scholarly journals Concurrent Control over Sequence and Dispersity in Multiblock Copolymers

2020 ◽  
Author(s):  
Maria-Nefeli Antonopoulou ◽  
Richard Whitfield ◽  
Nghia Truong ◽  
Athina Anastasaki
Keyword(s):  
Self Assembly ◽  
Material Design ◽  
Building Blocks ◽  
Polymer Science ◽  
One Pot ◽  
Concurrent Control ◽  
Molecular Weights ◽  
Monomer Sequence ◽  
High Dispersity ◽  
Synthetic Macromolecules

<p>Controlling monomer sequence in synthetic macromolecules is a major challenge in polymer science and the order of building blocks has already been demonstrated to determine macromolecular folding, self-assembly and fundamental polymer properties. Dispersity is another key parameter in material design, with both low and high dispersity polymers displaying complementary properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot, and rapid synthesis of sequence-controlled multiblocks with on demand control over dispersity while maintaining high livingness, excellent agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in chain transfer agent activity during controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (<i>Ɖ</i>=1.16 →1.60), descending (<i>Ɖ</i>=1.66 →1.22), alternating low and high dispersity values (<i>Ɖ</i>=1.17 →1.61 →1.24 →1.70 →1.26) or any combination thereof. The enormous potential of our methodology was further demonstrated through the impressive synthesis of highly ordered pentablock, octablock and decablock copolymers yielding the first generation of multiblocks with concurrent control over both sequence and dispersity.</p>

scholarly journals Concurrent Control over Sequence and Dispersity in Multiblock Copolymers

2020 ◽  
Author(s):  
Maria-Nefeli Antonopoulou ◽  
Richard Whitfield ◽  
Nghia Truong ◽  
Athina Anastasaki
Keyword(s):  
Self Assembly ◽  
Material Design ◽  
Building Blocks ◽  
Polymer Science ◽  
One Pot ◽  
Concurrent Control ◽  
Molecular Weights ◽  
Monomer Sequence ◽  
High Dispersity ◽  
Synthetic Macromolecules

<p>Controlling monomer sequence in synthetic macromolecules is a major challenge in polymer science and the order of building blocks has already been demonstrated to determine macromolecular folding, self-assembly and fundamental polymer properties. Dispersity is another key parameter in material design, with both low and high dispersity polymers displaying complementary properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot, and rapid synthesis of sequence-controlled multiblocks with on demand control over dispersity while maintaining high livingness, excellent agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in chain transfer agent activity during controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (<i>Ɖ</i>=1.16 →1.60), descending (<i>Ɖ</i>=1.66 →1.22), alternating low and high dispersity values (<i>Ɖ</i>=1.17 →1.61 →1.24 →1.70 →1.26) or any combination thereof. The enormous potential of our methodology was further demonstrated through the impressive synthesis of highly ordered pentablock, octablock and decablock copolymers yielding the first generation of multiblocks with concurrent control over both sequence and dispersity.</p>

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.

scholarly journals Inhibition of the urea-urease reaction by the components of the zeolite imidazole frameworks-8 and the formation of urease-zinc-imidazole hybrid compound

2022 ◽  
Author(s):  
Norbert Német ◽  
Ylenia Miele ◽  
Gábor Shuszter ◽  
Eszter L. Tóth ◽  
János Endre Maróti ◽  
...  
Keyword(s):  
Self Assembly ◽  
Enzymatic Reaction ◽  
Synthesis Method ◽  
Material Design ◽  
Building Blocks ◽  
Zinc Ions ◽  
Material Synthesis ◽  
Hybrid Compound ◽  
Inhibition Effect ◽  
Metal Organic

AbstractIn the past decade, much effort has been devoted to using chemical clock-type reactions in material design and driving the self-assembly of various building blocks. Urea-urease enzymatic reaction has chemical pH clock behavior in an unbuffered medium, in which the induction time and the final pH can be programmed by the concentrations of the reagents. The urea-urease reaction can offer a new alternative in material synthesis, where the pH and its course in time are crucial factors in the synthesis. However, before using it in any synthesis method, it is important to investigate the possible effects of the reagents on the enzymatic reaction. Here we investigate the effect of the reagents of the zeolite imidazole framework-8 (zinc ions and 2-methylimidazole) on the urea-urease reaction. We have chosen the zeolite imidazole framework-8 because its formation serves as a model reaction for the formation of other metal–organic frameworks. We found that, besides the inhibition effect of the zinc ions which is well-known in the literature, 2-methylimidazole inhibits the enzymatic reaction as well. In addition to the observed inhibition effect, we report the formation of a hybrid urease-zinc-2-methylimidazole hybrid material. To support the inhibition effect, we developed a kinetic model which reproduced qualitatively the experimentally observed kinetic curves.

