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41.
Martin Macháček 《Journal of statistical physics》1987,47(5-6):949-952
We define mathematically a class of dynamical systems that exhibit relaxation corresponding to that observed in physical systems, and then show that this class is identical with the class ofK-mixing dynamical systems. 相似文献
42.
Using the Picker flow microcalorimeter, excess heat capacities have been obtained at 25°C throughout the concentration range for 2,2-dimethylbutane,n-hexane, and cyclohexane each mixed with a series of hexadecane isomers of increasing degrees of orientational order, as determined by depolarized Rayleigh scattering. The isomers are 2,2,4,4,6,8,8-heptamethylnonane, 6-, 4-, and 2-methylpentadecane, andn-hexadecane. Thec
p
E
values are negative, increasing rapidly in magnitude with increase of orientational order, and are not predicted by the Prigogine—Flory theory which neglects order. Values ofc
p
E
are obtained at 10, 25, and 55°C for cyclohexane +6-, 4-, and 2-methylpentadecane which with other literature data lead to the temperature dependence of the thermodynamic excess functions for cyclohexane solutions of the five C16 isomers. The excess enthalpy and entropy vary with the C16 isomer and with temperature, but the corresponding variation of the excess free energy is small, indicating a high degree of enthalpy-entropy compensation. This is consistent with a rapid decrease with temperature of orientational order in the C16 isomers. 相似文献
43.
The kinetic method is one of the most widely used experimental techniques for the measurement of thermochemical parameters by mass spectrometry. Recently it has been realized that it can also be used to determine reaction entropies, but the validity of this approach has not been established. This Perspective evaluates kinetic method plots in cases where there is a significant entropy difference between the competing fragmentation channels (i.e. between sample and reference compounds in the dissociating cluster ion). The concept underlying this study is to calculate mass spectra theoretically, based on known thermochemical parameters and as a function of experimental conditions. This can be done accurately using the RRKM-based MassKinetics software. The resulting mass spectra are then interpreted by the kinetic method, yielding DeltaH and DeltaS values. These values are, in turn, compared with the true values used to generate the calculated mass spectra. The results show that the reaction entropy difference between sample and reference has a very large influence on kinetic method plots. This should always be considered when studying energy-dependent mass spectra (using metastable ions or low- or high-energy collision-induced dissociation (CID)), even if only DeltaH is to be determined. Kinetic method plots are not strictly linear and this becomes a serious issue in the case of small molecules showing a large entropy effect. In such cases, results obtained at a low degree of excitation are more accurate. Energy and entropy effects can be evaluated in a relatively straightforward manner: first, the apparent Gibbs energy (DeltaG(app)) and effective temperature (T(eff)) are determined from kinetic method plots (intercept and slope, respectively), obtained from experiments using various degrees of excitation. Second, the resulting DeltaG(app) is plotted against T(eff), the slope yielding DeltaS while the intercept (extrapolation to zero temperature) yields DeltaH. This data evaluation yields more accurate results than alternative methods used in the literature. The resulting DeltaH values are fairly accurate, with errors, in most cases, <4 kJ mol(-1). On the other hand, DeltaS is systematically underestimated by 20-40%. Empirically scaling DeltaS values determined by the kinetic method by 1.35 results in a DeltaS value within 20% (or 10 J mol(-1) K(-1)) of the theoretical value. 相似文献
44.
The pressure of thermal dissociation of platinum tetrachloride by the first step PtCl4(s) = PtCl3(s) + 0.5 Cl2(g) was measured by the static method with a quartz membrane-gauge zero-pressure manometer. An approximating equation for the dissociation pressure vs. temperature was found. The enthalpy (52160±880 J mol−1) and entropy (72.1±1.6 J mol−1 K−1) of dissociation were calculated. The heat of formation found for platinum tetrachloride (−246.3±1.3 kJ mol−1) at 298.15 K agrees well with the value obtained by the calorimetric method (−245.6±1.9 kJ mol−1).__________Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 10, pp. 2028–2031, October, 2004. 相似文献
45.
