scholarly journals Viscoelastic behavior of chemically fueled supramolecular hydrogels under load and influence of reaction side products

2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Martin Kretschmer ◽  
Benjamin Winkeljann ◽  
Brigitte A. K. Kriebisch ◽  
Job Boekhoven ◽  
Oliver Lieleg
Keyword(s):  
Self Assembly ◽  
Linear Response ◽  
Viscoelastic Behavior ◽  
Shear Load ◽  
Mechanical Forces ◽  
Waste Products ◽  
New Class ◽  
Synthetic Materials ◽  
New Generation

AbstractAbout ten years ago, chemically fueled systems have emerged as a new class of synthetic materials with tunable properties. Yet, applications of these materials are still scarce. In part, this is due to an incomplete characterization of the viscoelastic properties of those materials, which has – so far – mostly been limited to assessing their linear response under shear load. Here, we fill some of these gaps by comparing the viscoelastic behavior of two different, carbodiimide fueled Fmoc-peptide systems. We find that both, the linear and non-linear response of the hydrogels formed by those Fmoc-peptides depends on the amount of fuel driving the self-assembly process – but hardly on the direction of force application. In addition, we identify the concentration of accumulated waste products as a novel, so far neglected parameter that crucially affects the behavior of such chemically fueled hydrogels. With the mechanistic insights gained here, it should be possible to engineer a new generation of dynamic hydrogels with finely tunable material properties that can be tailored precisely for such applications, where they are challenged by mechanical forces.

scholarly journals Photoresponsive supramolecular coordination polyelectrolyte as smart anticounterfeiting inks

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Zhiqiang Li ◽  
Xiao Liu ◽  
Guannan Wang ◽  
Bin Li ◽  
Hongzhong Chen ◽  
...  
Keyword(s):  
Self Assembly ◽  
Ring Opening ◽  
Resonance Energy Transfer ◽  
Resonance Energy ◽  
Ring Closure ◽  
New Class ◽  
Supramolecular Coordination ◽  
Ligand Coordination ◽  
Information Patterns ◽  
New Generation

AbstractWhile photoluminescence printing is a widely applied anticounterfeiting technique, there are still challenges in developing new generation anticounterfeiting materials with high security. Here we report the construction of a photoresponsive supramolecular coordination polyelectrolyte (SCP) through hierarchical self-assembly of lanthanide ion, bis-ligand and diarylethene unit, driven by metal-ligand coordination and ionic interaction. Owing to the conformation-dependent photochromic fluorescence resonance energy transfer between the lanthanide donor and diarylethene acceptor, the ring-closure/ring-opening isomerization of the diarylethene unit leads to a photoreversible luminescence on/off switch in the SCP. The SCP is then utilized as security ink to print various patterns, through which photoreversible multiple information patterns with visible/invisible transformations are realized by simply alternating the irradiation with UV and visible light. This work demonstrates the possibility of developing a new class of smart anticounterfeiting materials, which could be operated in a noninvasive manner with a higher level of security.

scholarly journals Self-assembled DNA/RNA nanoparticles as a new generation of therapeutic nucleic acids: immunological compatibility and other translational considerations

2016 ◽  
Vol 3 (1) ◽  
Author(s):  
Marina A. Dobrovolskaia
Keyword(s):  
Nucleic Acids ◽  
Self Assembly ◽  
Genetic Disorders ◽  
Nucleic Acid Therapeutics ◽  
New Class ◽  
Effective Interventions ◽  
Microbial Infections ◽  
Reduced Toxicity ◽  
New Generation ◽  
2D And 3D

AbstractTherapeutic nucleic acids (TNAs) are rapidly being embraced as effective interventions in a variety of genetic disorders, cancers, and viral/microbial infections, as well as for use in improving vaccine efficacy. Many traditional nucleotide-based formulations have been approved for clinical use, while various macromolecular nucleic acids are in different phases of preclinical and clinical development. Various nanotechnology carriers, including but not limited to liposomes, emulsions, dendrimers, and polyplexes, are considered for their improved delivery and reduced toxicity compared to traditional TNAs. Moreover, a new generation of TNAs has recently emerged and is represented by DNA/RNA nanoparticles formed by the self-assembly of DNA, RNA, or hybrid DNA-RNA oligonucleotides into 1D, 2D, and 3D structures of different shapes. In this mini-review, I will discuss immunocompatibility and other translational aspects in the development of this new class of promising nucleic acid therapeutics.

