Entropic analysis of bistability and the general evolution criterion

Area of Science:

• Non-equilibrium thermodynamics
• Chemical kinetics
• Theoretical chemistry

Background:

• The Schlögl model is a fundamental system for studying chemical bi-stability and non-equilibrium phenomena.
• Understanding entropy production and exchange is crucial for characterizing the behavior of open systems far from equilibrium.
• The general evolution criterion (GEC) provides a theoretical framework for analyzing temporal changes in entropy production.

Purpose of the Study:

• To conduct a detailed study of entropy production, exchange, and balance in both clamped and open-flow versions of the Schlögl model.
• To validate the general evolution criterion (GEC) for transitions between unstable and stable non-equilibrium stationary states.
• To investigate the distribution of entropy production and exchange over elementary flux modes using stoichiometric network analysis (SNA).

Main Methods:

• Application of the general evolution criterion (GEC) to analyze entropy dynamics.
• Utilizing stoichiometric network analysis (SNA) to dissect entropy production and exchange.
• Comparison of clamped and volumetric open-flow Schlögl models.

Main Results:

• The general evolution criterion (GEC) was successfully validated for transitions to stable non-equilibrium stationary states.
• No evidence was found to support a principle of maximum entropy production.
• SNA provided insights into the distribution of entropy production and exchange across elementary flux modes.

Conclusions:

• The GEC is confirmed as the governing theorem for entropy production in non-equilibrium systems.
• The study challenges the notion of a maximum entropy production principle.
• SNA effectively elucidates the mechanisms of dissipation and entropy exchange in complex chemical systems.