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Temporally programmed polymer – solvent interactions using a chemical reaction network

Author

Listed:
  • Benjamin Klemm

    (Delft University of Technology)

  • Reece W. Lewis

    (Delft University of Technology)

  • Irene Piergentili

    (Delft University of Technology)

  • Rienk Eelkema

    (Delft University of Technology)

Abstract

Out of equilibrium operation of chemical reaction networks (CRNs) enables artificial materials to autonomously respond to their environment by activation and deactivation of intermolecular interactions. Generally, their activation can be driven by various chemical conversions, yet their deactivation to non-interacting building blocks remains largely limited to hydrolysis and internal pH change. To achieve control over deactivation, we present a new, modular CRN that enables reversible formation of positive charges on a tertiary amine substrate, which are removed using nucleophilic signals that control the deactivation kinetics. The modular nature of the CRN enables incorporation in diverse polymer materials, leading to a temporally programmed transition from collapsed and hydrophobic to solvated, hydrophilic polymer chains by controlling polymer-solvent interactions. Depending on the layout of the CRN, we can create stimuli-responsive or autonomously responding materials. This concept will not only offer new opportunities in molecular cargo delivery but also pave the way for next-generation interactive materials.

Suggested Citation

  • Benjamin Klemm & Reece W. Lewis & Irene Piergentili & Rienk Eelkema, 2022. "Temporally programmed polymer – solvent interactions using a chemical reaction network," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33810-y
    DOI: 10.1038/s41467-022-33810-y
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    References listed on IDEAS

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    1. Sarah M. Morrow & Ignacio Colomer & Stephen P. Fletcher, 2019. "A chemically fuelled self-replicator," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    2. Ignacio Colomer & Sarah M. Morrow & Stephen P. Fletcher, 2018. "A transient self-assembling self-replicator," Nature Communications, Nature, vol. 9(1), pages 1-6, December.
    3. Marta Tena-Solsona & Benedikt Rieß & Raphael K. Grötsch & Franziska C. Löhrer & Caren Wanzke & Benjamin Käsdorf & Andreas R. Bausch & Peter Müller-Buschbaum & Oliver Lieleg & Job Boekhoven, 2017. "Non-equilibrium dissipative supramolecular materials with a tunable lifetime," Nature Communications, Nature, vol. 8(1), pages 1-8, August.
    4. Diederik W. R. Balkenende & Christophe A. Monnier & Gina L. Fiore & Christoph Weder, 2016. "Optically responsive supramolecular polymer glasses," Nature Communications, Nature, vol. 7(1), pages 1-9, April.
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    Cited by:

    1. Natsumi Nishiie & Ryo Kawatani & Sae Tezuka & Miu Mizuma & Mikihiro Hayashi & Yasuhiro Kohsaka, 2024. "Vitrimer-like elastomers with rapid stress-relaxation by high-speed carboxy exchange through conjugate substitution reaction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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