Organocatalytic Control over a Fuel-Driven Transient-Esterification Network
M.P. van der Helm (TU Delft - ChemE/Advanced Soft Matter)
Chang Lin Wang (Student TU Delft)
B. Fan (TU Delft - ChemE/Advanced Soft Matter)
M. Macchione (TU Delft - ChemE/Advanced Soft Matter)
E. Mendes (TU Delft - ChemE/Advanced Soft Matter)
R Eelkema (TU Delft - ChemE/Advanced Soft Matter)
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Abstract
Signal transduction in living systems is the conversion of information into a chemical change, and is the principal process by which cells communicate. In nature, these functions are encoded in non-equilibrium (bio)chemical reaction networks (CRNs) controlled by enzymes. However, man-made catalytically controlled networks are rare. We incorporated catalysis into an artificial fuel-driven out-of-equilibrium CRN, where the forward (ester formation) and backward (ester hydrolysis) reactions are controlled by varying the ratio of two organocatalysts: pyridine and imidazole. This catalytic regulation enables full control over ester yield and lifetime. This fuel-driven strategy was expanded to a responsive polymer system, where transient polymer conformation and aggregation are controlled through fuel and catalyst levels. Altogether, we show that organocatalysis can be used to control a man-made fuel-driven system and induce a change in a macromolecular superstructure, as in natural non-equilibrium systems.
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