Luminescent Water Dispersible Microporous Polymeric Nanospheres

2018 ◽  
Author(s):  
Alex James ◽  
Matthew Derry ◽  
Jennifer Train ◽  
Robert Dawson
Keyword(s):  
Self Assembly ◽  
Picric Acid ◽  
Water Dispersible ◽  
X Ray Scattering ◽  
Reversible Addition ◽  
Wide Range ◽  
Small Primary ◽  
Shell Particles ◽  
Polymeric Nanospheres ◽  
Polymeric Dispersions

<p>Water-dispersible porous polymeric dispersions (PPDs) have been synthesised by reversible addition-fragmentation chain transfer mediated polymerisation-induced self-assembly (RAFT-mediated PISA). The core-shell particles posses a microporous core formed from divinylbenzene and fumaronitrile while the outer polyethylene glycol shell enables the particles to be dispersible in a wide range of solvents. The PPD was shown to have a heirarchical structure of small primary nanoparticles within larger, well-defined aggregates of 220 nm as measured by electron microscopy and small angle x-ray scattering (SAXS) and exhibited a surface area of 274 m<sup>2</sup>/g. Furthermore these samples were found to be fluoresent and demonstrate selective detection of harmful nitroaramatics in solution with extremly low limits of detection, 169 ppb for picric acid, as well as possessing a CO<sub>2</sub> uptake of 1.1 mmol/g at 273 K.</p>

scholarly journals Luminescent Water Dispersible Microporous Polymeric Nanospheres

2018 ◽  
Author(s):  
Alex James ◽  
Matthew Derry ◽  
Jennifer Train ◽  
Robert Dawson
Keyword(s):  
Self Assembly ◽  
Picric Acid ◽  
Water Dispersible ◽  
X Ray Scattering ◽  
Reversible Addition ◽  
Wide Range ◽  
Small Primary ◽  
Shell Particles ◽  
Polymeric Nanospheres ◽  
Polymeric Dispersions

<p>Water-dispersible porous polymeric dispersions (PPDs) have been synthesised by reversible addition-fragmentation chain transfer mediated polymerisation-induced self-assembly (RAFT-mediated PISA). The core-shell particles posses a microporous core formed from divinylbenzene and fumaronitrile while the outer polyethylene glycol shell enables the particles to be dispersible in a wide range of solvents. The PPD was shown to have a heirarchical structure of small primary nanoparticles within larger, well-defined aggregates of 220 nm as measured by electron microscopy and small angle x-ray scattering (SAXS) and exhibited a surface area of 274 m<sup>2</sup>/g. Furthermore these samples were found to be fluoresent and demonstrate selective detection of harmful nitroaramatics in solution with extremly low limits of detection, 169 ppb for picric acid, as well as possessing a CO<sub>2</sub> uptake of 1.1 mmol/g at 273 K.</p>

scholarly journals In situ SAXS studies of a prototypical RAFT aqueous dispersion polymerization formulation: monitoring the evolution in copolymer morphology during polymerization-induced self-assembly

2020 ◽  
Vol 11 (42) ◽  
pp. 11443-11454 ◽  
Author(s):  
Adam Czajka ◽  
Steven P. Armes
Keyword(s):  
Diblock Copolymer ◽  
Small Angle ◽  
Self Assembly ◽  
Dispersion Polymerization ◽  
Chain Transfer ◽  
Aqueous Dispersion ◽  
X Ray ◽  
X Ray Scattering ◽  
Reversible Addition

In situ small-angle X-ray scattering is used to monitor the formation of diblock copolymer spheres, worms and vesicles during reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of 2-hydroxypropyl methacrylate.

scholarly journals Synthesis of Aminated Polystyrene and Its Self-assembly with Nanoparticles at Oil/water Interface

2020 ◽  
Author(s):  
Chenliang Shi ◽  
Yukun Yang ◽  
Ling Lin ◽  
Wenjia Luo ◽  
Maoqing Deng ◽  
...  
Keyword(s):  
Interfacial Tension ◽  
Self Assembly ◽  
Carbon Dots ◽  
Dynamics Simulation ◽  
Functionalized Polymers ◽  
Amino Groups ◽  
Reversible Addition ◽  
Wide Range ◽  
Two Phases ◽  
Short Time

