An inelastic neutron scattering investigation of the temporal behaviour of the hydrocarbonaceous overlayer of a prototype Fischer-Tropsch to olefins catalyst

Sasol Ltd., the University of Glasgow and the EPSRC [award reference EP/P505534/1] are thanked for the provision of a postgraduate studentship (ALD). The Royal Society is thanked for the provision of an Industry Fellowship (PBW).A dual sodium and sulfur promoted haematite, representative of a candidate Fischer-Tropsch to olefins (FTO) catalyst, is prepared and contrasted with the performance of an unpromoted hematite sample in the ambient pressure CO hydrogenation reaction at 623 K as a function of time-on-stream (0–24 h). In-situ post-reaction temperature-programmed oxidation measurements show the carbon evolutionary phase of the catalyst conditioning process to be retarded for the FTO catalyst. Ex-situ inelastic neutron scattering measurements show the promoters perturb the formation of a previously described hydrocarbonaceous overlayer. Specifically, whilst the sp3 hybridised C–H modes of the hydrocarbonaceous overlayer are almost unaffected by the additives, the formation of the overlayer’s sp2 hybridised C–H modes are noticeably impeded. The results are discussed in terms of the Na/S promoters disturbing the formation of an ordered hydrocarbonaceous overlayer that is thought to constrain the supply of adsorbed hydrogen atoms, which favours the formation of unsaturated hydrocarbons associated with the FTO process.Publisher PDFPeer reviewe

The effect of co-feeding methyl acetate on the H-ZSM5 catalysed methanol-to-hydrocarbons reaction

The reactivity of methanol and methyl acetate mixtures over a HZSM-5 catalyst is studied over a period of 6 h at 350 °C, with small molecular weight olefins and aromatic compounds observed as reaction products. Post-reaction analysis of the catalyst shows the coke content to increase with methyl acetate content. Vibrational spectra (DRIFTS and inelastic neutron scattering, INS) indicate the major hydrocarbon species present in the coked catalysts to be methylated aromatic molecules, with INS spectra indicating a greater degree of methylation in the catalysts used with higher methyl acetate content. The greater extent of deactivation at higher methyl acetate concentrations is tentatively attributed to a diminishment of water in the zeolite cavity, which would otherwise facilitate re-generation of the active sites

RNA polymerase is poised for activation across the genome

Regulation of gene expression is integral to the development and survival of all organisms. Transcription begins with the assembly of a pre-initiation complex at the gene promoter, followed by initiation of RNA synthesis and the transition to productive elongation. In many cases, recruitment of RNA polymerase II (Pol II) to a promoter is necessary and sufficient for activation of genes. However, there are a few notable exceptions to this paradigm, including heat shock genes and several proto-oncogenes, whose expression is attenuated by regulated stalling of polymerase elongation within the promoter-proximal region. To determine the importance of polymerase stalling for transcription regulation, we carried out a genome-wide search for Drosophila melanogaster genes with Pol II stalled within the promoter-proximal region. Our data show that stalling is widespread, occurring at hundreds of genes that respond to stimuli and developmental signals. This finding indicates a role for regulation of polymerase elongation in the transcriptional responses to dynamic environmental and developmental cues

Testing decentralised treatment solutions for portable home toilet waste - Kumasi, Ghana

Water and Sanitation for the Urban Poor (WSUP) and Unilever have developed Clean Team, a business providing portable home toilets that are attractive and branded. Customers pay for their waste to be collected two to four times per week. Three “off-the-shelf” technologies are being tested to treat this waste and allow Clean Team to scale up to other cities. The three technologies are Sistema Biobolsa, which uses flexible tubes as anaerobic digesters, and aerobic planted gravel filter; Biorock, where an anaerobic pre-treatment tank is followed by an aerobic tank containing synthetic filtration media, pretreated with enzymes that stimulate the growth of aerobic bacteria and ventilation executed by natural draft; and Biofil, which will receive the sludge from the Biorock system, and digest it using macrofauna. The paper will present the initial trial results

Solar Intranetwork Magnetic Elements: bipolar flux appearance

The current study aims to quantify characteristic features of bipolar flux appearance of solar intranetwork (IN) magnetic elements. To attack such a problem, we use the Narrow-band Filter Imager (NFI) magnetograms from the Solar Optical Telescope (SOT) on board \emph{Hinode}; these data are from quiet and an enhanced network areas. Cluster emergence of mixed polarities and IN ephemeral regions (ERs) are the most conspicuous forms of bipolar flux appearance within the network. Each of the clusters is characterized by a few well-developed ERs that are partially or fully co-aligned in magnetic axis orientation. On average, the sampled IN ERs have total maximum unsigned flux of several 10^{17} Mx, separation of 3-4 arcsec, and a lifetime of 10-15 minutes. The smallest IN ERs have a maximum unsigned flux of several 10^{16} Mx, separations less than 1 arcsec, and lifetimes as short as 5 minutes. Most IN ERs exhibit a rotation of their magnetic axis of more than 10 degrees during flux emergence. Peculiar flux appearance, e.g., bipole shrinkage followed by growth or the reverse, is not unusual. A few examples show repeated shrinkage-growth or growth-shrinkage, like magnetic floats in the dynamic photosphere. The observed bipolar behavior seems to carry rich information on magneto-convection in the sub-photospheric layer.Comment: 26 pages, 14 figure

