Developing complex supramolecular biomaterials through highly dynamic and reversible noncovalent interactions has attracted great attention from the scientific community aiming key biomedical and biotechnological applications, including tissue engineering, regenerative medicine, or drug delivery. In this study, the authors report the fabrication of hybrid supramolecular multilayered biomaterials, comprising high‐molecular‐weight biopolymers and oppositely charged low‐molecular‐weight peptide amphiphiles (PAs), through combination of self‐assembly and electrostatically driven layer‐by‐layer (LbL) assembly approach. Alginate, an anionic polysaccharide, is used to trigger the self‐assembling capability of positively charged PA and formation of 1D nanofiber networks. The LbL technology is further used to fabricate supramolecular multilayered biomaterials by repeating the alternate deposition of both molecules. The fabrication process is monitored by quartz crystal microbalance, revealing that both materials can be successfully combined to conceive stable supramolecular systems. The morphological properties of the systems are studied by advanced microscopy techniques, revealing the nanostructured dimensions and 1D nanofibrous network of the assembly formed by the two molecules. Enhanced C2C12 cell adhesion, proliferation, and differentiation are observed on nanostructures having PA as outermost layer. Such supramolecular biomaterials demonstrate to be innovative matrices for cell culture and hold great potential to be used in the near future as promising biomimetic supramolecular nanoplatforms for practical applications.
Bioinspired and adhesive multilayer membranes are produced using the layer-by-layer (LbL) assembly of chitosan (CHT), alginate (ALG) and hyaluronic acid modified with dopamine (HA-DN). Freestanding multilayer membranes without DN are also produced as a control. The success of the synthesis of HA-DN was confirmed using UV-visible spectroscopy. Scanning electron microscopy images indicate that the surface of the DN-containing membranes is more porous than the control ones; they also present a higher average thickness value for the same number of CHT/ALG/CHT/HA(-DN) tetralayers (n = 100). Also, water uptake, mechanical strength and adhesion are enhanced with the introduction of DN moieties along the nano-layers. Besides, human dermal fibroblast viability, enhanced adhesion and proliferation were confirmed by immunofluorescence assays and by measuring both the metabolic activity and DNA content. Moreover, in vivo assays with such kinds of DN-containing multilayer membranes were performed; the application of these membranes in the treatment of dermal wounds induced in Wistar rats results in the highest decrease of inflammation of rat skin, compared with the control conditions. Overall, this investigation suggests that these mussel-inspired freestanding multilayer membranes may enhance either their mechanical performance or cellular adhesion and proliferation, leading to an improved wound healing process, being a promising material to restore the structural and functional properties of wounded skin.
In this study, thin LbL films were produced by combining the adhesive properties of the hyaluronic acid–dopamine conjugate with the bioactivity and bactericidal properties of silver doped bioactive glass nanoparticles.
This work outlines inexpensive patterning methodologies to create open-air microfluidic paperbased devices. A phase-separation methodology was used to obtain biomimetic superhydrophobic paper, hierarchically composed by micro and nano topographies. Writing and printing are simple actions that can be used to pattern flat superhydrophobic paper with more wettable channels. In particular, inkjet printing permits controlling the wettability of the surface by changing the darkness of the printed regions. The difference between capillary forces provides the possibility to control and drive liquid flows through the open path lines, just by titling the piece of paper. Additionally, maintaining a continuous flow, it is possible to direct the liquid at different volumetric rates in a horizontal position along non-linear channel paths printed/written over the surface.
Extracellular matrix (ECM) cues have been widely investigated for their impact on cellular behavior. Among mechanics, physics, chemistry, and topography, different ECM properties have been discovered as important parameters to modulate cell functions, activating mechanotransduction pathways that can influence gene expression, proliferation or even differentiation. Particularly, ECM topography has been gaining more and more interest based on the evidence that these physical cues can tailor cell behavior. Here, an overview of bottom‐up and top‐down approaches reported to produce materials capable of mimicking the ECM topography and being applied for biomedical purposes is provided. Moreover, the increasing motivation of using the layer‐by‐layer (LbL) technique to reproduce these topographical cues is highlighted. LbL assembly is a versatile methodology used to coat materials with a nanoscale fidelity to the geometry of the template or to produce multilayer thin films composed of polymers, proteins, colloids, or even cells. Different geometries, sizes, or shapes on surface topography can imply different behaviors: effects on the cell adhesion, proliferation, morphology, alignment, migration, gene expression, and even differentiation are considered. Finally, the importance of LbL assembly to produce defined topographical cues on materials is discussed, highlighting the potential of micro‐ and nanoengineered materials to modulate cell function and fate.
Traditionally in superhydrophobic surfaces history, the focus has frequently settled on the use of complex processing methodologies using nonbiodegradable and costly materials. In light of recent events on lab-on-paper emergence, there are now some efforts for the production of superhydrophobic paper but still with little development and confined to the fabrication of flat devices. This work gives a new look at the range of possible applications of bioinspired superhydrophobic paper-based substrates, obtained using a straightforward surface modification with poly-(hydroxybutyrate). As an end-of-proof of the possibility to create lab-on-chip portable devices, the patterning of superhydrophobic paper with different wettable shapes is shown with low-cost approaches. Furthermore, we suggest the use of superhydrophobic paper as an extremely low-cost material to design essential nonplanar lab apparatus, including reservoirs for liquid storage and manipulation, funnels, tips for pipettes, or accordion-shaped substrates for liquid transport or mixing. Such devices take the advantage of the self-cleaning and extremely water resistance properties of the surfaces as well as the actions that may be done with paper such as cut, glue, write, fold, warp, or burn. The obtained substrates showed lower propensity to adsorb proteins than the original paper, kept superhydrophobic character upon ethylene oxide sterilization and are disposable, suggesting that the developing devices could be especially adequate for use in contact with biological and hazardous materials.
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