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  • 1
    Electronic Resource
    Electronic Resource
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 98 (1994), S. 9637-9641 
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 98 (1994), S. 13625-13630 
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    Westerville, Ohio : American Ceramics Society
    Journal of the American Ceramic Society 84 (2001), S. 0 
    ISSN: 1551-2916
    Source: Blackwell Publishing Journal Backfiles 1879-2005
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Atomistic simulation techniques have been used to model the dissociative adsorption of water onto the low-index {100}, {110}, and {111} surfaces of spinel MgAl2O4. The Born model of solids and the shell model for oxygen polarization have been used. The resulting structures and chemical bonding on the clean and hydrated surfaces are described. The calculations show that the dissociative adsorption of water on the low-index surfaces is generally energetically favorable. For the {110} and {111} orientations, the surfaces cleaved between oxygen layers show high absorption and stability. The calculations also show that, for the {111} orientation, the surfaces may absorb chemically water molecules up to ∼90% coverage and have the highest stability. It is suggested that, during fracture, only partial hydration occurs, leading to cleavage preferentially along the {100} orientation.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    Westerville, Ohio : American Ceramics Society
    Journal of the American Ceramic Society 82 (1999), S. 0 
    ISSN: 1551-2916
    Source: Blackwell Publishing Journal Backfiles 1879-2005
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Chemisorption and physisorption of water onto the {0001}, {1011}, {1120}, and {2243} surfaces of alpha-alumina have been studied via atomistic simulation techniques, using potentials that have been verified against the structures of hydrated ß-alumina and diaspore. Both physisorption and chemisorption of all surfaces are energetically favorable, especially the hydroxylation of dipolar oxygen-terminated planes. The equilibrium morphology is calculated, as a way to assess the change in surface energies, and the equilibrium morphologies agree with the experimentally observed crystal morphologies. The calculated energies of both physisorption and chemisorption agree well with experimentally obtained hydration energies.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    Westerville, Ohio : American Ceramics Society
    Journal of the American Ceramic Society 83 (2000), S. 0 
    ISSN: 1551-2916
    Source: Blackwell Publishing Journal Backfiles 1879-2005
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Atomistic simulations with atomic potentials including anion polarizibility have been performed for the low-index surfaces of spinel MgAl2O4 with various terminations. The calculations show that for the most stable surface the surface energy is 2.27 J/m2 for the {100}, about 2.85 J/m2 for the {110}, and 3.07 J/m2 for the {111} orientation. The ratio between the experimental values to the calculated relaxed surface energies is about 1.5. Strong surface relaxation was found for the {110} and {111} orientation but only moderate surface relaxation for the {100} surface.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    Springer
    Physics and chemistry of minerals 10 (1984), S. 209-216 
    ISSN: 1432-2021
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences , Physics
    Notes: Abstract The aim of the work presented is to develop a computer simulation technique which will predict the structure and physical properties of forsterite and ringwoodite, the major mantle-forming polymorphs of Mg2SiO4. The technique is based upon energy minimization, in which all structural parameters are varied until the configuration with the lowest energy is achieved. The lattice energy and physical properties (e.g. elasticity and dielectric constants) are calculated from interatomic potentials, which generally include electrostatic and short-range terms. We investigate several types of traditional potential models, and present a new type of model which includes partial ionic charges and a Morse potential to describe the effect of covalency on the Si-O bond. This new form of potential model is highly successful, and not only reproduces the zero-pressure structural, elastic and dielectric properties of forsterite and ringwoodite, but also accurately describes their pressure dependence.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    Springer
    Physics and chemistry of minerals 15 (1987), S. 181-190 
    ISSN: 1432-2021
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences , Physics
    Notes: Abstract We use an approach based upon the Born model of solids, in which potential functions represent the interactions between atoms in a structure, to calculate the phonon dispersion of forsterite and the lattice dynamical behaviour of the beta-phase and spinel polymorphs of Mg2SiO4. The potential used (THB1) was derived largely empirically using data from simple binary oxides, and has previously been successfully used to model the infrared and Raman behaviour of forsterite. It includes ‘bond bending’ terms, that model the directionality of the Si-O bond, in addition to the pair-wise additive Coulombic and short range terms. The phonon dispersion relationships of the Mg2SiO4 polymorphs predicted by THB1 were used to calculate the heat capacities, entropies, thermal expansion coefficients and Gruneisen parameters of these phases. The predicted heat capacities and entropies are in outstandingly good agreement with those determined experimentally. The predicted thermodynamic data of these phases were used to construct a phase diagram for this system, which has Clausius-Clapeyron slopes in very close agreement with those found by experiment, but which has predicted transformation pressures that show less close agreement with those inferred from experiment. The overall success, however, that we have in predicting the lattice dynamical and thermodynamic properties of the Mg2SiO4 polymorphs shows that our potential THB1 represents a significant step towards finding the elusive quantitative link between the microscopic or atomistic behaviour of minerals and their macroscopic properties.
