature CO oxidation and supported AuPd bimetallic alloy catalysts for the direct production of H2O2