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◆ Angewandte Chemie (International ed. in English)2026-08-23

Reaction-Transport Coupling Drives Spatiotemporal Organization in Fuel-Driven Supramolecular Polymerization.

Akta Singh, Nayana Mukherjee, Jagannath Mondal, Pushpita Ghosh

原始摘要(英文原文)· Original abstract
Chemically fueled supramolecular systems provide a versatile platform for generating nonequilibrium structures and dynamical instabilities, including chemical oscillations and traveling waves reminiscent of biological organization. However, a minimal mechanistic framework capable of capturing the emergence of such spatiotemporal order is still lacking. Here, we develop a minimal reaction-transport framework for fuel-driven supramolecular polymerization that couples activation-deactivation chemistry with cooperative assembly, fragmentation, and polymer length-dependent diffusion. The model captures autonomous oscillations arising through a Hopf bifurcation and demonstrates how temporal instabilities evolve into spatial self-organization upon inclusion of transport. We show that the nonlinear interplay between reaction kinetics and state-dependent mobility gives rise to traveling polymerization fronts, oscillatory wave dynamics, and complex spatiotemporal patterns. The propagating fronts exhibit near-ballistic dynamics, revealing a fundamentally nonequilibrium transport mechanism emerging from reactive feedback and dynamically evolving diffusivity. These findings establish a minimal physical framework connecting dissipative self-assembly, nonlinear transport, and active matter, while providing design principles for programmable supramolecular materials capable of autonomous spatiotemporal organization.
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Reaction-Transport Coupling Drives Spatiotemporal Organization in Fuel-Driven Supramolecular Polymerization. — 科研速览 Science Skim