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Title: Dynamic and programmable morphology and size evolution via a living hierarchical self-assembly strategy

Abstract

Recent advances in the preparation of shape-shifting and size-growing nanostructures are hot topics in development of nanoscience, because many intelligent functions are always relied on their shape and dimension. Here we report a tunable manipulation of sequential self-assembled transformation in situ via a hierarchical assembly strategy based on a living thiol–disulfide exchange reaction. By tailoring the external stimuli, the reactive points can be generated at the ends of initially unimolecular micelles, which subsequently drive the pre-assemblies to periodically proceed into the hierarchically micellar connection, axial growth, bending, and cyclization processes from nanoscopic assemblies to macroscopic particles. Of particular interest would be systems that acquired the shape control and size adjustment of self-assemblies after termination or reactivation of disulfide reshuffling reaction by regulating external stimuli whenever needed. Such a hierarchical strategy for self-assembled evolution is universally applicable not only for other disulfide-linked dendritic polymers but also for exploitation of biological applications.

Authors:
 [1];  [2];  [3];  [4];  [4]
  1. Chinese Academy of Sciences (CAS), Beijing (China)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Chinese Academy of Sciences (CAS), Beijing (China); Zhengzhou Univ., Henan (China)
  4. Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1531348
Report Number(s):
PNNL-SA-136487
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Wang, Xing, Gao, Peiyuan, Yang, Yanyu, Guo, Hongxia, and Wu, Decheng. Dynamic and programmable morphology and size evolution via a living hierarchical self-assembly strategy. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05142-3.
Wang, Xing, Gao, Peiyuan, Yang, Yanyu, Guo, Hongxia, & Wu, Decheng. Dynamic and programmable morphology and size evolution via a living hierarchical self-assembly strategy. United States. https://doi.org/10.1038/s41467-018-05142-3
Wang, Xing, Gao, Peiyuan, Yang, Yanyu, Guo, Hongxia, and Wu, Decheng. Tue . "Dynamic and programmable morphology and size evolution via a living hierarchical self-assembly strategy". United States. https://doi.org/10.1038/s41467-018-05142-3. https://www.osti.gov/servlets/purl/1531348.
@article{osti_1531348,
title = {Dynamic and programmable morphology and size evolution via a living hierarchical self-assembly strategy},
author = {Wang, Xing and Gao, Peiyuan and Yang, Yanyu and Guo, Hongxia and Wu, Decheng},
abstractNote = {Recent advances in the preparation of shape-shifting and size-growing nanostructures are hot topics in development of nanoscience, because many intelligent functions are always relied on their shape and dimension. Here we report a tunable manipulation of sequential self-assembled transformation in situ via a hierarchical assembly strategy based on a living thiol–disulfide exchange reaction. By tailoring the external stimuli, the reactive points can be generated at the ends of initially unimolecular micelles, which subsequently drive the pre-assemblies to periodically proceed into the hierarchically micellar connection, axial growth, bending, and cyclization processes from nanoscopic assemblies to macroscopic particles. Of particular interest would be systems that acquired the shape control and size adjustment of self-assemblies after termination or reactivation of disulfide reshuffling reaction by regulating external stimuli whenever needed. Such a hierarchical strategy for self-assembled evolution is universally applicable not only for other disulfide-linked dendritic polymers but also for exploitation of biological applications.},
doi = {10.1038/s41467-018-05142-3},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Tue Jul 17 00:00:00 EDT 2018},
month = {Tue Jul 17 00:00:00 EDT 2018}
}

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A Filled-Honeycomb-Structured Crystal Formed by Self-Assembly of a Janus Polyoxometalate-Silsesquioxane (POM-POSS) Co-Cluster
journal, November 2015


Polymeric Nanoparticles Amenable to Simultaneous Installation of Exterior Targeting and Interior Therapeutic Proteins
journal, February 2016

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Molecular-Curvature-Induced Spontaneous Formation of Curved and Concentric Lamellae through Nucleation
journal, January 2016

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journal, January 2016


Cover Picture: Structurally Defined Molecular Hypervalent Iodine Catalysts for Intermolecular Enantioselective Reactions (Angew. Chem. Int. Ed. 1/2016)
journal, December 2015

