scholarly journals Homopolymer self-assembly of poly(propylene sulfone) hydrogels via dynamic noncovalent sulfone–sulfone bonding

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Fanfan Du ◽  
Baofu Qiao ◽  
Trung Dac Nguyen ◽  
Michael P. Vincent ◽  
Sharan Bobbala ◽  
...  
Keyword(s):  
Small Molecules ◽  
Self Assembly ◽  
Encapsulation Efficiency ◽  
Dynamic Network ◽  
Hierarchical Structures ◽  
Solvent Polarity ◽  
High Affinity ◽  
Wide Range ◽  
Poly Propylene ◽  
Water Ratio

Abstract Natural biomolecules such as peptides and DNA can dynamically self-organize into diverse hierarchical structures. Mimicry of this homopolymer self-assembly using synthetic systems has remained limited but would be advantageous for the design of adaptive bio/nanomaterials. Here, we report both experiments and simulations on the dynamic network self-assembly and subsequent collapse of the synthetic homopolymer poly(propylene sulfone). The assembly is directed by dynamic noncovalent sulfone–sulfone bonds that are susceptible to solvent polarity. The hydration history, specified by the stepwise increase in water ratio within lower polarity water-miscible solvents like dimethylsulfoxide, controls the homopolymer assembly into crystalline frameworks or uniform nanostructured hydrogels of spherical, vesicular, or cylindrical morphologies. These electrostatic hydrogels have a high affinity for a wide range of organic solutes, achieving >95% encapsulation efficiency for hydrophilic small molecules and biologics. This system validates sulfone–sulfone bonding for dynamic self-assembly, presenting a robust platform for controllable gelation, nanofabrication, and molecular encapsulation.

scholarly journals Polymer cyclization for the emergence of hierarchical nanostructures

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Chaojian Chen ◽  
Manjesh Kumar Singh ◽  
Katrin Wunderlich ◽  
Sean Harvey ◽  
Colette J. Whitfield ◽  
...  
Keyword(s):  
Self Assembly ◽  
Three Dimensional ◽  
Hierarchical Structures ◽  
Structural Similarity ◽  
Vital Role ◽  
Nanomaterial Synthesis ◽  
Wide Range ◽  
Linear Poly ◽  
Polymer Folding ◽  
Dynamics Simulations

AbstractThe creation of synthetic polymer nanoobjects with well-defined hierarchical structures is important for a wide range of applications such as nanomaterial synthesis, catalysis, and therapeutics. Inspired by the programmability and precise three-dimensional architectures of biomolecules, here we demonstrate the strategy of fabricating controlled hierarchical structures through self-assembly of folded synthetic polymers. Linear poly(2-hydroxyethyl methacrylate) of different lengths are folded into cyclic polymers and their self-assembly into hierarchical structures is elucidated by various experimental techniques and molecular dynamics simulations. Based on their structural similarity, macrocyclic brush polymers with amphiphilic block side chains are synthesized, which can self-assemble into wormlike and higher-ordered structures. Our work points out the vital role of polymer folding in macromolecular self-assembly and establishes a versatile approach for constructing biomimetic hierarchical assemblies.

Nanoparticles and self-organisation: the emergence of hierarchical properties from the nanoparticle soup (i.e., the small is getting bigger). Concluding remarks for Faraday Discussion: Nanoparticle Synthesis and Assembly.

2015 ◽  
Vol 181 ◽  
pp. 481-487 ◽  
Author(s):  
David J. Schiffrin
Keyword(s):  
Self Assembly ◽  
Optical Materials ◽  
Nanoparticle Synthesis ◽  
Hierarchical Structures ◽  
Building Blocks ◽  
Main Theme ◽  
Colloid Science ◽  
Wide Range ◽  
Properties Of Materials ◽  
Discussion Format

Some four years ago, one of the participants in this Discussion (Prof. Nicholas Kotov) predicted that: “within five years we shall see multiple examples of electronic, sensor, optical and other devices utilizing self-assembled superstructures” (N. A. Kotov, J. Mater. Chem., 2011, 21, 16673–16674). Although this prediction came partially to fruition, we have witnessed an unprecedented interest in the properties of materials at the nanoscale. The point highlighted by Kotov, however, was the importance of self-assembly of structures from well characterised building blocks to yield hierarchical structures, hopefully with predictable properties, a concept that is an everyday pursuit of synthetic chemists. This Discussion has brought together researchers from a wide range of disciplines, i.e., colloid science, modelling, nanoparticle synthesis and organisation, magnetic and optical materials, and new imaging methods, within the excellent traditional Faraday Discussion format, to discuss advances in areas relevant to the main theme of the meeting.

