Abstract
Chemical processes in closed systems inevitably relax to equilibrium. Living systems avoid this fate and give rise to a much richer diversity of phenomena by operating under nonequilibrium conditions. Recent experiments in dissipative self-assembly also demonstrated that by opening reaction vessels and steering certain concentrations, an ocean of opportunities for artificial synthesis and energy storage emerges. To navigate it, thermodynamic notions of energy, work and dissipation must be established for these open chemical systems. Here, we do so by building upon recent theoretical advances in nonequilibrium statistical physics. As a central outcome, we show how to quantify the efficiency of such chemical operations and lay the foundation for performance analysis of any dissipative chemical process.
Highlights
Chemical processes in closed systems inevitably relax to equilibrium
We provide one grounded in the recently established nonequilibrium thermodynamics of CRN7,8, which was born from the combination of state-of-the-art statistical mechanics[9,10,11,12,13,14] and mathematical chemical reaction networks (CRN) theory[15,16]
An open CRN initially at equilibrium with high concentrations of low-energy molecules and low concentrations of high-energy ones is brought out of equilibrium with the aim to increase the concentrations of the high-energy species
Summary
Chemical processes in closed systems inevitably relax to equilibrium. Living systems avoid this fate and give rise to a much richer diversity of phenomena by operating under nonequilibrium conditions. The first thermodynamic description of nonequilibrium chemical processes was achieved by the Brussels school founded by de Donder and perpetuated by Prigogine[1,2], but they focused on few reactions close to equilibrium in the so-called linear regime. Processes such as fuel-driven self-assembly involve open chemical reaction networks (CRN) with many reactions operating far away from equilibrium[3,4].
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