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Published on: May 5, 2022
Dynamic Fluorescence Visualization of Nonequilibrium Supramolecular Assembly Regulated by a Proton Reservoir
Qian Wang1, Hanren Xu1, Hongyu An1
1Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China.
Researchers developed novel fluorescent assemblies using amphiphiles and a programmable proton reservoir. This system mimics living cells by using a fuel cycle to control dynamic self-assembly and chemical reactions, offering real-time monitoring.
Area of Science:
- Supramolecular chemistry
- Biomimetic systems
- Materials science
Background:
- Living systems utilize energy input to maintain nonequilibrium states via supramolecular assemblies.
- Adenosine triphosphate (ATP) is a universal fuel regulating dynamic processes.
- Recreating this in artificial systems is difficult due to coupled fuel regulation and building-block structure.
Purpose of the Study:
- To develop amphiphile-based fluorescent assemblies regulated by a time-programmable proton reservoir.
- To decouple fuel-mediated regulation from building-block structure for independent control.
- To enable real-time monitoring of assembly dynamics and fuel consumption.
Main Methods:
- Utilized amphiphilic building blocks for stimulus-responsive assembly.
- Implemented a time-programmable proton reservoir with a fuel-consuming esterification-hydrolysis cycle.
- Tuned acid availability to control assembly dynamics and fluorescence output.
Main Results:
- Achieved tunable fluorescence color (blue to white) and quantum yields (1.7%-71.9%).
- Demonstrated control over assembly via programmed acid availability, with tunable masking and regeneration times.
- Successfully regulated nonequilibrium organization and enabled catalytic nucleophilic reactions.
Conclusions:
- The developed system decouples fuel consumption from building blocks, enabling independent control over dynamic assembly.
- The programmable proton reservoir provides a mechanism for time-controlled regulation of artificial nonequilibrium systems.
- The intrinsic optical signal allows real-time visualization of fuel consumption and assembly transformation.
