Neutron Scattering Studies of Heterogeneous Catalysis
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Engineering topics
Parker, Stewart F.
Publications and source records attributed to Parker, Stewart F..
Vibrational Spectroscopy of Hexahalo Complexes
Halogenated inorganic complexes A x [MHal y ] (A = alkali metal or alkaline earth, M = transition or main group metal, x = 1–3, and y = 2–9) are an archetypal class of compounds that provide entry points to large areas of inorganic and physical chemistry. All of the hexahalo complexes adopt an octahedral, O h , symmetry (or nearly so). Consequently, one of the bending modes is forbidden in both the infrared and Raman spectra. In the solid state, many of the complexes crystallize in the cubic space group Fm3̅m, which preserves the octahedral symmetry. Even for those that are not cubic, the octahedral symmetry of the [MHal 6 ] n- ion is largely retained and, to a good approximation, so are the selection rules. In the present work, we show that by using the additional information provided by neutron vibrational spectroscopy, in combination with conventional optical spectroscopies, we can generate complete and unambiguous assignments for all the modes. Comparison of the experimental and calculated transition energies for the systems where periodic-density functional theory was possible (i.e., those for which the crystal structure is known) shows that the agreement is almost quantitative. We also provide a linear relationship that enables the prediction of the forbidden mode.
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The characterisation of commercial 2D carbons: graphene, graphene oxide and reduced graphene oxide
Commercial 2D carbon materials are shown to be largely nanographite with a small percentage of single layer material present.
Albers, Peter W.↗
Control of zeolite microenvironment for propene synthesis from methanol
Optimising the balance between propene selectivity, propene/ethene ratio and catalytic stability and unravelling the explicit mechanism on formation of the first carbon–carbon bond are challenging goals of great importance in state-of-the-art methanol-to-olefin (MTO) research. We report a strategy to finely control the nature of active sites within the pores of commercial MFI-zeolites by incorporating tantalum(V) and aluminium(III) centres into the framework. The resultant TaAlS-1 zeolite exhibits simultaneously remarkable propene selectivity (51%), propene/ethene ratio (8.3) and catalytic stability (>50 h) at full methanol conversion. In situ synchrotron X-ray powder diffraction, X-ray absorption spectroscopy and inelastic neutron scattering coupled with DFT calculations reveal that the first carbon–carbon bond is formed between an activated methanol molecule and a trimethyloxonium intermediate. The unprecedented cooperativity between tantalum(V) and Brønsted acid sites creates an optimal microenvironment for efficient conversion of methanol and thus greatly promotes the application of zeolites in the sustainable manufacturing of light olefins.
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The structure and vibrational spectroscopy of cryolite, Na 3 AlF 6
We use a combination of infrared, Raman and inelastic neutron scattering spectroscopies to access all of the modes of cryolite, Na 3 [AlF 6 ], including those that are forbidden to the optical spectroscopies.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