scholarly journals Bottom-up Chemoenzymatic Synthesis Towards Novel Fluorinated Cellulose-like Materials

2020 ◽  
Author(s):  
Peterson de Andrade ◽  
Juan Munoz ◽  
Giulia Pergolizzi ◽  
Valeria Gabrielli ◽  
Sergey Nepogodiev ◽  
...  
Keyword(s):  
Self Assembly ◽  
Soft Matter ◽  
Water Solubility ◽  
Hierarchical Structures ◽  
Building Blocks ◽  
Chemoenzymatic Synthesis ◽  
Cellulose Ii ◽  
Fluorinated Building Blocks ◽  
A Minor

Understanding the fine details of self-assembly of building blocks into complex hierarchical structures represents a major challenge en route to the design and preparation of soft matter materials with specific properties. Enzymatically-synthesised cellodextrins are known to have limited water solubility beyond DP9, a point at which they self-assemble into particles resembling the anti-parallel cellulose II crystalline packing. We have prepared and characterized a series of site-selectively fluorinated cellodextrins of different degrees of fluorination and substitution patterns by chemoenzymatic synthesis. The structural characterization of these materials at different length scales, combining advanced NMR and microscopy methods, showed that multiply 6-fluorinated cellodextrin chains assembled into particles presenting morphological and crystallinity features that are unprecedented for cellulose-like materials. In contrast, the introduction of a single fluorine atom per cellodextrin chain had a minor impact on materials structure. Our work emphasizes the strength of combining chemoenzymatic synthesis, fluorinated building blocks and advanced NMR and microscopy methods for the thorough characterization of hierarchical structures, leading to the controlled design of new biomaterials with specific properties.

scholarly journals Bottom-up Chemoenzymatic Synthesis Towards Novel Fluorinated Cellulose-like Materials

2020 ◽  
Author(s):  
Peterson de Andrade ◽  
Juan Munoz ◽  
Giulia Pergolizzi ◽  
Valeria Gabrielli ◽  
Sergey Nepogodiev ◽  
...  
Keyword(s):  
Self Assembly ◽  
Soft Matter ◽  
Water Solubility ◽  
Hierarchical Structures ◽  
Building Blocks ◽  
Chemoenzymatic Synthesis ◽  
Cellulose Ii ◽  
Fluorinated Building Blocks ◽  
A Minor

Understanding the fine details of self-assembly of building blocks into complex hierarchical structures represents a major challenge en route to the design and preparation of soft matter materials with specific properties. Enzymatically-synthesised cellodextrins are known to have limited water solubility beyond DP9, a point at which they self-assemble into particles resembling the anti-parallel cellulose II crystalline packing. We have prepared and characterized a series of site-selectively fluorinated cellodextrins of different degrees of fluorination and substitution patterns by chemoenzymatic synthesis. The structural characterization of these materials at different length scales, combining advanced NMR and microscopy methods, showed that multiply 6-fluorinated cellodextrin chains assembled into particles presenting morphological and crystallinity features that are unprecedented for cellulose-like materials. In contrast, the introduction of a single fluorine atom per cellodextrin chain had a minor impact on materials structure. Our work emphasizes the strength of combining chemoenzymatic synthesis, fluorinated building blocks and advanced NMR and microscopy methods for the thorough characterization of hierarchical structures, leading to the controlled design of new biomaterials with specific properties.

scholarly journals Synthesis and characterization of poly(amino acid methacrylate)-stabilized diblock copolymer nano-objects

2015 ◽  
Vol 6 (10) ◽  
pp. 1805-1816 ◽  
Author(s):  
Vincent Ladmiral ◽  
Alexandre Charlot ◽  
Mona Semsarilar ◽  
Steven. P. Armes
Keyword(s):  
Amino Acid ◽  
Diblock Copolymer ◽  
Michael Addition ◽  
Self Assembly ◽  
Building Blocks ◽  
Synthesis And Characterization

Two amino acid methacrylates prepared via Michael addition are used as building blocks to prepare novel diblock copolymer nano-objects via polymerisation-induced self-assembly.

scholarly journals Synthesis and characterisation of non-ionic AB-diblock nanoparticles prepared by RAFT dispersion polymerization with polymerization-induced self-assembly

RSC Advances ◽  
2016 ◽  
Vol 6 (33) ◽  
pp. 28130-28139 ◽  
Author(s):  
Yiwen Pei ◽  
Kevin Jarrett ◽  
Leonardo Gutierrez Garces ◽  
Martin Saunders ◽  
Jean-Philippe Croue ◽  
...  
Keyword(s):  
Self Assembly ◽  
Soft Matter ◽  
Dispersion Polymerization ◽  
Synthesis And Characterization

The RAFT-PISA synthesis and characterization of non-ionic soft matter nanoparticles is described.

