Dynamic Fluorescence Visualization of Nonequilibrium Supramolecular Assembly Regulated by a Proton Reservoir
Abstract
ABSTRACT Living systems sustain nonequilibrium supramolecular assemblies through continuous energy input and concomitant dissipation, with adenosine triphosphate (ATP) serving as a universal chemical fuel that regulates dynamic processes by coupling hydrolysis to downstream chemical or conformational changes. Biomimetic recreation of this behavior remains challenging because fuel‐mediated regulation in artificial assemblies is typically coupled to building‐block structure, limiting independent control over assembly dynamics and real‐time monitoring. Here we report amphiphile‐based fluorescent assemblies regulated by a time‐programmable proton reservoir, where the fuel‐consuming esterification–hydrolysis cycle is decoupled from the building blocks and controls assembly through programmed acid availability. The amphiphilic building blocks undergo stimulus–responsive assembly with fluorescence color tunable from blue to green, yellow, and white, and quantum yields spanning 1.7%–71.9%. The proton reservoir temporarily holds acid in hydrolysable esterified forms and subsequently regenerates acid over prescribed timescales; by molecular design, the acid‐masking period is tuned from 0 to 250 min and acid regeneration from 10 to 120 min. Coupling this cycle to the fluorescent assembly regulates nonequilibrium organization, enables catalytic nucleophilic reactions, and provides an intrinsic optical signal for visualizing fuel consumption and assembly transformation in real time.
Article Details
Authors (7)
Qian Wang
Hanren Xu
Key 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
Hongyu An
Jianfeng Jiang
Boyi Fu
Precise Synthesis and Function Development Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering China West Normal University Nanchong Sichuan China
He Tian
Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou, China.
Da‐Hui Qu
Key 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