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A full understanding of the relationship between surface properties, protein adsorption, and immune responses is lacking but is of great interest for the design of biomaterials with desired biological profiles. In this study, polyelectrolyte multilayer (PEM) coatings with gradient changes in surface wettability were developed to shed light on how this impacts protein adsorption and immune response in the context of material biocompatibility. The analysis of immune responses by peripheral blood mononuclear cells to PEM coatings revealed an increased expression of proinflammatory cytokines tumor necrosis factor (TNF)-α, macrophage inflammatory protein (MIP)-1β, monocyte chemoattractant protein (MCP)-1, and interleukin (IL)-6 and the surface marker CD86 in response to the most hydrophobic coating, whereas the most hydrophilic coating resulted in a comparatively mild immune response. These findings were subsequently confirmed in a cohort of 24 donors. Cytokines were produced predominantly by monocytes with a peak after 24 h. Experiments conducted in the absence of serum indicated a contributing role of the adsorbed protein layer in the observed immune response. Mass spectrometry analysis revealed distinct protein adsorption patterns, with more inflammation-related proteins (e.g., apolipoprotein A-II) present on the most hydrophobic PEM surface, while the most abundant protein on the hydrophilic PEM (apolipoprotein A-I) was related to anti-inflammatory roles. The pathway analysis revealed alterations in the mitogen-activated protein kinase (MAPK)-signaling pathway between the most hydrophilic and the most hydrophobic coating. The results show that the acute proinflammatory response to the more hydrophobic PEM surface is associated with the adsorption of inflammation-related proteins. Thus, this study provides insights into the interplay between material wettability, protein adsorption, and inflammatory response and may act as a basis for the rational design of biomaterials.
The present publication reports the purification effort of two natural bone blocks, that is, an allogeneic bone block (maxgraft®, botiss biomaterials GmbH, Zossen, Germany) and a xenogeneic block (SMARTBONE®, IBI S.A., Mezzovico Vira, Switzerland) in addition to previously published results based on histology. Furthermore, specialized scanning electron microscopy (SEM) and in vitro analyses (XTT, BrdU, LDH) for testing of the cytocompatibility based on ISO 10993-5/-12 have been conducted. The microscopic analyses showed that both bone blocks possess a trabecular structure with a lamellar subarrangement. In the case of the xenogeneic bone block, only minor remnants of collagenous structures were found, while in contrast high amounts of collagen were found associated with the allogeneic bone matrix. Furthermore, only island-like remnants of the polymer coating in case of the xenogeneic bone substitute seemed to be detectable. Finally, no remaining cells or cellular remnants were found in both bone blocks. The in vitro analyses showed that both bone blocks are biocompatible. Altogether, the purification level of both bone blocks seems to be favorable for bone tissue regeneration without the risk for inflammatory responses or graft rejection. Moreover, the analysis of the maxgraft® bone block showed that the underlying purification process allows for preserving not only the calcified bone matrix but also high amounts of the intertrabecular collagen matrix.
Despite its success against cancer, photothermal therapy (PTT) (>50 °C) suffers from several limitations such as triggering inflammation and facilitating immune escape and metastasis and also damage to the surrounding normal cells. Mild-temperature PTT has been proposed to override these shortcomings. We developed a nanosystem using HepG2 cancer cell membrane-cloaked zinc glutamate-modified Prussian blue nanoparticles with triphenylphosphine-conjugated lonidamine (HmPGTL NPs). This innovative approach achieved an efficient mild-temperature PTT effect by downregulating the production of intracellular ATP. This disrupts a section of heat shock proteins that cushion cancer cells against heat. The physicochemical properties, anti-tumor efficacy, and mechanisms of HmPGTL NPs both in vitro and in vivo were investigated. Moreover, the nanoparticles cloaked with the HepG2 cell membrane substantially prolonged the circulation time in vivo. Overall, the designed nanocomposites enhance the efficacy of mild-temperature PTT by disrupting the production of ATP in cancer cells. Thus, we anticipate that the mild-temperature PTT nanosystem will certainly present its enormous potential in various biomedical applications.
