Light-triggered unfolding of single linear molecular bottlebrushes from compact globular to wormlike nano-objects in water

Henn, Daniel M.; Lau, C. Maggie; Zhao, Bin

doi:10.1039/c7py00279c

Cited by 32 publications

(34 citation statements)

References 58 publications

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“…Both morphologies have been reported previously for bottlebrush polymers depending on the grafting density, side‐chain length and other factors. [ 108,109 ] For bottlebrush samples B1‐ g ‐12700 and B1‐ g ‐17500, globular morphologies are observed with average size of ~300–400 nm, indicating successful achievement of bottlebrush structures.…”

Section: Resultsmentioning

confidence: 99%

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Qiang

Chen

et al. 2020

Journal of Polymer Science

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Thermo-cleavable bottlebrush polymers were synthesized by a facile grafting-to method via radical coupling and atom transfer radical polymerization (ATRP) without small-molecule synthesis involved. Bottlebrushes were achieved by coupling backbones of poly(4-methacryloyloxy-2,2,6,6-tetramethylpiperidine-1-oxyl), which contain nitroxide radicals, and ATRP-synthesized side chains, which can be halogen-abstracted to generate carbon-centered radicals. Bottlebrushes were prepared using homopolymer or block copolymer side chains. Alkoxyamine covalent bonds resulting from radical coupling are thermo-reversible at high temperature, and grafting density may be tuned by annealing of post-synthesis bottlebrush, with the bottlebrush regime going from loose bottlebrush to dense comb and loose comb. The effects of confinement on the T g and fragility of films of polystyrene bottlebrush were studied by ellipsometry; comparisons were made to thermally cleaved linear components obtained directly after annealing. Relative to linear polymer, bottlebrush topology reduces bulk fragility and suppresses T g-and fragility-confinement effects. The correlation between the strengths of the confinement effects is consistent with other film studies of linear and nonlinear polymers and supports the notion that fragility is a fundamental property underlying perturbations to T g. Besides providing a platform for advancing fundamental scientific understanding, our synthetic strategy may afford novel applications of bottlebrushes via incorporated dynamic chemistry.

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Section: Resultsmentioning

confidence: 99%

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Qiang

Chen

et al. 2020

Journal of Polymer Science

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“…The PEO mBBs used in this study were synthesized by a grafting-to method, where alkyne end-functionalized PEO was grafted onto an azidebearing backbone polymer using the highly efficient copper(I)catalyzed azide-alkyne cycloaddition click reaction (Supplementary Fig. 1) 21,[28][29][30][31] . Detailed synthesis and characterization of mBBs are summarized in the supporting information (SI, Supplementary Figs.…”

Section: Resultsmentioning

confidence: 99%

Breaking translational symmetry via polymer chain overcrowding in molecular bottlebrush crystallization

Liu

Henn

et al. 2020

Nat Commun

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One of the fundamental laws in crystallization is translational symmetry, which accounts for the profound shapes observed in natural mineral crystals and snowflakes. Herein, we report on the spontaneous formation of spherical hollow crystals with broken translational symmetry in crystalline molecular bottlebrush (mBB) polymers. The unique structure is named as mBB crystalsome (mBBC), highlighting its similarity to the classical molecular vesicles. Fluorescence resonance energy transfer (FRET) experiments show that the mBBC formation is driven by local chain overcrowding-induced asymmetric lamella bending, which is further confirmed by correlating crystalsome size with crystallization temperature and mBBʼs side chain grafting density. Our study unravels a new principle of spontaneous translational symmetry breaking, providing a general route towards designing versatile nanostructures.

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“…O-nitrobenzyl group is stable in an acidic and alkaline environment and has highly controllable photochemical properties [ 96 , 97 ]. Li et al synthesized a diblock copolymer PEG-b-poly (n-(s- (o-nitrobenzyl)-thioethyl) glycine) (PEG-b-PNSN) by ring-opening polymerization.…”

Section: Stimuli-responsive Polypeptoidmentioning

confidence: 99%

Stimulus-Responsive Polymers Based on Polypeptoid Skeletons

Fang

Wei

et al. 2021

Polymers

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Polypeptoids have attracted a lot of atteSDntion because of their unique structural characteristics and special properties. Polypeptoids have the same main chain structures to polypeptides, making them have low cytotoxicity and excellent biocompatibility. Polypeptoids can also respond to external environmental changes by modifying the configurations of the side chains. The external stimuli can be heat, pH, ions, ultraviolet/visible light and active oxygen or their combinations. This review paper discussed the recent research progress in the field of stimulus-responsive polypeptoids, including the design of new stimulus-responsive polypeptoid structures, controlled actuation factors in response to external stimuli and the application of responsive polypeptoid biomaterials in various biomedical and biological nanotechnology, such as drug delivery, tissue engineering and biosensing.

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Light-triggered unfolding of single linear molecular bottlebrushes from compact globular to wormlike nano-objects in water

Abstract: The photocleavage of o-nitrobenzyl moieties drives shape transitions from globular to wormlike in stimuli-responsive homografted and binary heterografted molecular bottlebrushes.

Cited by 32 publications

References 58 publications

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Breaking translational symmetry via polymer chain overcrowding in molecular bottlebrush crystallization

Stimulus-Responsive Polymers Based on Polypeptoid Skeletons

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Light-triggered unfolding of single linear molecular bottlebrushes from compact globular to wormlike nano-objects in water

Abstract: The photocleavage of o-nitrobenzyl moieties drives shape transitions from globular to wormlike in stimuli-responsive homografted and binary heterografted molecular bottlebrushes.

Cited by 32 publications

References 58 publications

Impact of bottlebrush chain architecture on Tg‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Impact of bottlebrush chain architecture on Tg‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Breaking translational symmetry via polymer chain overcrowding in molecular bottlebrush crystallization

Stimulus-Responsive Polymers Based on Polypeptoid Skeletons

Contact Info

Product

Resources

About

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization

Impact of bottlebrush chain architecture on T_g‐confinement and fragility‐confinement effects enabled by thermo‐cleavable bottlebrush polymers synthesized by radical coupling and atom transfer radical polymerization