Y. Marcus 《Journal of solution chemistry》1994,23(7):831-848
The water-structural contributions to the entropies and heat capacities of hydration of over 120 ions and the viscosity B-coefficients of nearly 80 aqueous ions are tabulated and correlated. B-coefficients for many more ions are predicted from this relationship and from their dependence on ionic size and charge. The structural entropies determine a unique scale of water structure making and breaking by the ions. 相似文献
46.
A laboratory information management system (LIMS) can make a major contribution to the quality and therefore to the efficiency
and competitiveness of a laboratory. Since it can impact all aspects of a laboratory's organization it must be the key if
not the principal player of the laboratory's quality system. It should support the laboratory in establishing, maintaining
and applying quality procedures thereby enabling the laboratory to achieve its quality goals. As a tool, LIMS permits the
laboratory to input and use its own know-how and experience to optimize the total organization (internal and external) and
workflow of generated information. However, perceived "quality" in the context of an LIMS, can be viewed as being made up
of different facets such as the security, reliability and accessibility of information as well as its turn around time and
production cost. This paper reviews the role of a LIMS in the laboratory and the contribution that both system design and
functionality can have on "building quality ".
Received: 5 October 1998 · Accepted: 20 October 1998 相似文献
47.
Information content of data and variables and types of weighting in least-squares regression methods
Algorithms are given for evaluating the relative amount of useful information related to a particular parameter which is carried by individual data points and intervals of the variables. The algorithms provide an efficient means of using the information contained in a set of data. Applications to the optimization of weighting in regression methods are described. Several informational and combined informational-statistical types of weighting are studied as a means of improving the accuracy and precision of the parameters obtained by non-linear regression. 相似文献
48.
Martin Anderle Herwig Schweng Karl E. Kürten Karl W. Kratky 《Journal of statistical physics》1995,81(3-4):843-849
We present evidence that the performance of the traditional fully connected Hopfield model can be dramatically improved by carefully selecting an information-specific connectivity structure, while the synaptic weights of the selected connections are the same as in the Hopfield model. Starting from a completely disconnected network we let genuine Hebbian synaptic connections grow, one by one, until a desired degree of stability is achieved. Neural pathways are thus fixed notbefore, butduring the learning phase. 相似文献
49.
L. Montrucchio 《Journal of Optimization Theory and Applications》1994,80(3):385-406
We study the relationship between the dynamical complexity of optimal paths and the discount factor in general infinite-horizon discrete-time concave problems. Given a dynamic systemx
t+1=h(x
t
), defined on the state space, we find two discount factors 0 < * ** < 1 having the following properties. For any fixed discount factor 0 < < *, the dynamic system is the solution to some concave problem. For any discount factor ** < < 1, the dynamic system is not the solution to any strongly concave problem. We prove that the upper bound ** is a decreasing function of the topological entropy of the dynamic system. Different upper bounds are also discussed.This research was partially supported by MURST, National Group on Nonlinear dynamics in Economics and Social Sciences. The author would like to thank two anonymous referees for helpful comments and suggestions. 相似文献
50.
C. David Levermore 《Journal of statistical physics》1996,83(5-6):1021-1065
This paper presents a systematicnonperturbative derivation of a hierarchy of closed systems of moment equations corresponding to any classical kinetic theory. The first member of the hierarchy is the Euler system, which is based on Maxwellian velocity distributions, while the second member is based on nonisotropic Gaussian velocity distributions. The closure proceeds in two steps. The first ensures that every member of the hierarchy is hyperbolic, has an entropy, and formally recovers the Euler limit. The second involves modifying the collisional terms so that members of the hierarchy beyound the second also recover the correct Navier-Stokes behavior. This is achieved through the introduction of a generalization of the BGK collision operator. The simplest such system in three spatial dimensions is a 14-moment closure, which also recovers the behavior of the Grad 13-moment system when the velocity distributions lie near local Maxwellians. The closure procedure can be applied to a general class of kinetic theories. 相似文献