Background/Aim: The aim of this study was the development of a new osteoconductivity index to determine the bone healing capacities of bone substitute materials (BSM) on the basis of 3D microcomputed tomographic (μ-CT) data. Materials and Methods: Sinus biopsies were used for the comparative analysis of the integration behavior of two xenogeneic BSM (cerabone® and Bio Oss®). 3D μ-CT and data sets from histomorphometrical measurements based on 2D histological slices were used to measure the bone-material-contact and the tissue distribution within the biopsies. The tissue reactions to both BSM were microscopically analyzed. Results: The 3D and 2D results of the osteoconductivity measurements showed comparable material-bone contacts for both BSM, but the 2D data were significantly lower. The same results were found when tissue distribution was measured in both groups. The histopathological analysis showed comparative tissue reactions in both BSM. Conclusion: Osteoconductivity index is a reliable measurement parameter for determining the healing capacities of BSM. The observed differences between both measurement methods could be assigned to the resolution capacity of μ-CT data that did not allow for a precise interface distinction between both BSM and bone tissue. Histomorphometrical data based on histological slides still allow for a more exact evaluation.
Polyelectrolyte multilayer coatings (PEM) are prepared by alternative layer-by-layer deposition of cationic and anionic polyelectrolyte monolayers on charged surfaces. The thickness of the coatings ranges from nm to few μm. Their properties such as roughness, stiffness, surface charge and surface energy can be precisely tuned to fulfil different technical or biological requirements. The coating process is based on self-assembly of polyelectrolytes. Advantages of these coatings are their easy handling, no harsh chemistry and the possibility for coatings on complex geometries. The PEM coatings can be prepared from a variety of suitable polyelectrolytes. Their stability varies from very durable PEM coatings that are only soluble in strong solvents to quickly degradable, which may be applied as drug release system. One example of such a degradable PEM system is the one based on the polyelectrolyte pair Hyaluronan (HA) and Chitosan (CHI). These biopolymers originate from natural sources and show low toxicity towards human cells. However, HA/CHI multilayers show only weak adhesiveness for human umbilical vein endothelial cells (HUVEC). In this article, we summarize our approaches to enhance the HA/CHI multilayer by incorporation of a non-polymer substance –graphene oxide– to improve the cell adhesion and keep such properties as low cytotoxicity and biodegradability. Different approaches for incorporation of graphene oxide were performed and the cellular adhesion was tested by metabolic assay.
Controlled adhesion of HUVEC on polyelectrolyte multilayers by regulation of coating conditions
(2021)
Adhesion of host cells on the surface of implants is necessary for a healthy ingrowth of the implanted material. One possibility of surface modification is the coating of the implant with a second material with advantageous physical–chemical surface properties for the biological system. The coverage with blood proteins takes place immediately after implantation. It is followed by host–cell interaction on the surface. In this work, the effect of polyelectrolyte multilayer coatings (PEMs) on adhesion and activity of human umbilical vein endothelial cells (HUVECs) was studied. The PEMs were formed from poly(styrenesulfonate) (PSS) and poly(allylamine hydrochloride) (PAH) from solutions with different concentrations of NaCl varying between 0 and 1.0 M. The adhesion of HUVEC and their viability on the PEM is related to the amount of adsorbed proteins from the applied cell growth medium. The amount of adsorbed proteins is controlled not only by the surface charge but also by the internal excess charge of the PEM. The internal excess charge of the PEM was controlled by changing the electrolyte concentration in the deposition solutions.