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Kinetically Controlled Sequential Growth of Surface-Grafted Chiral Supramolecular Copolymers
journal, March 2016

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Atomically Precise Prediction of 2D Self-Assembly of Weakly Bonded Nanostructures: STM Insight into Concentration-Dependent Architectures
journal, November 2015


Architecture, self-assembly and properties of well-defined hybrid polymers based on polyhedral oligomeric silsequioxane (POSS)
journal, August 2013


Molecular Biodynamers: Dynamic Covalent Analogues of Biopolymers
journal, January 2017


Fabrication of pH-Responsive Nanoparticles with an AIE Feature for Imaging Intracellular Drug Delivery
journal, August 2016


Synthesis, Self-Assembly, and Photoresponsive Behavior of Tadpole-Shaped Azobenzene Polymers
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Dynamic Combinatorial Chemistry
journal, September 2006

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Supramolecular Coordination: Self-Assembly of Finite Two- and Three-Dimensional Ensembles
journal, November 2011

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Applications of Orthogonal “Click” Chemistries in the Synthesis of Functional Soft Materials
journal, November 2009

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‘Living’ Controlled in Situ Gelling Systems: Thiol−Disulfide Exchange Method toward Tailor-Made Biodegradable Hydrogels
journal, November 2010

  • Wu, De-Cheng; Loh, Xian Jun; Wu, Yun-Long
  • Journal of the American Chemical Society, Vol. 132, Issue 43
  • DOI: 10.1021/ja106639c

A Giant Surfactant of Polystyrene−(Carboxylic Acid-Functionalized Polyhedral Oligomeric Silsesquioxane) Amphiphile with Highly Stretched Polystyrene Tails in Micellar Assemblies
journal, December 2010

  • Yu, Xinfei; Zhong, Sheng; Li, Xiaopeng
  • Journal of the American Chemical Society, Vol. 132, Issue 47
  • DOI: 10.1021/ja1078305

Dynamic Cylindrical Assembly of Triblock Copolymers by a Hierarchical Process of Covalent and Supramolecular Interactions
journal, February 2011

  • Li, Zhou; Ma, Jun; Lee, Nam S.
  • Journal of the American Chemical Society, Vol. 133, Issue 5
  • DOI: 10.1021/ja109191z

A Supramolecular Janus Hyperbranched Polymer and Its Photoresponsive Self-Assembly of Vesicles with Narrow Size Distribution
journal, March 2013

  • Liu, Yong; Yu, Chunyang; Jin, Haibao
  • Journal of the American Chemical Society, Vol. 135, Issue 12
  • DOI: 10.1021/ja3122608

Pathway toward Large Two-Dimensional Hexagonally Patterned Colloidal Nanosheets in Solution
journal, January 2015

  • Ni, Bo; Huang, Mingjun; Chen, Ziran
  • Journal of the American Chemical Society, Vol. 137, Issue 4
  • DOI: 10.1021/ja511694a

A Dual-Thermoresponsive Gemini-Type Supra-amphiphilic Macromolecular [3]Pseudorotaxane Based on Pillar[10]arene/Paraquat Cooperative Complexation
journal, February 2016

  • Chi, Xiaodong; Yu, Guocan; Shao, Li
  • Journal of the American Chemical Society, Vol. 138, Issue 9
  • DOI: 10.1021/jacs.5b13173

Programming Self-Assembly of DNA Origami Honeycomb Two-Dimensional Lattices and Plasmonic Metamaterials
journal, June 2016

  • Wang, Pengfei; Gaitanaros, Stavros; Lee, Seungwoo
  • Journal of the American Chemical Society, Vol. 138, Issue 24
  • DOI: 10.1021/jacs.6b03966

Synthesis of Nonequilibrium Supramolecular Peptide Polymers on a Microfluidic Platform
journal, July 2016

  • Mason, Thomas O.; Michaels, Thomas C. T.; Levin, Aviad
  • Journal of the American Chemical Society, Vol. 138, Issue 30
  • DOI: 10.1021/jacs.6b04136

Nanoscale Control of Polymer Assembly on a Synthetic Catalyst–Bilayer System
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