Deactivation of a single-site gold-on-carbon acetylene hydrochlorination catalyst: An X-ray absorption and inelastic neutron scattering study

Single-site Au species supported on carbon have been shown to be the active sites for acetylene hydrochlorination. The evolution of these single-site species has been monitored by Au L3 X-ray Absorption Spectroscopy (XAS). Alternating between a standard reaction mixture of HCl/C2H2 and the single reactants, has provided insights into the reaction mechanism and catalyst deactivation processes. We demonstrate that oxidative addition of HCl across an Au(I) chloride species requires concerted addition with C2H2, in accordance with both the XAS measurements of Au oxidation state and the reaction kinetics being 1st order with respect to each reactant. The addition of excess C2H2 changes the Au speciation and results in the formation of oligomeric acetylene species which were detected by inelastic neutron scattering. Catalyst deactivation at extended reaction times can be correlated with the formation of metallic Au particles. The presence of this Au(0) species generated during the sequential gas experiments or after prolonged reaction times, results in the analysis of the normalised near edge white line intensity of the Au L3 X-ray absorption spectrum alone becoming an unsuitable guide for identifying the active Au species, affecting the strong correlation between normalized white line height and VCM productivity usually observed in the active catalyst. Thus, a combination of scanning transmission electron microscopy and detailed modelling of whole XAS spectrum was required to distinguish active Au(I) and Au(III) species from the spectator Au(0) component

Red Queen Coevolution on Fitness Landscapes

Species do not merely evolve, they also coevolve with other organisms. Coevolution is a major force driving interacting species to continuously evolve ex- ploring their fitness landscapes. Coevolution involves the coupling of species fit- ness landscapes, linking species genetic changes with their inter-specific ecological interactions. Here we first introduce the Red Queen hypothesis of evolution com- menting on some theoretical aspects and empirical evidences. As an introduction to the fitness landscape concept, we review key issues on evolution on simple and rugged fitness landscapes. Then we present key modeling examples of coevolution on different fitness landscapes at different scales, from RNA viruses to complex ecosystems and macroevolution.Comment: 40 pages, 12 figures. To appear in "Recent Advances in the Theory and Application of Fitness Landscapes" (H. Richter and A. Engelbrecht, eds.). Springer Series in Emergence, Complexity, and Computation, 201

Influence of fast interstellar gas flow on dynamics of dust grains

The orbital evolution of a dust particle under the action of a fast interstellar gas flow is investigated. The secular time derivatives of Keplerian orbital elements and the radial, transversal, and normal components of the gas flow velocity vector at the pericentre of the particle's orbit are derived. The secular time derivatives of the semi-major axis, eccentricity, and of the radial, transversal, and normal components of the gas flow velocity vector at the pericentre of the particle's orbit constitute a system of equations that determines the evolution of the particle's orbit in space with respect to the gas flow velocity vector. This system of differential equations can be easily solved analytically. From the solution of the system we found the evolution of the Keplerian orbital elements in the special case when the orbital elements are determined with respect to a plane perpendicular to the gas flow velocity vector. Transformation of the Keplerian orbital elements determined for this special case into orbital elements determined with respect to an arbitrary oriented plane is presented. The orbital elements of the dust particle change periodically with a constant oscillation period or remain constant. Planar, perpendicular and stationary solutions are discussed. The applicability of this solution in the Solar system is also investigated. We consider icy particles with radii from 1 to 10 micrometers. The presented solution is valid for these particles in orbits with semi-major axes from 200 to 3000 AU and eccentricities smaller than 0.8, approximately. The oscillation periods for these orbits range from 10^5 to 2 x 10^6 years, approximately.Comment: 22 pages, 3 figures; Accepted for publication in Celestial Mechanics and Dynamical Astronom

A new measurement of direct CP violation in two pion decays of the neutral kaon

The NA48 experiment at CERN has performed a new measurement of direct CP violation, based on data taken in 1997 by simultaneously collecting K_L and K_S decays into pi0pi0 and pi+pi-. The result for the CP violating parameter Re(epsilon'/epsilon) is (18.5 +/- 4.5(stat)} +/- 5.8 (syst))x10^{-4}.Comment: 18 pages, 6 figure

Small-scale solar magnetic fields

As we resolve ever smaller structures in the solar atmosphere, it has become clear that magnetism is an important component of those small structures. Small-scale magnetism holds the key to many poorly understood facets of solar magnetism on all scales, such as the existence of a local dynamo, chromospheric heating, and flux emergence, to name a few. Here, we review our knowledge of small-scale photospheric fields, with particular emphasis on quiet-sun field, and discuss the implications of several results obtained recently using new instruments, as well as future prospects in this field of research.Comment: 43 pages, 18 figure