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13 items found (0 items not approved), displaying 11 to 13.[First/Prev] 1, 2 [Next/Last]

Instruments / Technical Area	Publication Details	Published
B18-Core EXAFS	Directed aqueous-phase reforming of glycerol through tailored platinum nanoparticles J. Callison , N. D. Subramanian , S. M. Rogers , A. Chutia , D. Gianolio , C. R. A. Catlow , P. P. Wells , N. Dimitratos Applied Catalysis B: Environmental 238, 618 - 628 DOI: 10.1016/j.apcatb.2018.07.008 Diamond Proposal Number(s): [10306] Open Access Show Abstract ▼ Abstract: Sustainable technologies require both renewable feedstocks and catalysts that are able to direct their conversion to specific products. We establish a structure-activity relationship for the aqueous phase reforming of glycerol over 2% Pt/Al2O3 catalysts, whereby the reaction pathway can be controlled to produce either hydrogen or 1,2-propanediol as the main product. Using the colloidal synthesis method, the reduction temperature was altered to produce Pt nanoparticle catalysts supported on Al2O3 with varying Pt particle size. The catalytic activity of the samples for the APR of glycerol resulted in a higher conversion of glycerol (34%) for the larger Pt particle size of ∼3.5 nm, producing the liquid 1,2-propanediol as the major product with a yield of 12.5%, whereas smaller particles of ∼2.2 nm gave hydrogen as the main product (5.5% yield). This work demonstrates how the APR of glycerol can be tuned to yield both valuable liquid and gas products using tailored Pt nanoparticles.	Dec 2018
B18-Core EXAFS	Structural behaviour of copper chloride catalysts during the chlorination of CO to phosgene Shaoliang Guan , Philip R. Davies , Emma K. Gibson , David Lennon , Giovanni E. Rossi , John M. Winfield , June Callison , Peter P. Wells , David J. Willock Faraday Discussions DOI: 10.1039/C8FD00005K Diamond Proposal Number(s): [10306] Open Access Show Abstract ▼ Abstract: The interaction of CO with an attapulgite-supported Cu(II)Cl2 catalyst has been examined in a micro-reactor arrangement. CO exposure to the dried, as-received catalyst at elevated temperatures leads to the formation of CO2 as the only identifiable product. However, phosgene production can be induced by a catalyst pre-treatment where the supported Cu(II)Cl2 sample is exposed to a diluted stream of chlorine. Subsequent CO exposure at  370C then leads to phosgene production. In order to investigate the origins of this atypical set of reaction characteristics, a series of x-ray absorption experiments were performed that were supplemented by DFT calculations. XANES measurements establish that at the elevated temperatures connected with phosgene formation, the catalyst is comprised of Cu+ and a small amount of Cu2+. Moreover, the data show that unique to the chlorine pre-treated sample, CO exposure at elevated temperature results in a short-lived oxidation of the copper. On the basis of calculated CO adsorption energies, DFT calculations indicate that a mixed Cu+/Cu2+ catalyst is required to support CO chemisorption.	Feb 2018
B18-Core EXAFS	Design and control of Lewis acid sites in Sn-substituted microporous architectures Mohammed Khaled , Arunabhiram Chutia , June Callison , Peter Philip Wells , Emma Gibson , Andrew Michael Beale , C Richard A Catlow , Robert Raja Journal Of Materials Chemistry A DOI: 10.1039/C5TA10283A Diamond Proposal Number(s): [10306] Show Abstract ▼ Abstract: Monometallic and bimetallic tin-containing framework architectures have been prepared by hydrothermal methods. Structural and spectroscopic techniques were used to probe the nature of the solid-acid sites, at the molecular level, using a combination of XRD, DR UV-Vis, solid state MAS NMR (119Sn, 27Al and 31P) and XAFS. The nature and strength of the solid-acid sites were experimentaly probed by FT-IR spectroscopy using CD3CN as a probe molecule. To elucidate further the local-structure, the structural characteristics of the Sn sites were probed using DFT calculations, with a view to rationalising the experimental findings. These detailed structural and spectroscopic studies revealed the presence of multiple Sn environments, with the monometallic SnAlPO-5 catalyst displaying a greater number of tetrahedral Sn(IV) active centres. These framework Sn(IV) centres generated stong Lewis acid sites, when compared with their bimetallic Co-Sn analogue, thereby affording attractive possibilities for modulating catalytic reactivity.	Mar 2016

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