195,114 research outputs found
Recent advances on simulation and theory of hydrogen storage in metal–organic frameworks and covalent organic frameworks
This critical review covers the application of computer simulations, including quantum calculations (ab initio and DFT), grand canonical Monte-Carlo simulations, and molecular dynamics simulations, to the burgeoning area of the hydrogen storage by metal–organic frameworks and covalent-organic frameworks. This review begins with an overview of the theoretical methods obtained from previous studies. Then strategies for the improvement of hydrogen storage in the porous materials are discussed in detail. The strategies include appropriate pore size, impregnation, catenation, open metal sites in metal oxide parts and within organic linker parts, doping of alkali elements onto organic linkers, substitution of metal oxide with lighter metals, functionalized organic linkers, and hydrogen spillover (186 references)
The Influence of Aromatic Compounds on Viscosity
Imperial Users onl
Vibrational properties of alpha- and sigma-phase Fe-Cr alloy
Experimental investigation as well as theoretical calculations, of the
Fe-partial phonon density-of-states (DOS) for nominally Fe_52.5Cr_47.5 alloy
having (a) alpha- and (b) sigma-phase structure were carried out. The former at
sector 3-ID of the Advanced Photon Source, using the method of nuclear resonant
inelastic X-ray scattering, and the latter with the direct method [K. Parlinski
et al., Phys. Rev. Lett. {78, 4063 (1997)]. The characteristic features of
phonon DOS, which differentiate one phase from the other, were revealed and
successfully reproduced by the theory. Various data pertinent to the dynamics
such as Lamb-Mossbauer factor, f, kinetic energy per atom, E_k, and the mean
force constant, D, were directly derived from the experiment and the
theoretical calculations, while vibrational specific heat at constant volume,
C_V, and vibrational entropy, S were calculated using the Fe-partial DOS. Using
the values of f and C_V, we determined values for Debye temperatures, T_D. An
excellent agreement for some quantities derived from experiment and
first-principles theory, like C_V and quite good one for others like D and S
was obtained.Comment: 4 pages, 3 figure
Glass transition and layering effects in confined water: a computer simulation study
Single particle dynamics of water confined in a nanopore is studied through
Computer Molecular Dynamics. The pore is modeled to represent the average
properties of a pore of Vycor glass. Dynamics is analyzed at different
hydration levels and upon supercooling. At all hydration levels and all
temperatures investigated a layering effect is observed due to the strong
hydrophilicity of the substrate. The time density correlators show, already at
ambient temperature, strong deviations from the Debye and the stretched
exponential behavior. Both on decreasing hydration level and upon supercooling
we find features that can be related to the cage effect typical of a
supercooled liquid undergoing a kinetic glass transition. Nonetheless the
behavior predicted by Mode Coupling Theory can be observed only by carrying out
a proper shell analysis of the density correlators. Water molecules within the
first two layers from the substrate are in a glassy state already at ambient
temperature (bound water). The remaining subset of molecules (free water)
undergoes a kinetic glass transition; the relaxation of the density correlators
agree with the main predictions of the theory. From our data we can predict the
temperature of structural arrest of free water.Comment: 14 pages, 15 figures inserted in the text, to be published in J.
Chem. Phys. (2000
Equilibrium Clusters in Concentrated Lysozyme Protein Solutions
We have studied the structure of salt-free lysozyme at 293 K and pH 7.8 using
molecular simulations and experimental SAXS effective potentials between
proteins at three volume fractions, 0.012, 0.033, and 0.12. We found that the
structure of lysozyme near physiological conditions strongly depends on the
volume fraction of proteins. The studied lysozyme solutions are dominated by
monomers only for <0.012; for the strong dilution 70% of proteins are in a form
of monomers. For 0.033 only 20% of proteins do not belong to a cluster. The
clusters are mainly elongated. For 0.12 almost no individual particles exits,
and branched, irregular clusters of large extent appear. Our simulation study
provides new insight into the formation of equilibrium clusters in charged
protein solutions near physiological conditions
Adsorption Mechanism and Uptake of Methane in Covalent Organic Frameworks: Theory and Experiment
We determined the methane (CH_4) uptake (at 298 K and 1 to 100 bar pressure) for a variety of covalent organic frameworks (COFs), including both two-dimensional (COF-1, COF-5, COF-6, COF-8, and COF-10) and three-dimensional (COF-102, COF-103, COF-105, and COF-108) systems. For all COFs, the CH_4 uptake was predicted from grand canonical Monte Carlo (GCMC) simulations based on force fields (FF) developed to fit accurate quantum mechanics (QM) [second order Møller−Plesset (MP2) perturbation theory using doubly polarized quadruple-ζ (QZVPP) basis sets]. This FF was validated by comparison with the equation of state for CH_4 and by comparison with the experimental uptake isotherms at 298 K (reported here for COF-5 and COF-8), which agrees well (within 2% for 1−100 bar) with the GCMC simulations. From our simulations we have been able to observe, for the first time, multilayer formation coexisting with a pore filling mechanism. The best COF in terms of total volume of CH_4 per unit volume COF absorbent is COF-1, which can store 195 v/v at 298 K and 30 bar, exceeding the U.S. Department of Energy target for CH_4 storage of 180 v/v at 298 K and 35 bar. The best COFs on a delivery amount basis (volume adsorbed from 5 to 100 bar) are COF-102 and COF-103 with values of 230 and 234 v(STP: 298 K, 1.01 bar)/v, respectively, making these promising materials for practical methane storage
Different Approaches to Proof Systems
The classical approach to proof complexity perceives proof systems as deterministic, uniform, surjective, polynomial-time computable functions that map strings to (propositional) tautologies. This approach has been intensively studied since the late 70’s and a lot of progress has been made. During the last years research was started investigating alternative notions of proof systems. There are interesting results stemming from dropping the uniformity requirement, allowing oracle access, using quantum computations, or employing probabilism. These lead to different notions of proof systems for which we survey recent results in this paper
Interacting Frobenius Algebras are Hopf
Theories featuring the interaction between a Frobenius algebra and a Hopf
algebra have recently appeared in several areas in computer science: concurrent
programming, control theory, and quantum computing, among others. Bonchi,
Sobocinski, and Zanasi (2014) have shown that, given a suitable distributive
law, a pair of Hopf algebras forms two Frobenius algebras. Here we take the
opposite approach, and show that interacting Frobenius algebras form Hopf
algebras. We generalise (BSZ 2014) by including non-trivial dynamics of the
underlying object---the so-called phase group---and investigate the effects of
finite dimensionality of the underlying model. We recover the system of Bonchi
et al as a subtheory in the prime power dimensional case, but the more general
theory does not arise from a distributive law.Comment: 32 pages; submitte
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