Nanoparticle (NP)&ndash;surfactants formed by the self-assembly of NPs and end-functionalized polymers at the hydrophilic/hydrophobic interface have a wide range of applications in many fields. In this study, the influence of density of amino groups, NPs dimension and pH on the interaction between end-functionalized polymers and NPs were extensively investigated. Single amino-terminated polystyrene (PS-NH2, Mw &asymp; 0.6k, 2.5k, 3.5k, 3.9k) and diamino-terminated polystyrene (H2N-PS-NH2, Mw &asymp; 1.1k, 2.8k) were prepared using reversible addition&ndash;fragmentation chain transfer polymerization and atom transfer radical polymerization. NPs with different dimensions (zero-dimensional carbon dots with sulfonate groups, one-dimensional cellulose nanocrystals with sulfate groups and two-dimensional graphene with sulfonate groups) in the aqueous phase were added into the toluene phase containing the aminated PS. The influence of pH and the molecular weight of amino-terminated PS on the interfacial tension between two phases were investigated. The results indicate that aminated PS exhibited the strongest interfacial activity after compounding with sulfonated NPs at a pH of 3. Terminating PS with amino groups on both ends leads to better performance in in reducing the water/toluene interfacial tension than modifying the molecular structure of PS on a single end. The dimension of sulfonated NPs also contributed significantly to the reduction of the water/toluene interfacial tension. The minimal interfacial tension was 4.49 mN/m after compounding PS-NH2 with sulfonated zero-dimensional carbon dots. Molecular dynamics simulation on the evolution of the water/toluene interface in the presence of sulfonated carbon dots and H2N-PS-NH2 revealed that these opposite charged substances moved towards the interface in an extreme short time and orderly assembled in a thermodynamic equilibrium.

Structure of Cobalt Nanosphere Superlattice Films by Small Angle X-ray Scattering

2004 ◽  
Vol 818 ◽  
Author(s):  
Michael Beerman ◽  
Masato Ohnuma ◽  
Yuping Bao ◽  
Kannan M. Krishnan
Keyword(s):  
Small Angle ◽  
Self Assembly ◽  
The Self ◽  
Interparticle Spacing ◽  
Face Centered Cubic ◽  
X Ray ◽  
X Ray Scattering ◽  
Least Squares Fit ◽  
Wide Range ◽  
Ray Scattering

AbstractCobalt nanocrystals, recently synthesized with narrow size distributions and controlled shapes, organize in a wide range of arrays as a function of shape, size and interparticle interactions. The nanocrystals (NCs) consist of a cobalt metal core with a nominal diameter of 11 nm, and an organic surfactant surface layer with a chain length of ∼1.7 nm. For the simplest case (ε-Co nanospheres, super-paramagnetic at room temperature) a hexagonal arrangement of NCs is observed in transmission electron microscope (TEM) images when precipitated from solution onto carbon films. For practical applications and for further understanding of the self-assembly process, long range order of the super lattice must be probed over regions that are greater in extent than may be examined by TEM. Hence, small angle x-ray scattering (SAXS) measurements were performed on cobalt nanospheres randomly dispersed in solution and assembled on glass substrates. Least squares fit to the intensity distribution as a function of the scattering vector q gave an average particle diameter of 11.0 ± 0.8 nm. Structure factor contribution to the intensity profile agrees well with a quasi-random model for scattering from a face centered cubic (FCC) superlattice composed of uniform radius cobalt spheres. The measured nearest neighbor interparticle spacing, 14.1 nm, agrees to within 2% of the predicted value of 14.4 nm based on a free energy model that governs the self-assembly of the nanoparticle system.

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.

In situ Time-Resolved Small-Angle X-ray Scattering Reveals the Formation Kinetics of Polyelectrolyte Complex Micelles

2019 ◽  
Author(s):  
Hao Wu ◽  
Jeffrey Ting ◽  
Siqi Meng ◽  
Matthew Tirrell
Keyword(s):  
Small Angle ◽  
Self Assembly ◽  
Electrostatic Interactions ◽  
Polyelectrolyte Complex ◽  
Time Resolved ◽  
X Ray ◽  
X Ray Scattering ◽  
Kinetics Of ◽  
Ray Scattering

We have directly observed the <i>in situ</i> self-assembly kinetics of polyelectrolyte complex (PEC) micelles by synchrotron time-resolved small-angle X-ray scattering, equipped with a stopped-flow device that provides millisecond temporal resolution. This work has elucidated one general kinetic pathway for the process of PEC micelle formation, which provides useful physical insights for increasing our fundamental understanding of complexation and self-assembly dynamics driven by electrostatic interactions that occur on ultrafast timescales.

scholarly journals Interfacial Crystallization and Supramolecular Self-Assembly of Spider Silk Inspired Protein at the Water-Air Interface

Materials ◽  
2021 ◽  
Vol 14 (15) ◽  
pp. 4239
Author(s):  
Pezhman Mohammadi ◽  
Fabian Zemke ◽  
Wolfgang Wagermaier ◽  
Markus B. Linder
Keyword(s):  
Self Assembly ◽  
Spider Silk ◽  
Assembly Process ◽  
Protein Solution ◽  
Time Resolved ◽  
Macromolecular Assembly ◽  
X Ray Scattering ◽  
Air Interface ◽  
Fundamental Research ◽  
Β Sheet

