Nonequilibrium Thermodynamics of Non-Ideal Reaction-Diffusion Systems: Implications for Active Self-Organization

Abstract

We develop a framework describing the dynamics and thermodynamics of open non-ideal reaction-diffusion systems, which embodies Flory-Huggins theories of mixtures and chemical reaction network theories. Our theory elucidates the mechanisms underpinning the emergence of self-organized dissipative structures in these systems. It evaluates the dissipation needed to sustain and control them, discriminating the contributions from each reaction and diffusion process with spatial resolution. It also reveals the role of the reaction network in powering and shaping these structures. We identify particular classes of networks in which diffusion processes always equilibrate within the structures, while dissipation occurs solely due to chemical reactions. The spatial configurations resulting from these processes can be derived by minimizing a kinetic potential, contrasting with the minimization of the thermodynamic free energy in passive systems. This framework opens the way to investigating the energetic cost of phenomena such as liquid-liquid phase separation, coacervation, and the formation of biomolecular condensates.

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