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Solid-phase reaction kinetics

Meaningful kinetic constants vs. formal parameters

Journal of Thermal Analysis and Calorimetry
Author: A. Korobov

Abstract  

It is argued that, for the macroscopic parameters of conventional kinetic models to become meaningful, they may be and must be expressed in terms of elementary single-barrier processes. To accomplish this means to associate some (external) extensional measure with a single-barrier elementary act, remaining within the logic of the existing geometrical-probabilistic scheme. A manner of doing this involving the use of Dirichlet fragmentations is suggested.

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The convexity of localization forms, strictly required by conventional geometric-probabilistic formalism, is not in agreement with many experimental observations concerning solid-phase chemical reactions. In a discussion of the essence of this requirement, it is shown that it may be weakened for non-convex localization forms consistent with the symmetry of a solid reagent and described within the geometric-probabilistic approach in terms of planigons and Wigner-Seitz cells.

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A self-consistent mathematical model is proposed to describe the heat evolution during the hydration of inorganic binders. Such an approach reflects the sufficient role of the feedbacks in the systems under discussion. The principal physico-chemical reasons for the self-consistent description of the hydration kinetics are argued. To complete the phenomenology of the hydration of binders two more problems are solved: (i) quantitative determination of the characteristic periods of the hydration process, and (ii) the long-range forecast of integral heat evolution.

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