Macromolecular assembly into complex morphologies and architectural shapes is an area of fundamental research and technological innovation. In this work, we investigate the self-assembly process of recombinantly produced protein inspired by spider silk (spidroin). To elucidate the first steps of the assembly process, we examined highly concentrated and viscous pendant droplets of this protein in air. We show how the protein self-assembles and crystallizes at the water–air interface into a relatively thick and highly elastic skin. Using time-resolved in situ synchrotron X-ray scattering measurements during the drying process, we showed that the skin evolved to contain a high β-sheet amount over time. We also found that β-sheet formation strongly depended on protein concentration and relative humidity. These had a strong influence not only on the amount, but also on the ordering of these structures during the β-sheet formation process. We also showed how the skin around pendant droplets can serve as a reservoir for attaining liquid–liquid phase separation and coacervation from the dilute protein solution. Essentially, this study shows a new assembly route which could be optimized for the synthesis of new materials from a dilute protein solution and determine the properties of the final products.

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.

scholarly journals Synthesis of aminated polystyrene and its self-assembly with nanoparticles at oil/water interface

e-Polymers ◽  
2020 ◽  
Vol 20 (1) ◽  
pp. 317-327
Author(s):  
Chenliang Shi ◽  
Ling Lin ◽  
Yukun Yang ◽  
Wenjia Luo ◽  
Maoqing Deng ◽  
...  
Keyword(s):  
Interfacial Tension ◽  
Self Assembly ◽  
Carbon Dots ◽  
Chain Transfer ◽  
Functionalized Polymers ◽  
Amino Groups ◽  
One Dimensional ◽  
Reversible Addition ◽  
Oil Water ◽  
Chain Transfer Polymerization

AbstractThe influence of density of amino groups, nanoparticles dimension and pH on the interaction between end-functionalized polymers and nanoparticles was extensively investigated in this study. PS–NH2 and H2N–PS–NH2 were prepared using reversible addition–fragmentation chain transfer polymerization and atom transfer radical polymerization. Zero-dimensional carbon dots with sulfonate groups, one-dimensional cellulose nanocrystals with sulfate groups and two-dimensional graphene with sulfonate groups in the aqueous phase were added into the toluene phase containing the aminated PS. The results indicate that aminated PS exhibited the strongest interfacial activity after compounding with sulfonated nanoparticles at a pH of 3. PS ended with two amino groups performed better in reducing the water/toluene interfacial tension than PS ended with only one amino group. The dimension of sulfonated nanoparticles also contributed significantly to the reduction in the water/toluene interfacial tension. The minimal interfacial tension was 4.49 mN/m after compounding PS–NH2 with sulfonated zero-dimensional carbon dots.

scholarly journals Hybrid Acrylated Chitosan and Thiolated Pectin Cross-Linked Hydrogels with Tunable Properties

Polymers ◽  
2021 ◽  
Vol 13 (2) ◽  
pp. 266
Author(s):  
Shaked Eliyahu ◽  
Alexandra Galitsky ◽  
Esther Ritov ◽  
Havazelet Bianco-Peled
Keyword(s):  
Electrostatic Interactions ◽  
Profile Analysis ◽  
Hybrid Hydrogel ◽  
Texture Profile ◽  
Ph Values ◽  
X Ray Scattering ◽  
Wide Range ◽  
Michael Type Addition ◽  
Physical And Chemical ◽  
Hydrogel System

We developed and characterized a new hydrogel system based on the physical and chemical interactions of pectin partially modified with thiol groups and chitosan modified with acrylate end groups. Gelation occurred at high pectin thiol ratios, indicating that a low acrylated chitosan concentration in the hydrogel had a profound effect on the cross-linking. Turbidity, Fourier transform infrared spectroscopy, and free thiol determination analyses were performed to determine the relationships of the different bonds inside the gel. At low pH values below the pKa of chitosan, more electrostatic interactions were formed between opposite charges, but at high pH values, the Michael-type addition reaction between acrylate and thiol took place, creating harder hydrogels. Swelling experiments and Young’s modulus measurements were performed to study the structure and properties of the resultant hydrogels. The nanostructure was examined using small-angle X-ray scattering. The texture profile analysis showed a unique property of hydrogel adhesiveness. By implementing changes in the preparation procedure, we controlled the hydrogel properties. This hybrid hydrogel system can be a good candidate for a wide range of biomedical applications, such as a mucosal biomimetic surface for mucoadhesive testing.

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