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  • Chemical Engineering  (6)
  • 1
    Electronic Resource
    Electronic Resource
    Stamford, Conn. [u.a.] : Wiley-Blackwell
    Polymer Engineering and Science 32 (1992), S. 1654-1664 
    ISSN: 0032-3888
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: We review briefly the general assumptions underlying hole theories of the configurational thermodynamic functions for single and multiconstituent systems. From the original Simha-Somcynsky theory several important modifications have recently evolved. First, there is a revision of the combinatorial entropy originating from the mixing of segments and holes in the spirit of Huggins's theory. With consistent additional modifications of the configurational free energy, quantitatively significant consequences for certain aspects of phase equilibria can arise. Finally, allowance for nonrandom mixing of constituents species and holes has been made. We illustrate the theory's potentials first in terms of pressure-volume-temperature (PVT) data for high and low molar mass species and their miscible mixtures. The influence of PVT properties on the miscibility behavior of solutions and blends is examined next. Of particular concern are the connections between predictability of lower from upper mixing spinodals, pressure effects, and the binary interaction χ-function.
    Additional Material: 11 Ill.
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  • 2
    Electronic Resource
    Electronic Resource
    Stamford, Conn. [u.a.] : Wiley-Blackwell
    Polymer Engineering and Science 19 (1979), S. 845-848 
    ISSN: 0032-3888
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Recent equation of state data are analyzed in terms of the hole theory of polymer melts. The good agreement between experimental and theoretical volume-temperature curves at atmospheric pressure, observed previously for a number of amorphous and crystallizable polymers, is again confirmed. Similarly, satisfactory theoretical results for the isotherms ensue, with deviations however becoming noticeable at elevated pressures and low temperatures. The linearity of the isochores observed experimentally is confirmed by the theory, however with somewhat different slopes. Departures of maximally 10 percent from the thermal pressure coefficients derived from the experimental PVT data are noted. Significant differences between theory and experiment apper only in the third derivatives of the partition function, as has also been observed with other pollymers. The characteristic scaling parameters of volume, temperature and pressure show the expected similarity with hevea rubber. Earlier correlations for scaling entropy and segmental volume with scaling temperature are found to be valid within the scatter of these relations. Finally, the applicability of the empirical Tait equation in the form applied to the equation of state in other polymer melts is confirmed. Although the resulting thermal pressure coefficient exhibits an explicit even if smal dependence on temperature, in disagreement with experiment or theory, the Tait equation remains a useful relation for the representation of PVT information.
    Additional Material: 4 Ill.
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  • 3
    Electronic Resource
    Electronic Resource
    Stamford, Conn. [u.a.] : Wiley-Blackwell
    Polymer Engineering and Science 24 (1984), S. 1284-1290 
    ISSN: 0032-3888
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: We discuss the free-energy expressions for homogeneous melts and their blends, based on our hole theory. Equation of state (PVT) and free energy of mixing (ΔGm) are considered from a common point of view without the introduction of additional parameters to pass from the first to the second set of properties. Practical problems arise from the fact that ΔGm represents a difference between large quantities. As illustrations we analyze two typical systems. One is the n - C6 + n - C16 pair where PVT and ΔGm, the latter at atmospheric pressure only, have been studied experimentally. The other is n - C6 with a low and high molecular weight respectively of polyethylene as solute. Here the PVT relations of the components only are known. The effects of intercomponent attractions, temperature, pressure, and molecular weight on phase behavior are investigated. Critical coordinates, lower critical-solution temperatures (LCST) and their pressure dependence are computed. An iso-free volume condition obtains for this dependence where free volume is defined by the hole fraction inherent in the theory. Comparisons with experimental observations and other theoretical computations for different molecular weights are limited by the effect of polydispersity. Moreover, cloud point curves are shown. We finally compute the composition and pressure dependence of the χ-parameter which is implicit in the theory. We conclude with some comments regarding polymer blends.
    Additional Material: 6 Ill.
