Harnessing autocatalytic reactions in polymerization and depolymerization

Autocatalysis and its relevance to various polymeric systems are discussed by taking inspiration from biology. A number of research directions related to synthesis, characterization, and multi-scale modeling are discussed in order to harness autocatalytic reactions in a useful manner for different applications ranging from chemical upcycling of polymers (depolymerization and reconstruction after depolymerization), self-generating micelles and vesicles, and polymer membranes. Overall, a concerted effort involving in situ experiments, multi-scale modeling, and machine learning algorithms is proposed to understand the mechanisms of physical and chemical autocatalysis. It is argued that a control of the autocatalytic behavior in polymeric systems can revolutionize areas such as kinetic control of the self-assembly of polymeric materials, synthesis of self-healing and self-immolative polymers, as next generation of materials for a sustainable circular economy. Graphic Abstract

Non-Equilibrium Thermodynamics View on Kinetics of Autocatalytic Reactions—Two Illustrative Examples

Autocatalytic reactions are in certain contrast with the linear algebra of reaction stoichiometry, on which rate equations respecting the permanence of atoms are constructed. These mathematical models of chemical reactions are called conservative. Using a non-equilibrium thermodynamics-based theory of chemical kinetics, it is shown how to introduce autocatalytic step into such (conservative) rate equation properly. Further, rate equations based on chemical potentials or affinities are derived, and conditions for the consistency of rate equations with the entropic inequality (the second law of thermodynamics) are illustrated. The theory illustrated here can be viewed as a tool for verifying and generalizing traditional mass-action kinetics by means of modern non-equilibrium thermodynamics, which is able to deal also with such rather problematic cases.

Leveraging autocatalytic reactions for chemical domain image classification

Kinetic models of autocatalytic reactions have mathematical forms similar to activation functions used in artificial neural networks. Inspired by these similarities, we use a copper-catalyzed reaction to perform digital image recognition tasks.

A Non-Equilibrium Thermodynamics-Based View of the Kinetics of Autocatalytic Reactions – a Simple Illustrative Example

Autocatalytic reactions are in a certain contrast with the linear algebra of reaction stoichiometry, on whose basis rate equations respecting the permanence of atoms are constructed. These mathematical models of chemical reactions are termed conservative.Using a non-equilibrium thermodynamics-based theory of chemical kinetics, this paper demonstrates how to properly introduce an autocatalytic step into a (conservative) rate equation. Further, rate equations based on chemical potentials or affinities are derived, and conditions for the consistency of rate equations with entropic inequality (the second law of thermodynamics) are illustrated.<br><div><br></div>

A Non-Equilibrium Thermodynamics-Based View of the Kinetics of Autocatalytic Reactions – a Simple Illustrative Example

Autocatalytic reactions are in a certain contrast with the linear algebra of reaction stoichiometry, on whose basis rate equations respecting the permanence of atoms are constructed. These mathematical models of chemical reactions are termed conservative.Using a non-equilibrium thermodynamics-based theory of chemical kinetics, this paper demonstrates how to properly introduce an autocatalytic step into a (conservative) rate equation. Further, rate equations based on chemical potentials or affinities are derived, and conditions for the consistency of rate equations with entropic inequality (the second law of thermodynamics) are illustrated.<br><div><br></div>

Rapid and colorimetric detection of nucleic acids based on entropy-driven circuit and DNAzyme-mediated autocatalytic reactions

In this work, a novel, rapid and enzyme-free colorimetric biosensor for the detection of nucleic acids has been developed based on entropy-driven (EDC) circuit and DNAzyme-mediated autocatalytic reactions.