Surface topographies are often discussed as an important parameter influencing basic cell behavior. Whereas most in vitro studies deal with microstructures with sharp edges, smooth, curved microscale topographies might be more relevant concerning in-vivo situations. Addressing the lack of highly defined surfaces with varying curvature, we present a topography chip system with 3D curved features of varying spacing, curvature radii as well as varying overall dimensions of curved surfaces. The CurvChip is produced by low-cost photolithography with thermal reflow, subsequent (repetitive) PDMS molding and hot embossing. The platform facilitates the systematic in-vitro investigation of the impact of substrate curvature on cell types like epithelial, endothelial, smooth muscle cells, or stem cells. Such investigations will not only help to further understand the mechanism of curvature sensation but may also contribute to optimize cell-material interactions in the field of regenerative medicine.
Introduction: Bioresorbable collagenous barrier membranes are used to prevent premature soft tissue ingrowth and to allow bone regeneration. For volume stable indications, only non-absorbable synthetic materials are available. This study investigates a new bioresorbable hydrofluoric acid (HF)-treated magnesium (Mg) mesh in a native collagen membrane for volume stable situations. Materials and Methods: HF-treated and untreated Mg were compared in direct and indirect cytocompatibility assays. In vivo, 18 New Zealand White Rabbits received each four 8 mm calvarial defects and were divided into four groups: (a) HF-treated Mg mesh/collagen membrane, (b) untreated Mg mesh/collagen membrane (c) collagen membrane and (d) sham operation. After 6, 12 and 18 weeks, Mg degradation and bone regeneration was measured using radiological and histological methods. Results: In vitro, HF-treated Mg showed higher cytocompatibility. Histopathologically, HF-Mg prevented gas cavities and was degraded by mononuclear cells via phagocytosis up to 12 weeks. Untreated Mg showed partially significant more gas cavities and a fibrous tissue reaction. Bone regeneration was not significantly different between all groups. Discussion and Conclusions: HF-Mg meshes embedded in native collagen membranes represent a volume stable and biocompatible alternative to the non-absorbable synthetic materials. HF-Mg shows less corrosion and is degraded by phagocytosis. However, the application of membranes did not result in higher bone regeneration.
In this study, a novel strategy has been developed for the assembly of polyelectrolyte multilayer (PEM) on CaCO3 templates in acidic pH solutions, where consecutive polyelectrolyte layers (heparin/poly(allylamine hydrochloride) or heparin/chitosan) were deposited on PEM hollow microcapsules established previously on CaCO3 templates. The PEM build-up, hollow capsule characterization and successful encapsulation of fluorescein 5(6)-isothiocyanate (FITC)-Dextran by coprecipitation with CaCO3 are demonstrated. Improvement by the removal of CaCO3 core was achieved while the depositions. In the course of the release profile, high retardation for encapsulated FITC-Dextran was observed. The combined shell capsules system is a significant trait that has potential use in tailoring functional layer-by-layer capsules as intelligent drug delivery vehicles where the preliminary in vitro tests showed the responsiveness on the enzymes.
In this article, liposome-based coatings aiming to control drug release from therapeutic soft contact lenses (SCLs) materials are analyzed. A PHEMA based hydrogel material loaded with levofloxacin is used as model system for this research. The coatings are formed by polyelectrolyte layers containing liposomes of 1,2-dimyristoyl-sn-glycero-3- phosphocholine (DMPC) and DMPC1cholesterol (DMPC1 CHOL). The effect of friction and temperature on the drug release is investigated. The aim of the friction tests is to simulate the blinking of the eyelid in order to verify if the SCLs materials coated with liposomes are able to keep their properties, in particular the drug release ability. It was observed that under the study conditions, friction did not affect significantly the drug release from the liposome coated PHEMA material. In contrast, increasing the temperature of release leads to an increase of the drug diffusion rate through the hydrogel. This phenomenon is recorded both in the control and in the coated samples.