    Type of Medium: Electronic Resource
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  • 8
    ISSN: 1572-879X
    Keywords: gold ; TiO2 ; model catalysts ; CO oxidation ; support effects
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Very tiny Au particles on TiO2 show excellent activity and selectivity in a number of oxidation reactions. We have studied the vapor deposition of Au onto a TiO2(110) surface using XPS, LEIS, LEED and TPD and found that we can prepare Au islands with controlled thicknesses from one to several monolayers. In order to understand at the atomic level the unusual catalytic activity in oxidation reactions of this system, we have studied oxygen adsorption on Au/TiO2(110) as a function of Au island thickness, and have measured the titration of this adsorbed oxygen with CO gas to yield CO2, as function of Au island thickness, CO pressure and temperature. A hot filament was used to dose gaseous oxygen atoms. TPD results show higher O2 desorption temperatures (741 K) from ultrathin gold particles on TiO2(110) than from thicker particles (545 K). This implies that Oa bonds much more strongly to ultrathin islands of Au. Thus from Brønsted relations, ultrathin gold particles should be able to dissociatively adsorb O2 more readily than thick gold particles. Our studies of the titration reaction of oxygen adatoms with CO (to produce CO2) show that this reaction is extremely rapid at room temperature, but its rate is slightly slower for the thinnest Au islands. Thus the association reaction (COg + Oa → CO2,g) gets faster as the oxygen adsorption strength decreases, again as expected from Brønsted relations. For islands of about two atomic layers thickness, the rate increases slowly with temperature, with an apparent activation energy of 11.4 ± 2.8 kJ/mol, and shows a first‐order rate in CO pressure and oxygen coverage, similar to bulk Au(110).
    Type of Medium: Electronic Resource
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  • 9
    ISSN: 1572-9028
    Keywords: adsorption energies ; adhesion energies ; model catalysts ; metal nanoparticles ; oxide surfaces ; structural sensitivity ; Pt/ZnO ; Cu/ZnO ; Au/TiO2
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Many industrially important catalysts consist of late transition metal particles supported on the surfaces of oxide materials. Our studies of such systems using model catalysts consisting of metal films vapor deposited onto the surfaces of single-crystalline oxides are reviewed here. Systems studied include Cu on ZnO, Pt on ZnO, Au on TiO2 and Cu, Ag and Pb on MgO. A unique adsorption microcalorimeter was developed to measure directly the energetic stability of the metal atoms on the oxide surfaces and the adhesion energy at the metal/oxide interface, which clarify the structural and chemisorption properties of the ultrathin metal particles. The structure of the oxide surface and the metal particles was elucidated by low-energy electron diffraction (LEED), low-energy ion scattering spectroscopy (ISS), angular-resolved X-ray photoelectron spectroscopy (XPS) and X-ray photoelectron diffraction (XPD). The electronic character of the metal particles was revealed by XPS, Auger electron spectroscopy (AES), band-bending and work function measurements. Sintering rates were measured by temperature-programmed ion scattering spectroscopy (TPISS). The chemisorption properties of these particles and their catalytic reactivity were monitored by mass spectroscopy and temperature-programmed desorption (TPD).
    Type of Medium: Electronic Resource
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  • 10
    Publication Date: 2017-02-13
    Description: Genome-wide association studies (GWAS) have identified 〉100 independent SNPs that modulate the risk of type 2 diabetes (T2D) and related traits. However, the pathogenic mechanisms of most of these SNPs remain elusive. Here, we examined genomic, epigenomic, and transcriptomic profiles in human pancreatic islets to understand the links between genetic variation, chromatin landscape, and gene expression in the context of T2D. We first integrated genome and transcriptome variation across 112 islet samples to produce dense cis-expression quantitative trait loci (cis-eQTL) maps. Additional integration with chromatin-state maps for islets and other diverse tissue types revealed that cis-eQTLs for islet-specific genes are specifically and significantly enriched in islet stretch enhancers. High-resolution chromatin accessibility profiling using assay for transposase-accessible chromatin sequencing (ATAC-seq) in two islet samples enabled us to identify specific transcription factor (TF) footprints embedded in active regulatory elements, which are highly enriched for islet cis-eQTL. Aggregate allelic bias signatures in TF footprints enabled us de novo to reconstruct TF binding affinities genetically, which support the high-quality nature of the TF footprint predictions. Interestingly, we found that T2D GWAS loci were strikingly and specifically enriched in islet Regulatory Factor X (RFX) footprints. Remarkably, within and across independent loci, T2D risk alleles that overlap with RFX footprints uniformly disrupt the RFX motifs at high-information content positions. Together, these results suggest that common regulatory variations have shaped islet TF footprints and the transcriptome and that a confluent RFX regulatory grammar plays a significant role in the genetic component of T2D predisposition.
    Print ISSN: 0027-8424
    Electronic ISSN: 1091-6490
    Topics: Biology , Medicine , Natural Sciences in General
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