scholarly journals Aptamer Functionalized DNA Hydrogel for Wise-Stage Controlled Protein Release

2018 ◽  
Vol 8 (10) ◽  
pp. 1941 ◽  
Author(s):  
Chen Liu ◽  
Jialun Han ◽  
Yuxuan Pei ◽  
Jie Du
Keyword(s):  
Self Assembly ◽  
Protein Delivery ◽  
Stable State ◽  
Building Blocks ◽  
One Pot ◽  
Protein Capture ◽  
Whole Process ◽  
Good Biocompatibility ◽  
Release Program ◽  
Dna Hydrogel

With the simple functionalization method and good biocompatibility, an aptamer-integrated DNA hydrogel is used as the protein delivery system with an adjustable release rate and time by using complementary sequences (CSs) as the biomolecular trigger. The aptamer-functionalized DNA hydrogel was prepared via a one-pot self-assembly process from two kinds of DNA building blocks (X-shaped and L-shaped DNA units) and a single-stranded aptamer. The gelling process was achieved under physiological conditions within one minute. In the absence of the triggering CSs, the aptamer grafted in the hydrogel exhibited a stable state for protein-specific capture. While hybridizing with the triggering CSs, the aptamer is turned into a double-stranded structure, resulting in the fast dissociation of protein with a wise-stage controlled release program. Further, the DNA hydrogel with excellent cytocompatibility has been successfully applied to human serum, forming a complex matrix. The whole process of protein capture and release were biocompatible and could not refer to any adverse factor of the protein or cells. Thus, the aptamer-functionalized DNA hydrogel will be a good candidate for controlled protein delivery.

Factors Affecting Molecular Self-Assembly and Its Mechanism

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

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 of peptides 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 of biological self-assembly systems represents a significant advancement in molecular engineering and is a rapidly growing scientific and engineering field that crosses the boundaries of existing disciplines. Many self-assembling systems are range from bi- and tri-block copolymers to DNA structures as well as simple and complex proteins and peptides. The ultimate goal is to harness molecular self-assembly such that design and control of bottom-up processes is achieved thereby enabling exploitation of structures developed at the meso- and macro-scopic scale for the purposes of life and non-life science applications. Such aspirations can be achieved through understanding the fundamental principles behind the self­ organisation and self-synthesis processes exhibited by biological systems.

Self-Assembly of Peptide Amphiphiles: Molecularly Engineered Bionanomaterials

2015 ◽  
Vol 1113 ◽  
pp. 586-593 ◽  
Author(s):  
Hamizah Shamsudeen ◽  
Huey Ling Tan
Keyword(s):  
Self Assembly ◽  
Building Blocks ◽  
Molecular Engineering ◽  
Molecular Structures ◽  
Significant Advance ◽  
Polymer Science ◽  
New Approach ◽  
Dna Structures ◽  
Self Assembling ◽  
Wide Range

Molecular self-assembly is ubiquitous in nature and has now emerged as a new approach in chemical synthesis, engineering, nanotechnology, polymer science, and materials. Molecular self-assembly has been attracting increasing interest from the scientific community in the 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 of peptides as building blocks to produce biological materials for wide range of applications, including fabricating novel supra-molecular structures and scaffolding for tissue repair. Today, the study of biological self-assembly systems represent a significant advance in the molecular engineering and is a rapidly growing scientific and engineering field that crosses the boundaries of existing disciplines. Many self-assembling systems are range from bi-and tri-block copolymers to complex DNA structures as well as simple and complex proteins and peptides. The attractiveness of such bottom-up processes lies in their capability to build uniform, functional units or arrays and the possibility to exploit such structures at meso-and macroscopic scale for life and non-life science applications.

Mesoporous Hybrid Thin Films: Building Blocks for Complex Materials with Spatial Organization

2007 ◽  
Vol 1007 ◽  
Author(s):  
Galo J. Soler-Illia ◽  
Paula C. Angelomé ◽  
M. Cecilia Fuertes ◽  
Alejandro Wolosiuk ◽  
Sara A. Bilmes ◽  
...  
Keyword(s):  
Thin Films ◽  
Self Assembly ◽  
Spatial Organization ◽  
Sol Gel ◽  
Building Blocks ◽  
Film Deposition ◽  
One Pot ◽  
Selective Functionalization ◽  
Hybrid Thin Films ◽  
Sol Gel Synthesis

