475 research outputs found
Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles
Open Access Article. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.Two phosphine-stabilised gold clusters, Au101(PPh3)21Cl5 and Au9(PPh3)8(NO3)3, were deposited and activated on anatase TiO2 and fumed SiO2. These catalysts showed an almost complete oxidation of benzyl alcohol (>90%) within 3 hours at 80 °C and 3 bar O2 in methanol with a high substrate-to-metal molar ratio of 5800 and turn-over frequency of 0.65 s−1. Factors influencing catalytic activity were investigated, including metal–support interaction, effects of heat treatments, chemical composition of gold clusters, the size of gold nanoparticles and catalytic conditions. It was found that the anions present in gold clusters play a role in determining the catalytic activity in this reaction, with NO3− diminishing the catalytic activity. High catalytic activity was attributed to the formation of large gold nanoparticles (>2 nm) that coincides with partial removal of ligands which occurs during heat treatment and catalysis. Selectivity towards the formation of methyl benzoate can be tuned by selection of the reaction temperature. The catalysts were characterised using transmission electron microscopy, UV-vis diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy
Towards Better Integrators for Dissipative Particle Dynamics Simulations
Coarse-grained models that preserve hydrodynamics provide a natural approach
to study collective properties of soft-matter systems. Here, we demonstrate
that commonly used integration schemes in dissipative particle dynamics give
rise to pronounced artifacts in physical quantities such as the compressibility
and the diffusion coefficient. We assess the quality of these integration
schemes, including variants based on a recently suggested self-consistent
approach, and examine their relative performance. Implications of
integrator-induced effects are discussed.Comment: 4 pages, 3 figures, 2 tables, accepted for publication in Phys. Rev.
E (Rapid Communication), tentative publication issue: 01 Dec 200
Random Resonators and Prelocalized Modes in Disordered Dielectric Films
Areal density of disorder-induced resonators with a high quality factor,
, in a film with fluctuating refraction index is calculated
theoretically. We demonstrate that for a given , where is the light
wave vector, and is the transport mean free path, when {\em on average} the
light propagation is diffusive, the likelihood for finding a random resonator
increases dramatically with increasing the correlation radius of the disorder.
Parameters of {\em most probable} resonators as functions of and are
found.Comment: 6 pages including 2 figure
Bottom mixed layer oxygen dynamics in the Celtic Sea
The seasonally stratified continental shelf seas are highly productive, economically important environments which are under considerable pressure from human activity. Global dissolved oxygen concentrations have shown rapid reductions in response to anthropogenic forcing since at least the middle of the twentieth century. Oxygen consumption is at the same time linked to the cycling of atmospheric carbon, with oxygen being a proxy for carbon remineralisation and the release of CO2. In the seasonally stratified seas the bottom mixed layer (BML) is partially isolated from the atmosphere and is thus controlled by interplay between oxygen consumption processes, vertical and horizontal advection. Oxygen consumption rates can be both spatially and temporally dynamic, but these dynamics are often missed with incubation based techniques. Here we adopt a Bayesian approach to determining total BML oxygen consumption rates from a high resolution oxygen time-series. This incorporates both our knowledge and our uncertainty of the various processes which control the oxygen inventory. Total BML rates integrate both processes in the water column and at the sediment interface. These observations span the stratified period of the Celtic Sea and across both sandy and muddy sediment types. We show how horizontal advection, tidal forcing and vertical mixing together control the bottom mixed layer oxygen concentrations at various times over the stratified period. Our muddy-sand site shows cyclic spring-neap mediated changes in oxygen consumption driven by the frequent resuspension or ventilation of the seabed. We see evidence for prolonged periods of increased vertical mixing which provide the ventilation necessary to support the high rates of consumption observed
Maintenance care for treated periodontitis patients
This paper is a review of current literature combined with clinical observations. Well-controlled maintenance care is a key consideration in the long-term prognosis of treated periodontitis patients. Periodic professional tooth cleaning every 3 to 4 months often is recommended. Furthermore, recent studies indicate a potential need for selected retreatment in problem areas, since minute residual accretions may be left behind during active therapy - even with “open” surgery. While efficient plaque control is essential for optimal results during the healing phase of periodontal therapy, periodic prophylaxis may prevent loss of clinical attachment over long periods of time even for patients with less than perfect oral hygiene.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/72615/1/j.1600-051X.1987.tb02247.x.pd
Heterodinuclear ruthenium(II)-cobalt(III) complexes as models for a new approach to selective cancer treatment
Heterodinuclear ruthenium(ii)-cobalt(iii) complexes have been prepared as part of investigations into a new approach to selective cancer treatment. A cobalt(iii) centre bearing amine ligands, which serve as models for cytotoxic nitrogen mustard ligands, is connected by a bridging ligand to a ruthenium(ii)-polypyridyl moiety. Upon excitation of the ruthenium centre by visible light, electron transfer to the cobalt(iii) centre results in reduction to cobalt(ii) and consequent release of its ligands. We have synthesised several such structures and demonstrated their ability to release ligands upon excitation of the ruthenium centre by visible light
Mycobacterium marinum antagonistically induces an autophagic response while repressing the autophagic flux in a TORC1- and ESX-1-dependent manner.
Autophagy is a eukaryotic catabolic process also participating in cell-autonomous defence. Infected host cells generate double-membrane autophagosomes that mature in autolysosomes to engulf, kill and digest cytoplasmic pathogens. However, several bacteria subvert autophagy and benefit from its machinery and functions. Monitoring infection stages by genetics, pharmacology and microscopy, we demonstrate that the ESX-1 secretion system of Mycobacterium marinum, a close relative to M. tuberculosis, upregulates the transcription of autophagy genes, and stimulates autophagosome formation and recruitment to the mycobacteria-containing vacuole (MCV) in the host model organism Dictyostelium. Antagonistically, ESX-1 is also essential to block the autophagic flux and deplete the MCV of proteolytic activity. Activators of the TORC1 complex localize to the MCV in an ESX-1-dependent manner, suggesting an important role in the manipulation of autophagy by mycobacteria. Our findings suggest that the infection by M. marinum activates an autophagic response that is simultaneously repressed and exploited by the bacterium to support its survival inside the MCV
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Detection and attribution of human influence on regional precipitation
Understanding how human influence on climate is affecting precipitation around the world is immensely important for defining mitigation policies, and for adaptation planning. Yet despite increasing evidence for the influence of climate change on global patterns of precipitation, and expectations that significant changes in regional precipitation should have already occurred as a result of human influence on climate, compelling evidence of anthropogenic fingerprints on regional precipitation is obscured by observational and modelling uncertainties and is likely to remain so using current methods for years to come. This is in spite of substantial ongoing improvements in models, new reanalyses and a satellite record that spans over thirty years. If we are to quantify how human-induced climate change is affecting the regional water cycle, we need to consider novel ways of identifying the effects of natural and anthropogenic influences on precipitation that take full advantage of our physical expectations
Conformation and interactions of polystyrene and fullerenes in dilute to semidilute solutions
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