Optimizing reaction and transport fluxes in temperature gradient-driven chemical reaction-diffusion systems

TL;DR

This paper develops a theoretical framework for temperature gradient-driven chemical reaction-diffusion systems, enabling optimization and control of nonequilibrium fluxes for applications like energy harvesting and targeted chemical processes.

Contribution

It introduces a comprehensive theoretical model for 1D chemical systems under temperature gradients, including an exact solution for a two-compartment model and numerical generalizations.

Findings

Temperature gradients induce steady chemical fluxes analogous to electric circuits.

System symmetry and temperature profile shape control reaction and transport localization.

Entropy production rate quantifies system activity and dissipation.

Abstract

Temperature gradients represent energy sources that can be harvested to generate steady reaction or transport fluxes. Technological developments could lead to the transfer of free energy from heat sources and sinks to chemical systems for the purpose of extraction, thermal batteries, or nonequilibrium synthesis. We present a theoretical study of 1D chemical systems subjected to temperature gradients, for sustaining nonequilibrium chemical fluxes. A complete theoretical framework describes the behavior of the system induced by various temperature profiles. An exact mathematical derivation was established for a simple two-compartment model and was generalized to arbitrary reaction-diffusion systems based on numerical models. An experimental system was eventually scaled and tuned to optimize either nonequilibrium chemical transport or reaction. The relevant parameters for this description were identified; they focused on the system symmetry for chemical reaction and transport. Nonequilibrium thermodynamic approaches lead to a description analogous to electric circuits. Temperature gradients lead to the onset of a steady chemical force, which maintains steady reaction-diffusion fluxes moderated by chemical resistance. The system activity was then assessed using the entropy production rate as a measure of its dissipated power. The chemical characteristics of the system can be tuned for general optimization of the nonequilibrium state or for the specific optimization of either transport or reaction processes. The shape of the temperature gradient can be tailored to precisely control the spatial localization of active processes, targeting either precise spatial localization or propagation over large areas. The resulting temperature-driven chemical system can in turn be used to drive secondary processes into either nonequilibrium reaction fluxes or concentration gradients.