ABSTRACTMesoporous Hybrid Thin Films (MHTF) of a variety of compositions and embedded organic functions are produced by combining sol-gel synthesis, template self-assembly and surface modification. One-pot or post-grafting strategies permit to modify the pore surface behavior. Highly controlled MHTF issued from a reproducible and modular synthesis can be used as building blocks for more complex structures, presenting order at larger scales, and novel properties derived from this multiscale order. Multilayer stacks of MHTF presenting specific and different functions and frameworks located in a well-defined position have been produced by combining sequential film deposition, selective functionalization and dissolution. These systems present new properties such as localized chemistry or modulable photonic crystal behavior.

scholarly journals Cooperative Assembly of Asymmetric Carbonaceous Bivalve-Like Superstructures from Multiple Building Blocks

Research ◽  
2018 ◽  
Vol 2018 ◽  
pp. 1-10 ◽  
Author(s):  
Lei Xie ◽  
Haiyan Wang ◽  
Chunhong Chen ◽  
Shanjun Mao ◽  
Yiqing Chen ◽  
...  
Keyword(s):  
Self Assembly ◽  
Materials Science ◽  
Building Blocks ◽  
Hydrothermal Carbonization ◽  
Solid Particles ◽  
Porous Polymers ◽  
One Pot ◽  
In Suit ◽  
Cooperative Assembly ◽  
Ordered Porous

The assembly of superstructures from building blocks is of fundamental importance for engineering materials with distinct morphologies and properties, and deepening our understanding of self-assembly processes in nature. Up to now, it is still a great challenge in materials science to construct multiple-component superstructure with unprecedented architectural complexity and symmetry from molecular. Here, we demonstrate an improved one-pot hydrothermal carbonization of biomass strategy that is capable of fabricating unprecedented asymmetric carbonaceous bivalve-like superstructures with in suit generated solid particles and ordered porous polymers as two kinds of building blocks. In our system, different building blocks can be controllably generated, and they will assemble into complex superstructures through a proposed “cooperative assembly of particles and ordered porous polymers” mechanism. We believe that this assembly principle will open up new potential fields for the synthesis of superstructures with diverse morphologies, compositions, and properties.

Bionanocomposite from self-assembled building blocks of nacre-like crystalline polymorph of chitosan with clay nanoplatelets

RSC Advances ◽  
2016 ◽  
Vol 6 (40) ◽  
pp. 33501-33509 ◽  
Author(s):  
Sergey Sarin ◽  
Sophia Kolesnikova ◽  
Irina Postnova ◽  
Chang-Sik Ha ◽  
Yury Shchipunov
Keyword(s):  
Self Assembly ◽  
Building Blocks ◽  
One Pot ◽  
Evaporation Induced Self Assembly ◽  
Self Assembled ◽  
Pot Technique

Films containing a new crystalline polymorph are prepared by a one-pot technique combining the formation of building blocks of clay nanoplatelets with chitosan macromolecules and their evaporation-induced self-assembly.

scholarly journals An Amphiphilic-DNA Platform for the Design of Crystalline Frameworks with Programmable Structure and Functionality

2018 ◽  
Author(s):  
Ryan A. Brady ◽  
Nicholas J. Brooks ◽  
Vito Foderà ◽  
Pietro Cicuta ◽  
Lorenzo Di Michele
Keyword(s):  
Self Assembly ◽  
Rational Design ◽  
Dna Nanotechnology ◽  
Building Blocks ◽  
Lattice Parameter ◽  
One Pot ◽  
Dna Crystals ◽  
Dna Materials ◽  
Fine Tune ◽  
Highly Porous

<div> <div> <div> <p>The reliable preparation of functional, ordered, nanostructured frameworks would be a game changer for many emerging technologies, from energy storage to nanomedicine. Underpinned by the excellent molecular recognition of nucleic acids, along with their facile synthesis and breadth of available functionalizations, DNA Nanotechnology is widely acknowledged as a prime route for the rational design of nanostructured materials. Yet, the preparation of crystalline DNA frameworks with programmable structure and functionality remains a challenge. Here we demonstrate the potential of simple amphiphilic DNA motifs, dubbed C-stars, as a versatile platform for the design of programmable DNA crystals. In contrast to all-DNA materials, in which structure depends on the precise molecular details of individual building blocks, the self-assembly of C-stars is controlled uniquely by their topology and symmetry. Exploiting this robust self-assembly principle we design a range of topologically identical, but structurally and chemically distinct C-stars that following a one-pot reaction self- assemble into highly porous, functional, crystalline frameworks. Simple design variations allow us to fine-tune the lattice parameter and thus control the partitioning of macromolecules within the frameworks, embed responsive mo- tifs that can induce isothermal disassembly, and include chemical moieties to capture target proteins specifically and reversibly.</p></div> </div> </div>

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