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  • 4
    Electronic Resource
    Electronic Resource
    Stamford, Conn. [u.a.] : Wiley-Blackwell
    Polymer Engineering and Science 24 (1984), S. 1071-1078 
    ISSN: 0032-3888
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: We review first recent results concerning the relation between the relaxation of extensive thermodynamic and of viscoelastic functions. In the underlying theory a central role is assigned to a particular excess-free volume function h. It was originally introduced in a theory of the equilibrium melt. The time dependence of h can then be derived from volume (or enthalpy) recovery data and serves to predict other quantities, such as mean-square density fluctuations and viscoelastic-temperature shift factors during the aging process. Next the physical basis and results of two kinetic theories of volume relaxation are summarized. In both approaches the h-function is employed as an expression of the molecular dynamics in the drive to equilibrium. The first describes a gradual elimination of free-volume gradients through a diffusion process, characterized by a diffusion parameter, varying with the local free volume in accord with a Doolittle relation. The second, a stochastic theory, derives expressions for the matrix of transition rates between different free-volume states, the resulting spectrum of retardation times, and the size distribution of free volume in the relaxing system. Satisfactory agreement between observed and predicted volume recovery of poly(vinyl acetate) ensues. In the limit of an infinitesimal temperature jump, both theories yield a Williams-Watts correlation function as an approximate interpolation expression. The exponent β, however, varies in time with a constant value of approximately 0.60 over a limited time interval.
    Additional Material: 11 Ill.
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  • 5
    Electronic Resource
    Electronic Resource
    Stamford, Conn. [u.a.] : Wiley-Blackwell
    Polymer Engineering and Science 20 (1980), S. 82-86 
    ISSN: 0032-3888
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: The PVT properties of polymer glasses are discussed from two points of view. First, as a low frequency tool in the study of sub-glass relaxations. Dilatometric results illustrate the sensitivity of the thermal expansivity and its temperature coefficient to dynamic processes occuring in the glass. The second point of view considers the quasi-thermodynamics of the non-equilibrium system, under conditions where the rates of relaxational processes are small in comparison with experimental rates, and time dependent processes are practically absent. The starting point is a theory of the equilibrium melt which describes the characteristic liquid disorder in terms of a temperature and pressure dependent hole or loosely, free volume fraction. This function is obtained by the minimization of a configurational free energy. Upon reaching the glass transition, this dependence is reduced, and further so in a sub-glass relaxation region. However, it is not eliminated until temperatures of the order of 50 to 70 K are reached. While this picture is qualitatively universal, significant quantitative differences are observed with different chemical structures and different thermal and pressure histories. A comparison of thermal expansivities of high and low Tg systems indicates that in the former the free volume retained upon reaching Tg is comparatively large and the departure from equilibrium or degree of freeze-in comparatively small. Similarly, it appears that the glassy densification generated by cooling the melt under pressure is more extensive in high Tg glasses. Such results imply structural differences. These should be investigated by comparative studies of (a) time dependent processes in terms of the free volume functions, (b) sorption and transport, and (c) the temperature dependent dynamics of density fluctuations.
    Additional Material: 7 Ill.
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  • 6
    Electronic Resource
    Electronic Resource
    Brookfield, Conn. : Wiley-Blackwell
    Polymer Composites 5 (1984), S. 3-10 
    ISSN: 0272-8397
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Physical properties of composites as a function of filler content have been described in the past through models requiring the solution of macroscopic equations of motion for an elastic continuum or, on a more empirical level, by the assumption of various compositional averaging schemes. We discuss a model drawn from our molecular mixture theory. This allows us to avoid the formal problems attending concentrated suspensions and introduces molecular filler-medium interaction parameters. Comparisons with experimental material and empirical equations involving bulk modulus and thermal expansivity will be given. The theory opens the possibility of determining interfacial strengths from appropriate mechanical and thermal measurements and of predicting one set from another set of data.
    Additional Material: 8 Ill.
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