scholarly journals Synthesis and Characterization of Bio-Active GFP-P4VP Core–Shell Nanoparticles

Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 627
Author(s):  
Erik Sarnello ◽  
Yuzi Liu ◽  
Bethany Palen ◽  
Elaine Sun ◽  
Xiaobing Zuo ◽  
...  
Keyword(s):  
Self Assembly ◽  
Core Protein ◽  
Core Shell ◽  
Shell Nanoparticles ◽  
Assembly Method ◽  
Synthetic Materials ◽  
Transmission Electron ◽  
Core Shell Nanoparticles ◽  
Enzyme Functionality

Bioactive core–shell nanoparticles (CSNPs) offer the unique ability for protein/enzyme functionality in non-native environments. For many decades, researchers have sought to develop synthetic materials which mimic the efficiency and catalytic power of bioactive macromolecules such as enzymes and proteins. This research studies a self-assembly method in which functionalized, polymer-core/protein-shell nanoparticles are prepared in mild conditions. Transmission electron microscopy (TEM) and dynamic light scattering (DLS) techniques were utilized to analyze the size and distribution of the CSNPs. The methods outlined in this research demonstrate a mild, green chemistry synthesis route for CSNPs which are highly tunable and allow for enzyme/protein functionality in non-native conditions.

Triple-decker cadmium phthalocyanine sandwich complexes: self-assembled EPR active complexes

2009 ◽  
Vol 13 (02) ◽  
pp. 175-187 ◽  
Author(s):  
Isabelle Chambrier ◽  
Jannie C. Swarts ◽  
David L. Hughes ◽  
Michael J. Cook
Keyword(s):  
Self Assembly ◽  
Redox State ◽  
Chemical Oxidation ◽  
Electrochemical Study ◽  
Sandwich Complex ◽  
New Class ◽  
Epr Signal ◽  
Spin Species ◽  
Radical Character

The discovery and characterization of the first example of a bis-cadmiumtris-phthalocyanine triple-decker sandwich complex is reviewed. The compound, with each Pc ring substituted at the eight non-peripheral positions with hexyl chains, was obtained unexpectedly during recrystallization of the corresponding monomeric 1,4,8,11,15,18,22,25-octa-hexyl cadmium phthalocyanine from CH 2 Cl 2 and methanol. The scope for obtaining further examples of this new class of complex bearing different ring substituents is also described. A feature of the compounds is that they give an EPR signal. An electrochemical study has shown that the rest state of the core of the sandwich structure is a dianion arising from the imbalance of the charges on the two cadmium atoms and the three Pc 2- ligands. This is a spin 0 species. It is proposed that the free radical character arises because the potential for the first one-electron oxidation is unusually low for a phthalocyanine, allowing for the partial presence of the spin ½ species for non-peripherally substituted complexes and a more extensive presence of the EPR active redox state for peripherally substituted analogs. Results of chemical oxidation using iodine are also discussed. A spectroscopic and electrochemical study on the monomeric precursors revealed the mode of formation of the triple-decker complexes. It has been established that octa-alkyl cadmium phthalocyanines unexpectedly exist very predominantly as dimeric structures in CH 2 Cl 2 and these are proposed to be intermediates in the formation of the triple-decker complexes. Results from a series of cross experiments using differently substituted Pcs indicate that cadmium can be scrambled between a CdPc and a metal-free Pc . Furthermore, when either species is added to a solution of a triple-decker complex, the ligand from the added species becomes incorporated into new "mixed" triple-decker complexes. From these results it is proposed that the triple-decker structures are formed by self-assembly processes and that they can disassemble and reassemble in the solution phase. Preliminary measurements have identified ring substitution patterns that lead to higher oligomers.

Synthesis and Characterization of D-Galactopyranose-Containing Amphiphilic Block Copolymers via ATRP

2010 ◽  
Vol 663-665 ◽  
pp. 1057-1060
Author(s):  
Xin Wang ◽  
Yuan Yuan Dou ◽  
Mei Shan Pei ◽  
Xin De Tang
Keyword(s):  
Self Assembly ◽  
Average Molecular Weight ◽  
Gel Permeation Chromatography ◽  
Monomethyl Ether ◽  
Amphiphilic Copolymers ◽  
Molecular Weights ◽  
Synthetic Materials ◽  
Potential Applications ◽  
Poly Ethylene

