Stepwise Unfolding of Single-Chain Nanoparticles by Chemically Triggered Gates

Tobias S. Fischer; David Schulze-Sünninghausen; Burkhard Luy; Ozcan Altintas; Christopher Barner-Kowollik

doi:10.1002/anie.201602894

Stepwise Unfolding of Single-Chain Nanoparticles by Chemically Triggered Gates

Tobias S. Fischer, David Schulze-Sünninghausen, Burkhard Luy, Ozcan Altintas, Christopher Barner-Kowollik

Chemistry (Twin Cities)

Research output: Contribution to journal › Article › peer-review

64 Scopus citations

Abstract

The orthogonal, stepwise, and order-independent unfolding of single-chain nanoparticles (SCNPs) is introduced as a key step towards actively controlling the folding dynamics of SCNPs. The SCNPs are compacted by multiple hydrogen bonds and host–guest interactions. Well-defined diblock (AB) and tetrablock (ABCD) copolymers are equipped with orthogonal recognition motifs via modular ligation along the lateral chain. Initially, single-chain folding of the diblock copolymer was induced by the host–guest complexation of benzo-21-crown-7 (B21C7, host) and a secondary ammonium salt (AS, guest), representing an efficient avenue for single-chain collapse. Next, both orthogonal Hamilton wedge (HW) and cyanuric acid (CA) as well as B21C7–AS motifs were employed to generate SCNPs based on the ABCD polymer system. Subsequently, the stepwise dual-gated and order-independent unfolding of the SCNPs was investigated by the addition of external stimuli. The folding and unfolding were explored by 1D¹H NMR spectroscopy, dynamic light scattering (DLS), and diffusion-ordered NMR spectroscopy (DOSY).

Original language	English (US)
Pages (from-to)	11276-11280
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	55
Issue number	37
DOIs	https://doi.org/10.1002/anie.201602894
State	Published - Sep 5 2016

Bibliographical note

Funding Information:
C.B.-K. and B.L. acknowledge funding for this project by the Sonderforschungsbereich 1176, project A1, of the German Research Council (DFG). C.B.-K. and B.L. also acknowledge long-term funding by the Helmholtz Association in the context of the Biointerfaces in Technology and Medicine (BIFTM) program. NMR measurements were performed in the DFG instrumentation facility Pro

Publisher Copyright:
© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

host–guest interactions
orthogonal unfolding
polymer synthesis
single-chain folding
supramolecular chemistry

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10.1002/anie.201602894

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abstract = "The orthogonal, stepwise, and order-independent unfolding of single-chain nanoparticles (SCNPs) is introduced as a key step towards actively controlling the folding dynamics of SCNPs. The SCNPs are compacted by multiple hydrogen bonds and host–guest interactions. Well-defined diblock (AB) and tetrablock (ABCD) copolymers are equipped with orthogonal recognition motifs via modular ligation along the lateral chain. Initially, single-chain folding of the diblock copolymer was induced by the host–guest complexation of benzo-21-crown-7 (B21C7, host) and a secondary ammonium salt (AS, guest), representing an efficient avenue for single-chain collapse. Next, both orthogonal Hamilton wedge (HW) and cyanuric acid (CA) as well as B21C7–AS motifs were employed to generate SCNPs based on the ABCD polymer system. Subsequently, the stepwise dual-gated and order-independent unfolding of the SCNPs was investigated by the addition of external stimuli. The folding and unfolding were explored by 1D1H NMR spectroscopy, dynamic light scattering (DLS), and diffusion-ordered NMR spectroscopy (DOSY).",

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Stepwise Unfolding of Single-Chain Nanoparticles by Chemically Triggered Gates

Abstract

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