A dissipative reaction network drives transient solid-liquid and liquid-liquid phase cycling of nanoparticles

Soumendu Roy, Laura Gravener, Douglas Philp*, Euan Robert Kay*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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Abstract

Transient states maintained by energy dissipation are an essential feature of dynamic systems where structures and functions are regulated by fluxes of energy and matter through chemical reaction networks. Perfected in biology, chemically fueled dissipative networks incorporating nanoscale components allow the unique properties of nanomaterials to be bestowed with spatiotemporal adaptability and chemical responsiveness. We report the transient dispersion of gold nanoparticles in water, powered by dissipation of a chemical fuel. A dispersed state that is generated under nonequilibrium conditions permits fully reversible solid–liquid or liquid–liquid phase transfer. The molecular basis of the out-of-equilibrium process is reversible covalent modification of nanoparticle-bound ligands by a simple inorganic activator. Activator consumption by a coupled dissipative reaction network leads to autonomous cycling between phases. The out-of-equilibrium lifetime is tunable by adjusting pH, and reversible phase cycling is reproducible over several cycles.
Original languageEnglish
Article numbere202217613
Number of pages9
JournalAngewandte Chemie International Edition
Volume62
Issue number22
Early online date20 Apr 2023
DOIs
Publication statusPublished - 22 May 2023

Keywords

  • Dissipative Reaction Networks
  • Dynamic Covalent Chemistry
  • Nanoparticles
  • Non-equilibrium Processes
  • Phase Transfer

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