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We present first-principles kinetic Monte Carlo (1p-kMC) simulations addressing the CO oxidation reaction at Pd(100) for gas-phase conditions ranging from ultra-high vacuum to ambient pressures and elevated temperatures. For the latter technologically relevant regime there is a long-standing debate regarding the nature of the active surface. The pristine metallic surface, an ultra-thin $(\sqrt{5}\times \sqrt{5})R27^{\circ}$ PdO(101) surface oxide, and thicker oxide layers have each been suggested as the active state. We investigate these hypotheses with 1p-kMC simulations focusing on either the Pd(100) surface or the PdO(101) surface oxide and intriguingly obtain a range of (T, p)-conditions where both terminations appear metastable. The predicted bistability regime nicely ties in with oscillatory behavior reported experimentally by Hendriksen et al. (Catal Today 105:234, 2005). Within this regime we find that both surface terminations exhibit very similar intrinsic reactivity, which puts doubts on attempts to assign the catalytic function to just one active state. 相似文献
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Karsten J. Quint Stefan Hartmann Steffen Rothe Nicolas Saba Kurt Steinhoff 《Computational Mechanics》2011,48(1):81-96
An accurate prediction of the temperature distribution in space and time plays an important role in many industrial applications,
in particular when phase transformations are involved. In this article the thermo-physical properties of steel 51CrV4 (SAE
6150) are determined and used in numerical simulations. For the simulation of the temperature field a semi-discrete approach
is used, consisting of a finite element approximation in space and a high order Runge– Kutta integration in time. Several
adaptive high-order time integration method (stiffly accurate diagonally implicit Runge–Kutta methods) are applied and their
computational efficiency is investigated. The theoretical rates of convergence are achieved for all problems, including the
non-linear case. Whereas the second order accurate method of Ellsiepen with time adaptive step-size control proves to be most
efficient. Further, the influence of the material model on the simulation results is studied and the numerical results are
verified by experiments. The best correlation of the simulation and experimental data is achieved using temperature-dependent
parameters. 相似文献
75.
Volatilization of organotin species from municipal waste deposits: novel species identification and modeling of atmospheric stability 总被引:1,自引:0,他引:1
Krupp EM Merle JK Haas K Foote G Maubec N Feldmann J 《Environmental science & technology》2011,45(3):943-950
Organotin compounds are used as pesticides and fungicides as well as additives in plastics. This study identifies the de novo generation of novel volatile organotins in municipal waste deposits and their release via landfill gas. Besides tetramethyltin (Me(4)Sn), a strong neurotoxin, and 5 previously reported organotins, 13 novel ethylated, propylated, and butylated tetraalkyltin compounds were identified. A concentration of 2-4 μg of Sn m(-3) landfill gas was estimated for two landfill sites in Scotland. The atmospheric stability of Me(4)Sn and methylated tin hydrides was determined empirically in a static atmosphere in the dark and under UV light to simulate night- and daytime conditions. Theoretical calculations were carried out to help predict the experimentally obtained stabilities and to estimate the relative stabilities of other alkylated species. Assuming first-order kinetics, the atmospheric half-life for Me(3)SnH was found to be 33 ± 16 and 1311 ± 111 h during day- and nighttime conditions, respectively. Polyalkylation and larger alkyl substitutes tend to reduce the atmospheric stability. These results show that substantial concentrations of neurotoxic organotin compounds can be released from landfill sites and are sufficiently stable in the atmosphere to travel over large distances in night- and daytime conditions to populated areas. 相似文献
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Daniel H. Mendelsohn Katja Schnabel Andreas Mamilos Samuel Sossalla Steffen Pabel Georg Daniel Duerr Karsten Keller Volker H. Schmitt Friedrich Barsch Nike Walter Ronald Man Yeung Wong Thaqif El Khassawna Tanja Niedermair Volker Alt Markus Rupp Christoph Brochhausen 《International journal of molecular sciences》2022,23(9)
Mitochondria play a crucial role in cell physiology and pathophysiology. In this context, mitochondrial dynamics and, subsequently, mitochondrial ultrastructure have increasingly become hot topics in modern research, with a focus on mitochondrial fission and fusion. Thus, the dynamics of mitochondria in several diseases have been intensively investigated, especially with a view to developing new promising treatment options. However, the majority of recent studies are performed in highly energy-dependent tissues, such as cardiac, hepatic, and neuronal tissues. In contrast, publications on mitochondrial dynamics from the orthopedic or trauma fields are quite rare, even if there are common cellular mechanisms in cardiovascular and bone tissue, especially regarding bone infection. The present report summarizes the spectrum of mitochondrial alterations in the cardiovascular system and compares it to the state of knowledge in the musculoskeletal system. The present paper summarizes recent knowledge regarding mitochondrial dynamics and gives a short, but not exhaustive, overview of its regulation via fission and fusion. Furthermore, the article highlights hypoxia and its accompanying increased mitochondrial fission as a possible link between cardiac ischemia and inflammatory diseases of the bone, such as osteomyelitis. This opens new innovative perspectives not only for the understanding of cellular pathomechanisms in osteomyelitis but also for potential new treatment options. 相似文献
80.
Influence of Temperature on the Colloidal Stability of Polymer‐Coated Gold Nanoparticles in Cell Culture Media 下载免费PDF全文
Mikhail V. Zyuzin Tobias Honold Susana Carregal‐Romero Karsten Kantner Matthias Karg Wolfgang J. Parak 《Small (Weinheim an der Bergstrasse, Germany)》2016,12(13):1723-1731
The temperature‐dependence of the hydrodynamic diameter and colloidal stability of gold‐polymer core‐shell particles with temperature‐sensitive (poly(N‐isopropylacrylamide)) and temperature‐insensitive shells (polyallylaminine hydrochloride/polystyrensulfonate, poly(isobutylene‐alt‐maleic anhydride)‐graft‐dodecyl) are investigated in various aqueous media. The data demonstrate that for all nanoparticle agglomeration, i.e., increase in effective nanoparticle size, the presence of salts or proteins in the dispersion media has to be taken into account. Poly(N‐isopropylacrylamide) coated nanoparticles show a reversible temperature‐dependent increase in size above the volume phase transition of the polymer shell when they are dispersed in phosphate buffered saline or in media containing protein. In contrast, the nanoparticles coated with temperature‐insensitive polymers show a time‐dependent increase in size in phosphate buffered saline or in medium containing protein. This is due to time‐dependent agglomeration, which is particularly strong in phosphate buffered saline, and induces a time‐dependent, irreversible increase in the hydrodynamic diameter of the nanoparticles. This demonstrates that one has to distinguish between temperature‐ and time‐induced agglomerations. Since the size of nanoparticles regulates their uptake by cells, temperature‐dependent uptake of thermosensitive and non‐thermosensitive nanoparticles by cells lines is compared. No temperature‐specific difference between both types of nanoparticles could be observed. 相似文献