A rapid and universal approach for multifunctional material coatings was developed based on a mussel-inspired dendritic polymer. This new kind of polymer mimics not only the functional groups of mussel foot proteins (mfps) but also their molecular weight and molecular structure. The large number of catechol and amine groups set the basis for heteromultivalent anchoring and crosslinking. The molecular weight reaches 10 kDa, which is similar to the most adhesive mussel foot protein mfp-5. Also, the dendritic structure exposes its functional groups on the surface like the folded proteins. As a result, a very stable coating can be prepared on virtually any type of material surface within 10 min by a simple dip-coating method, which is as fast as the formation of mussel byssal threads in nature.
A fundamental issue for biomedical applications of graphene is the correlation between its physicochemical properties and cellular uptake mechanism. However, such studies are challenging due to the intrinsic polydispersity of graphene. In this work, a series of water soluble graphene sheets with the same polymer coverage, density of functional groups, and fluorescence intensity but three different sizes and surface charges are produced. The effect of the latter two factors and their combination on the mechanism of cellular uptake and intracellular pathways of these defined nanosheets is investigated via confocal and Raman microscopies. While positively (NH3+) and negatively (OSO3−) charged sheets show an energy dependent uptake, their neutral analogs do not show any significant uptake. The cellular uptake efficacy of positively charged graphene sheets is independent of the size and occurs both through phagocytosis and clathrin‐mediated endocytosis pathways. However, cellular uptake efficacy of graphene sheets with negative surface charge strongly depends on the size of the sheets. They cross the membrane mainly through phagocytosis and sulfate‐receptor‐mediated endocytosis. This study demonstrates that the impact of the size of graphene derivatives on their cellular uptake pathways highly depends on their surface charges and vice versa.
Supramolecular polymerization for non-wetting surface coatings is described. The self-assembly of low-molecular-weight gelators (LMWGs) with perfluorinated side chains can be utilized to rapidly construct superhydrophobic, as well as liquid-infused slippery surfaces within minutes. The lubricated slippery surface exhibits impressive repellency to biological li-quids, such as human serum and blood, and very fast self-healing.
A supramolecular carbohydrate-functionalized two-dimensional (2D) surface was designed and synthesized by decorating thermally reduced graphene sheets with multivalent sugar ligands. The formation of host-guest inclusions on the carbon surface provides a versatile strategy, not only to increase the intrinsic water solubility of graphene-based materials, but more importantly to let the desired biofunctional binding groups bind to the surface. Combining the vital recognition role of carbohydrates and the unique 2D large flexible surface area of the graphene sheets, the addition of multivalent sugar ligands makes the resulting carbon material an excellent platform for selectively wrapping and agglutinating Escherichia coli (E. coli). By taking advantage of the responsive property of supramolecular interactions, the captured bacteria can then be partially released by adding a competitive guest. Compared to previously reported scaffolds, the unique thermal IR-absorption properties of graphene derivatives provide a facile method to kill the captured bacteria by IR-laser irradiation of the captured graphene-sugar-E. coli complex.
Bolaamphiphiles (“bolas”) containing two secondary amide groups at the ends of an oligomethylene chain and two amino acid type headgroups were synthesized. The structures of crystals, of noncovalent fibers, and of surface monolayers on gold strongly depended on odd−even effects. In the crystal structures of alanine−alanine dipeptides with C11- and C12-α,ω-amino acid linkers, helical (even number of methylene groups in the chain) or sheetlike (odd) arrangements of the headgroups were found. Bolas containing two different amino acid end groups, namely, d- or l-alanine and l-lysine, connected by the same C11- and C12 linkers did not crystallize. Only the even-numbered bolas gave fibers. l- and d- configurations of alanine headgroups affected the curvature of the fibers. Diamido bolas with terminal SH-groups self-assembled on gold. Only those with even-numbered chains gave rigid monolayers. Simple stereochemical arguments concerning the fitting of amide hydrogen bond chains on both ends of the bolas are given to explain the observed differences in crystals, fibers, and monolayers.
Abstract. Bone organ culture makes it possible to observe the direct influence of hormones on bone cells. We studied the effect of growth hormone in vitro on embryonal rat tibiae during culture for 7 days, functionally by measuring the levels of alkaline phosphatase in the culture medium, and morphologically by means of semithin sections and electron microscopic examination. Since growth hormone (GH) is supposed to exert an indirect effect on bone cells, somatomedin-C/insulin-like growth factor I (SM-C/IGF I) as a possible mediator was also measured radioimmunologically in the culture medium. In the controls alkaline phosphatase levels showed a continuous increase up to the 7th day which was significantly higher in the presence of GH. There was also a significantly enhanced increase of SM-C/IGF I in the presence of GH during culture in comparison to the controls. Evidently IGF I is produced locally in bone and mediates the effect of GH on bone formation.
A quite simple, achiral benzo-21-crown-7-substituted bis(urea) low-molecular weight gelator hierarchically assembles into helical fibrils, which further develop into bundles and finally form a stable gel in acetonitrile. The gel-sol transition can be controlled by three different molecular recognition events: K + binding to the crown ethers, pseudorotaxane formation with secondary ammonium ions and Cl À binding to the urea units. Addition of a cryptand that scavenges the K + ions and Ag + addition to remove the chloride and bases/acids, which mediate pseudorotaxane formation, can reverse this process. With the gelator, and these chemical stimuli, a number of different systems can be designed that behave as logic gates. Depending on the choice of components, OR, AND, XOR, NOT, NOR, XNOR and INHIBIT gates have been realized. Thus, the gel-sol transition as a property of the system as a whole is influenced in a complex manner. For some cases, the type of logic gate is defined by input signal concentration so that an even more complex reaction of the gel towards the two input signals is achieved.
RNA interference provides great opportunities for treating diseases from genetic disorders, infection, and cancer. The successful application of small interference RNA (siRNA) in cells with high transfection efficiency and low cytotoxicity is, however, a major challenge in gene-mediated therapy. Several pH-responsive core shell architectures have been designed that contain a nitrogen shell motif and a polyglycerol core, which has been prepared by a two-step protocol involving the activation of primary and secondary hydroxyl groups by phenyl chloroformate and amine substitution. Each polymer was analyzed by particle size and ζ potential measurements, whereas the respective polyplex formation was determined by ethidium bromide displacement assay, atomic force microscopy (AFM), and surface charge analysis. The in vitro gene silencing properties of the different polymers were evaluated by using a human epithelial carcinoma cell (HeLaS3) line with different proteins (Lamin, CDC2, MAPK2). Polyplexes yielded similar knockdown efficiencies as HiPerFect controls, with comparably low cytotoxicity. Therefore, these efficient and highly biocompatible dendritic polyamines are promising candidates for siRNA delivery in vivo.
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