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.

scholarly journals Development of Natural-Drugs-Based Low-Molecular-Weight Supramolecular Gels

Gels ◽  
2021 ◽  
Vol 7 (3) ◽  
pp. 105
Author(s):  
Xiaoyi Feng ◽  
Yuning Luo ◽  
Fangjie Li ◽  
Xueting Jian ◽  
Yang Liu
Keyword(s):  
Molecular Weight ◽  
Self Assembly ◽  
Water Solubility ◽  
Drug Loading ◽  
Building Blocks ◽  
Low Molecular Weight ◽  
Assembly Mechanism ◽  
Supramolecular Gels ◽  
Potential Applications ◽  
Natural Drugs

Natural small molecular drugs with excellent biocompatibility, diverse pharmacological activities, and wide sources play an increasingly important role in the development of new drug and disease treatment. In recent years, the utilization of paclitaxel, camptothecin, rhein, curcumin, and other natural small molecular drugs with unique rigid backbone structures and modifiable multiple sites as building blocks to form gels by self-assembly has attracted widespread attention. The obtained low-molecular-weight supramolecular gel not only retains the general characteristics of the gel but also overcomes the shortcomings of natural drugs, such as poor water solubility and low bioavailability. It has the advantages of high drug loading, low toxicity, and outstanding stimulus responsiveness, which is widely used in biomedical fields. Here, we provided a comprehensive review of natural-drugs-based low-molecular-weight supramolecular gels reported in recent years and summarized their assembly mechanism, gel structure, gel properties, and potential applications. It is expected to provide a reference for further research of natural-drugs-based supramolecular gels.

Hierarchically Engineered Nanostructures from Compositionally Anisotropic Molecular Building Blocks

2022 ◽  
Author(s):  
Ruiqi Liang ◽  
Yazhen Xue ◽  
Xiaowei Fu ◽  
An Le ◽  
Qingliang Song ◽  
...  
Keyword(s):  
Block Copolymers ◽  
Nanostructured Materials ◽  
Self Assembly ◽  
Structural Parameters ◽  
Hierarchical Structures ◽  
Building Blocks ◽  
Assembly Process ◽  
Multifunctional Materials ◽  
Assembly Strategy ◽  
Molecular Building Blocks

The inability to synthesize hierarchical structures with independently tailored nanoscale and mesoscale features limits the discovery of next-generation multifunctional materials. We present a programmable molecular self-assembly strategy to craft nanostructured materials with a variety of phase-in-phase hierarchical morphologies. The compositionally anisotropic building blocks employed in the assembly process are formed by multi-component graft block copolymers (GBCPs) containing sequence-defined side chains. The judicious design of various structural parameters in the GBCPs enables broadly tunable compositions, morphologies, and lattice parameters across the nanoscale and mesoscale in the assembled structures. Our strategy introduces new design principles for the efficient creation of complex hierarchical structures and provides a facile synthetic platform to access nanomaterials with multiple precisely integrated functionalities.

Self-Assembly of Cyclic Dipeptides: Platforms for Functional Materials

2020 ◽  
Vol 27 (8) ◽  
pp. 688-697
Author(s):  
Yu Chen ◽  
Kai Tao ◽  
Wei Ji ◽  
Pandeeswar Makam ◽  
Sigal Rencus-Lazar ◽  
...  
Keyword(s):  
Self Assembly ◽  
Functional Materials ◽  
Building Blocks ◽  
Cyclic Dipeptide ◽  
Design Synthesis ◽  
Cyclic Dipeptides ◽  
The Past ◽  
Supramolecular Architectures ◽  
Structural Rigidity