Polymer Cyclization as a General Strategy for the Emergence of Hierarchical Nanostructures

2020 ◽  
Author(s):  
Chaojian Chen ◽  
Manjesh Kumar Singh ◽  
Katrin Wunderlich ◽  
Sean Harvey ◽  
Manfred Wagner ◽  
...  
Keyword(s):  
Self Assembly ◽  
Three Dimensional ◽  
Hierarchical Structures ◽  
Structural Similarity ◽  
Vital Role ◽  
General Strategy ◽  
Wide Range ◽  
Linear Poly ◽  
Polymer Folding ◽  
Dynamics Simulations

The creation of synthetic polymer nanoobjects with well-defined hierarchical structures is important for a wide range of applications such as nanomaterial synthesis, catalysis, and therapeutics. Inspired by the programmability and precise three-dimensional architectures of biomolecules, here wedemonstrate the strategy of fabricating controlled hierarchical structures through self-assembly of folded synthetic polymers. Linear poly(2-hydroxyethyl methacrylate) of different lengths are folded into cyclic polymers and their self-assembly into hierarchical structures is elucidated by various experimental techniques and molecular dynamics simulations. Based on their structural similarity, macrocyclic brush polymers with amphiphilic block side chains are synthesized, which can self-assemble into wormlike structures and higher-ordered networks. Our work points out the vital role of polymer folding in macromolecular self-assembly and establishes a versatile approach for constructing biomimetic hierarchical assemblies.

Computational modeling of bacteriophage self-assembly during formation of hierarchical structures

2015 ◽  
Vol 1722 ◽  
Author(s):  
Christopher M Warner ◽  
Olexandr Isayev ◽  
Aimee R. Poda ◽  
Michael F. Cuddy ◽  
Wayne D Hodo ◽  
...  
Keyword(s):  
Surface Charge ◽  
Molecular Dynamic ◽  
Self Assembly ◽  
Materials Science ◽  
Hierarchical Structures ◽  
Qualitative Assessment ◽  
Dynamic Simulations ◽  
Phage Types ◽  
Wide Range ◽  
Mutant Phage

ABSTRACTDesigning new materials with well-defined structures and desired functions is a challenge in materials science, especially with nanomaterials. Nature, however, solves design of these materials through a self-assembling, hierarchically ordered process. We have investigated the mechanisms by which the high- aspect ratio and unique surface chemistry of M13 bacteriophage can give rise to increasingly complex, hierarchically ordered, bundled phage structures with a wide range of material applications. A molecular dynamic simulation of the 3-D structure of a 20-nm section of wild type (WT) and mutant phage types were developed based on WT phage crystal structure and ab initio calculations. Simulations of these phage were then used to examine repulsive and attractive forces of the particles in solution. Examination of contact interactions between two WT phage indicated the phage were maximally attracted to each other in a head to tail orientation. A mutant phage (4E) with a higher negative surface charge relative to WT phage also preferentially ordered head to tail in solution. In contrast, a mutant phage (CLP8) with a net positive surface charge had minimal repulsion in a 90° orientation. Understanding the self-assembly process through molecular dynamic simulations and decomposition of fundamental forces driving inter- and intra-strand interactions has provided a qualitative assessment of mechanisms that lead to hierarchical phage bundle structures. Results from simulation agree with experimentally observed patterns from self-assembly. We anticipate using this system to further investigate development of hierarchical structures not only from biological molecules but also from synthetic materials.

scholarly journals Polymer Cyclization as a General Strategy for the Emergence of Hierarchical Nanostructures

2020 ◽  
Author(s):  
Chaojian Chen ◽  
Manjesh Kumar Singh ◽  
Katrin Wunderlich ◽  
Sean Harvey ◽  
Manfred Wagner ◽  
...  
Keyword(s):  
Self Assembly ◽  
Three Dimensional ◽  
Hierarchical Structures ◽  
Structural Similarity ◽  
Vital Role ◽  
General Strategy ◽  
Wide Range ◽  
Linear Poly ◽  
Polymer Folding ◽  
Dynamics Simulations

