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arXiv · 1412.6234

A general theory of kinetics and thermodynamics of steady-state copolymerization

Yao-Gen Shu·Yong-Shun Song·Zhong-Cun Ou-Yang·Ming Li
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Abstract

Kinetics of steady-state copolymerization has been investigated since 1940s. Irreversible terminal and penultimate models were successfully applied to a number of comonomer systems, but failed for systems where depropagation is significant. Although a general mathematical treatment of the terminal model with depropagation was established in 1980s, penultimate model and higher-order terminal models with depropagation have not been systematically studied, since depropagation leads to hierarchically-coupled and unclosed kinetic equations which are hard to be solved analytically. In this work, we propose a truncation method to solve the steady-state kinetic equations of any-order terminal models with depropagation in an unified way, by reducing them into closed steady-state equations which give the exact solution of the original kinetic equations. Based on the steady-state equations, we also derive a general thermodynamic equality in which the Shannon entropy of the copolymer sequence is explicitly introduced as part of the free energy dissipation of the whole copolymerization system.

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Yao-Gen Shu, Yong-Shun Song, Zhong-Cun Ou-Yang, Ming Li. 2014-12-19. A general theory of kinetics and thermodynamics of steady-state copolymerization. https://doi.org/10.1088/0953-8984%2F27%2F23%2F235105

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