Supramolecular self-assembled functional materials comprised of cyclic dipeptide building blocks have excellent prospects for biotechnology applications due to their exceptional structural rigidity, morphological flexibility, ease of preparation and modification. Although the pharmacological uses of many natural cyclic dipeptides have been studied in detail, relatively little is reported on the engineering of these supramolecular architectures for the fabrication of functional materials. In this review, we discuss the progress in the design, synthesis, and characterization of cyclic dipeptide supramolecular nanomaterials over the past few decades, highlighting applications in biotechnology and optoelectronics engineering.

scholarly journals Synthesis by self-assembly and structural characterization of a new co-crystal system {[Cu(NO3)2(H2O)2]L1(NO3)2} (L1 = 1,1′-dibenzyl-3,3′-butyl-diimidazolium-2,2′-diylidene) from copper nitrate and a carbene precursor

2008 ◽  
Vol 6 (4) ◽  
pp. 505-508 ◽  
Author(s):  
Jorge Doimeadios
Keyword(s):  
Solid State ◽  
Hydrogen Bonds ◽  
Structural Characterization ◽  
Self Assembly ◽  
Three Dimensional ◽  
Building Blocks ◽  
Copper Nitrate ◽  
Supramolecular Network ◽  
Crystal System

AbstractHerein, the first example of a co-crystal system formed by an imidazolium nitrate, a carbene precursor, and copper (II) nitrate, {[Cu(NO3)2(H2O)2]L1(NO3)2} (1) (L1 = 1,1′-dibenzyl-3,3′-butyl-diimidazolium-2,2′-diylidene) is reported. These two building blocks are connected in the solid state through hydrogen bonds to generate a three-dimensional supramolecular network.

scholarly journals Supramolecular Alloys from Fluorinated Hybrid [4+6] Imine Cages

2021 ◽  
Author(s):  
Tom Kunde ◽  
Tobias Pausch ◽  
Bernd M. Schmidt
Keyword(s):  
Thermal Stability ◽  
Self Assembly ◽  
Gain Control ◽  
Building Blocks ◽  
The Self ◽  
Feed Ratio ◽  
Assembly Process ◽  
Fluorinated Building Blocks ◽  
Efficient Control ◽  
Innovative Materials

To create innovative materials, efficient control and engineering of pore sizes and their characteristics, crystallinity and stability is required. Eight hybrid [4+6] imine cages with a tuneable degree of fluorination and one fully fluorinated [4+6] imine cage are investigated. Although the fluorinated and the non-fluorinated building blocks used herein differ vastly in reactivity, we are able to gain control over the outcome of the self-assembly process, by carefully controlling the feed ratio. This represents the first hybrid material based on fluorinated/hydrogenated porous organic cages (POCs). These alloys with unlimited miscibility in the solid state were obtained as highly crystalline samples after recrystallization and even showed retention of the crystal lattice. All alloys and the fully fluorinated [4+6] imine cage were analysed by MALDI-MS, SCXRD, PXRD and in regards to thermal stability (TGA). <br>

scholarly journals Hierarchical self-assembly of polydisperse colloidal bananas into a two-dimensional vortex phase

2021 ◽  
Vol 118 (33) ◽  
pp. e2107241118
Author(s):  
Carla Fernández-Rico ◽  
Roel P. A. Dullens
Keyword(s):  
Self Assembly ◽  
Hierarchical Structures ◽  
Building Blocks ◽  
Dimensional Structure ◽  
Two Dimensional ◽  
Complex Materials ◽  
Monodisperse Particles ◽  
Vortex Phase ◽  
Structure And Dynamics ◽  
Particle Level

Self-assembly of microscopic building blocks into highly ordered and functional structures is ubiquitous in nature and found at all length scales. Hierarchical structures formed by colloidal building blocks are typically assembled from monodisperse particles interacting via engineered directional interactions. Here, we show that polydisperse colloidal bananas self-assemble into a complex and hierarchical quasi–two-dimensional structure, called the vortex phase, only due to excluded volume interactions and polydispersity in the particle curvature. Using confocal microscopy, we uncover the remarkable formation mechanism of the vortex phase and characterize its exotic structure and dynamics at the single-particle level. These results demonstrate that hierarchical self-assembly of complex materials can be solely driven by entropy and shape polydispersity of the constituting particles.

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