The creation of synthetic polymer nanoobjects with well-defined hierarchical structures is important for a wide range of applications such as nanomaterial synthesis, catalysis, and therapeutics. Inspired by the programmability and precise three-dimensional architectures of biomolecules, here wedemonstrate the strategy of fabricating controlled hierarchical structures through self-assembly of folded synthetic polymers. Linear poly(2-hydroxyethyl methacrylate) of different lengths are folded into cyclic polymers and their self-assembly into hierarchical structures is elucidated by various experimental techniques and molecular dynamics simulations. Based on their structural similarity, macrocyclic brush polymers with amphiphilic block side chains are synthesized, which can self-assemble into wormlike structures and higher-ordered networks. Our work points out the vital role of polymer folding in macromolecular self-assembly and establishes a versatile approach for constructing biomimetic hierarchical assemblies.

scholarly journals Polymer Cyclization as a General Strategy for the Emergence of Hierarchical Nanostructures

2020 ◽  
Author(s):  
Chaojian Chen ◽  
Manjesh Kumar Singh ◽  
Katrin Wunderlich ◽  
Sean Harvey ◽  
Manfred Wagner ◽  
...  
Keyword(s):  
Self Assembly ◽  
Three Dimensional ◽  
Hierarchical Structures ◽  
Structural Similarity ◽  
Vital Role ◽  
General Strategy ◽  
Wide Range ◽  
Linear Poly ◽  
Polymer Folding ◽  
Dynamics Simulations

The creation of synthetic polymer nanoobjects with well-defined hierarchical structures is important for a wide range of applications such as nanomaterial synthesis, catalysis, and therapeutics. Inspired by the programmability and precise three-dimensional architectures of biomolecules, we report the strategy of fabricating controlled hierarchical structures through self-assembly of folded synthetic polymers. Linear poly(2-hydroxyethyl methacrylate) of different lengths are folded into cyclic polymers and their self-assembly into hierarchical structures is elucidated by various experimental techniques and molecular dynamics simulations. Based on their structural similarity, macrocyclic brush polymers with amphiphilic block side chains are synthesized, which can self-assemble into wormlike structures and higher-ordered networks. Our work points out the vital role of polymer folding in macromolecular self-assembly and establishes a versatile approach for constructing biomimetic hierarchical assemblies.

scholarly journals Homopolymer Self-Assembly via Poly(propylene Sulfone) Networks

2019 ◽  
Author(s):  
Fanfan Du ◽  
Baofu Qiao ◽  
Sharan Bobbala ◽  
sijia yi ◽  
Monica Olvera de la Cruz ◽  
...  
Keyword(s):  
Aqueous Solution ◽  
Self Assembly ◽  
Organic Molecules ◽  
Hierarchical Structures ◽  
Polymer Chains ◽  
Simple System ◽  
Molecular Networks ◽  
Synthetic Materials ◽  
Assembly Behavior ◽  
Poly Propylene

<p>Natural molecules such as peptides and DNA organize dynamically into hierarchical structures with diverse morphologies and sizes. The ability to mimic this self-assembly behavior in synthetic materials has remained an elusive goal. We report on poly(propylene sulfone), a synthetic homopolymer that self-assembles into nanoscale hydrogels of various morphologies including spherical, vesicular, and cylindrical in aqueous solution. Experiments and simulations demonstrate that while the polymer chains are roughly extended and minimally aggregated in DMSO, the addition of water overcomes the steric limitations imposed by the sulfones and induces formation of molecular networks through sulfone-sulfone bonding. Networks collapse and reorganize into distinct morphologies upon hydration, endowing an exceptional capability for capturing organic molecules. This simple system presents a robust platform for controlling nanofabrication.<br></p>

scholarly journals Homopolymer Self-Assembly via Poly(propylene Sulfone) Networks

