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

Soumendu Roy; Laura Gravener; Douglas Philp; Euan Robert Kay

doi:10.1002/anie.202217613

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 journal › Article › peer-review

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 language	English
Article number	e202217613
Number of pages	9
Journal	Angewandte Chemie International Edition
Volume	62
Issue number	22
Early online date	20 Apr 2023
DOIs	https://doi.org/10.1002/anie.202217613
Publication status	Published - 22 May 2023

Keywords

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

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10.1002/anie.202217613Licence: CC BY

Roy-2023-A-dissipative-reaction-network-AngewandteChemie-202217613-CCBY
Copyright © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Final published version, 1.61 MBLicence: CC BY

Hierarchical reaction networks: Hierarchical reaction networks: nanoscale amplification by molecular replication
Kay, E. R. (PI) & Philp, D. (CoI)
The Leverhulme Trust
1/09/20 → 26/05/24
Project: Standard

Data underpinning "A Dissipative Reaction Network Drives Transient Solid-Liquid and Liquid-Liquid Phase Cycling of Nanoparticles"
Roy, S. (Contributor), Gravener, L. (Contributor), Philp, D. (Contributor) & Kay, E. R. (Creator), University of St Andrews, 24 Mar 2023
DOI: 10.17630/2bb8f289-2a16-4940-9527-c71fbc21a394
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Cite this

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title = "A dissipative reaction network drives transient solid-liquid and liquid-liquid phase cycling of nanoparticles",

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.",

keywords = "Dissipative Reaction Networks, Dynamic Covalent Chemistry, Nanoparticles, Non-equilibrium Processes, Phase Transfer",

author = "Soumendu Roy and Laura Gravener and Douglas Philp and Kay, {Euan Robert}",

note = "Funding: Financial support for this work was provided by the University of St Andrews and EaStCHEM, and the Leverhulme Trust [Grant RPG-2019-155]. ",

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AU - Gravener, Laura

AU - Philp, Douglas

AU - Kay, Euan Robert

N1 - Funding: Financial support for this work was provided by the University of St Andrews and EaStCHEM, and the Leverhulme Trust [Grant RPG-2019-155].

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Y1 - 2023/5/22

N2 - 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.

AB - 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.

KW - Dissipative Reaction Networks

KW - Dynamic Covalent Chemistry

KW - Nanoparticles

KW - Non-equilibrium Processes

KW - Phase Transfer

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

Abstract

Keywords

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Hierarchical reaction networks: Hierarchical reaction networks: nanoscale amplification by molecular replication

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Data underpinning "A Dissipative Reaction Network Drives Transient Solid-Liquid and Liquid-Liquid Phase Cycling of Nanoparticles"

Cite this