TY - JOUR
T1 - Stepwise Unfolding of Single-Chain Nanoparticles by Chemically Triggered Gates
AU - Fischer, Tobias S.
AU - Schulze-Sünninghausen, David
AU - Luy, Burkhard
AU - Altintas, Ozcan
AU - Barner-Kowollik, Christopher
N1 - Publisher Copyright:
© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2016/9/5
Y1 - 2016/9/5
N2 - 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).
AB - 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).
KW - host–guest interactions
KW - orthogonal unfolding
KW - polymer synthesis
KW - single-chain folding
KW - supramolecular chemistry
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U2 - 10.1002/anie.201602894
DO - 10.1002/anie.201602894
M3 - Article
C2 - 27357944
AN - SCOPUS:84976902134
SN - 1433-7851
VL - 55
SP - 11276
EP - 11280
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 37
ER -