2019 ◽  
Author(s):  
Fanfan Du ◽  
Baofu Qiao ◽  
Sharan Bobbala ◽  
sijia yi ◽  
Monica Olvera de la Cruz ◽  
...  
Keyword(s):  
Aqueous Solution ◽  
Self Assembly ◽  
Organic Molecules ◽  
Hierarchical Structures ◽  
Polymer Chains ◽  
Simple System ◽  
Molecular Networks ◽  
Synthetic Materials ◽  
Assembly Behavior ◽  
Poly Propylene

<p>Natural molecules such as peptides and DNA organize dynamically into hierarchical structures with diverse morphologies and sizes. The ability to mimic this self-assembly behavior in synthetic materials has remained an elusive goal. We report on poly(propylene sulfone), a synthetic homopolymer that self-assembles into nanoscale hydrogels of various morphologies including spherical, vesicular, and cylindrical in aqueous solution. Experiments and simulations demonstrate that while the polymer chains are roughly extended and minimally aggregated in DMSO, the addition of water overcomes the steric limitations imposed by the sulfones and induces formation of molecular networks through sulfone-sulfone bonding. Networks collapse and reorganize into distinct morphologies upon hydration, endowing an exceptional capability for capturing organic molecules. This simple system presents a robust platform for controlling nanofabrication.<br></p>

Biomimetic materials: An introduction

1992 ◽  
Vol 50 (2) ◽  
pp. 1020-1021 ◽  
Author(s):  
M. Sarikaya ◽  
J. T. Staley ◽  
I. A. Aksay
Keyword(s):  
Self Assembly ◽  
Structural Control ◽  
Hierarchical Structures ◽  
Ceramic Composites ◽  
Advanced Materials ◽  
Length Scale ◽  
Spider Webs ◽  
Biomimetic Materials ◽  
Synthetic Materials ◽  
All Ceramic

Biomimetics is an area of research in which the analysis of structures and functions of natural materials provide a source of inspiration for design and processing concepts for novel synthetic materials. Through biomimetics, it may be possible to establish structural control on a continuous length scale, resulting in superior structures able to withstand the requirements placed upon advanced materials. It is well recognized that biological systems efficiently produce complex and hierarchical structures on the molecular, micrometer, and macro scales with unique properties, and with greater structural control than is possible with synthetic materials. The dynamism of these systems allows the collection and transport of constituents; the nucleation, configuration, and growth of new structures by self-assembly; and the repair and replacement of old and damaged components. These materials include all-organic components such as spider webs and insect cuticles (Fig. 1); inorganic-organic composites, such as seashells (Fig. 2) and bones; all-ceramic composites, such as sea urchin teeth, spines, and other skeletal units (Fig. 3); and inorganic ultrafine magnetic and semiconducting particles produced by bacteria and algae, respectively (Fig. 4).

Factors Affecting Molecular Self-Assembly and Its Mechanism

2012 ◽  
Vol 9 (1) ◽  
pp. 43 ◽  
Author(s):  
Hueyling Tan
Keyword(s):  
Self Assembly ◽  
Building Blocks ◽  
Molecular Engineering ◽  
Molecular Structures ◽  
Polymer Science ◽  
New Approach ◽  
Factors Affecting ◽  
Dna Structures ◽  
Self Assembling ◽  
Wide Range

Molecular self-assembly is ubiquitous in nature and has emerged as a new approach to produce new materials in chemistry, engineering, nanotechnology, polymer science and materials. Molecular self-assembly has been attracting increasing interest from the scientific community in recent years due to its importance in understanding biology and a variety of diseases at the molecular level. In the last few years, considerable advances have been made in the use ofpeptides as building blocks to produce biological materials for wide range of applications, including fabricating novel supra-molecular structures and scaffolding for tissue repair. The study ofbiological self-assembly systems represents a significant advancement in molecular engineering and is a rapidly growing scientific and engineering field that crosses the boundaries ofexisting disciplines. Many self-assembling systems are rangefrom bi- andtri-block copolymers to DNA structures as well as simple and complex proteins andpeptides. The ultimate goal is to harness molecular self-assembly such that design andcontrol ofbottom-up processes is achieved thereby enabling exploitation of structures developed at the meso- and macro-scopic scale for the purposes oflife and non-life science applications. Such aspirations can be achievedthrough understanding thefundamental principles behind the selforganisation and self-synthesis processes exhibited by biological systems.

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