Biocompatible and biodegradable synthetic materials have attracted considerable attention during the past two decades. In this work, a series of amphiphilic triblock copolymers containing D-galactopyranose were synthesized by atom transfer radical polymerization (ATRP). The macroinitiator was prepared by the esterification between poly(ethylene glycol) monomethyl ether with a number-average molecular weight of 1200 g/mol (MeOPEO-1200) and 2-bromoisobutyryl bromide. The sugar-bearing monomer, 6-O-methacryloyl-1,2;3,4-di-O-isopropylidene-D-galactopyranose (MAIPG) was polymerized using PMDETA/CuBr as catalytic system and anisol as solvent. The chemical structure and composition of the resultant polymer MeOPEO-b-PMAIPG were verified by 1H NMR. The molecular weights and their polydispersities were characterized by gel permeation chromatography (GPC). The results indicate that the polymerization follows the mechanism of ATRP. The amphiphilic copolymers can self-assembly to from micelles with PMAIPG as the core and PEO as the corona, which have potential applications as biomaterials or controlled release drug delivery systems.

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).

A Bottom-Up Approach to Solution-Processed, Atomically Precise Graphitic Cylinders on Surfaces

2018 ◽  
Author(s):  
Erik Leonhardt ◽  
Jeff M. Van Raden ◽  
David Miller ◽  
Lev N. Zakharov ◽  
Benjamin Aleman ◽  
...  
Keyword(s):  
Self Assembly ◽  
Carbon Nanostructures ◽  
Carbon Nanomaterials ◽  
Circle Packing ◽  
Pyrolytic Graphite ◽  
Building Blocks ◽  
Bottom Up ◽  
Casting Technique ◽  
New Class ◽  
Solution Casting Technique

Extended carbon nanostructures, such as carbon nanotubes (CNTs), exhibit remarkable properties but are difficult to synthesize uniformly. Herein, we present a new class of carbon nanomaterials constructed via the bottom-up self-assembly of cylindrical, atomically-precise small molecules. Guided by supramolecular design principles and circle packing theory, we have designed and synthesized a fluorinated nanohoop that, in the solid-state, self-assembles into nanotube-like arrays with channel diameters of precisely 1.63 nm. A mild solution-casting technique is then used to construct vertical “forests” of these arrays on a highly-ordered pyrolytic graphite (HOPG) surface through epitaxial growth. Furthermore, we show that a basic property of nanohoops, fluorescence, is readily transferred to the bulk phase, implying that the properties of these materials can be directly altered via precise functionalization of their nanohoop building blocks. The strategy presented is expected to have broader applications in the development of new graphitic nanomaterials with π-rich cavities reminiscent of CNTs.

Targeting IDH Mutations in AML: Wielding the Double-edged Sword of Differentiation

2020 ◽  
Vol 20 (7) ◽  
pp. 490-500 ◽  
Author(s):  
Justin S. Becker ◽  
Amir T. Fathi
Keyword(s):  
Genome Structure ◽  
Cellular Metabolism ◽  
Standard Of Care ◽  
Competitive Inhibitor ◽  
Driver Mutations ◽  
New Class ◽  
Regulatory Enzymes ◽  
Idh Mutations ◽  
Genomic Characterization

The genomic characterization of acute myeloid leukemia (AML) by DNA sequencing has illuminated subclasses of the disease, with distinct driver mutations, that might be responsive to targeted therapies. Approximately 15-23% of AML genomes harbor mutations in one of two isoforms of isocitrate dehydrogenase (IDH1 or IDH2). These enzymes are constitutive mediators of basic cellular metabolism, but their mutated forms in cancer synthesize an abnormal metabolite, 2- hydroxyglutarate, that in turn acts as a competitive inhibitor of multiple gene regulatory enzymes. As a result, leukemic IDH mutations cause changes in genome structure and gene activity, culminating in an arrest of normal myeloid differentiation. These discoveries have motivated the development of a new class of selective small molecules with the ability to inhibit the mutant IDH enzymes while sparing normal cellular metabolism. These agents have shown promising anti-leukemic activity in animal models and early clinical trials, and are now entering Phase 3 study. This review will focus on the growing preclinical and clinical data evaluating IDH inhibitors for the treatment of IDH-mutated AML. These data suggest that inducing cellular differentiation is central to the mechanism of clinical efficacy for IDH inhibitors, while also mediating toxicity for patients who experience IDH Differentiation Syndrome. Ongoing trials are studying the efficacy of IDH inhibitors in combination with other AML therapies, both to evaluate potential synergistic combinations as well as to identify the appropriate place for IDH inhibitors within existing standard-of-care regimens.

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