Polyelectrolyte multilayer (PEM) are thin polymeric films produced by alternating adsorption of positively and negatively charged polyelectrolytes (PE) on a substrate. These films are considered drug delivery agents as well as coating material for implants, due to their antibiofouling and biologically benign properties. For these reasons the film mechanical properties as well as response to mechanical stress are important measurement parameters. Especially intriguing is the correlation of the mechanical properties of PEM on macroscopic level with the structure of PEM on molecular level, which is addressed here for the first time. This study investigates PEM from PDADMA/PSS produced by spraying technique with neutron and X-ray reflectometry. Reflectometry technique provides precise information on thickness and density (i.e., electron density or scattering length density, respectively), and, this way, allows to conclude on changes in film composition. Thus, neutron and X-ray reflectometry technique is suitable to investigate the overall and the internal transformations, which PEM films might undergo upon exposure to mechanical load. During uniaxial elongation two regimes of PEM deformation can be observed: An elastic regime at small elongations (below ca. 0.2%), which is characterized by a reversible change of film thickness, and a plastic regime with a permanent change above this limit. Both regimes have in common, that the mechanical load induces an increase of the film thickness, which is accompanied by an uptake of water from the surrounding atmosphere. The strain causes a molecular rearrangement within the PEM-structure of stratified layers, which, even in elastic regime, is permanent, although the thickness change remains reversible.
Hypothesis
The origin of negative surface charge at water/air interface is still not clear. The most probable origin is specific adsorption of OH− ions. From diffuse layer potential, we can evaluate the surface density of ions in the Stern layer which can be a measure for the specific adsorption of ions and determines whether the surface charge is solely due to the specific adsorption of OH− ions.
Experiments
Equilibrium thickness of foam films of pure water and aqueous solutions of NaCl, HCl, and NaOH was measured as a function of disjoining pressure for water and as a function of concentration for the aqueous solutions at 298.15 K. Quartz-glass cells thoroughly cleaned and immersed in pure water before use were used for the measurement.
Findings
Application of a modified Poisson-Boltzmann equation to the equilibrium film thickness gave the diffuse layer potential and the surface density of ions in the Stern layer. From the concentration dependence of the surface density, it was concluded that not only OH− ions but also Cl− ions and HCO3− and/or CO32− ions adsorb specifically at the water/air interface.
Medical implants play a central role in modern medicine and both, naturally derived and synthetic materials have been explored as biomaterials for such devices. However, when implanted into living tissue, most materials initiate a host response. In addition, implants often cause bacterial infections leading to complications. Polyelectrolyte multilayer (PEM) coatings can be used for functionalization of medical implants improving the implant integration and reducing foreign body reactions. Some PEMs are also known to show antibacterial properties. We developed a PEM coating suggesting that it can decrease the risk of bacterial infections occurring after implantation while being highly biocompatible. We applied two different standard tests for evaluating the PEM’s antibacterial properties, the ISO norm (ISO 22196) and one ASTM norm (ASTM E2180) test. We found a reduction of bacterial growth on the PEM but to a different degree depending on the testing method. This result demonstrates the need for defining proper method to evaluate antibacterial properties of surface coatings.
Polyethylene glycol (PEG) is a widely used modification for drug delivery systems. It reduces undesired interaction with biological components, aggregation of complexes and serves as a hydrophilic linker of ligands for targeted drug delivery. However, PEGylation can also lead to undesired changes in physicochemical characteristics of chitosan/siRNA nanoplexes and hamper gene silencing.
To address this conflicting issue, PEG-chitosan copolymers were synthesized with stepwise increasing degrees of PEG substitution (1.5% to 8.0%). Subsequently formed PEG-chitosan/siRNA nanoplexes were characterized physicochemically and biologically. The results showed that small ratios of chitosan PEGylation did not affect nanoplex stability and density. However, higher PEGylation ratios reduced nanoplex size and charge, as well as cell uptake and final siRNA knockdown efficiency.
Therefore, we recommend fine-tuning of PEGylation ratios to generate PEG-chitosan/siRNA delivery systems with maximum bioactivity. The degree of PEGylation for chitosan/siRNA nanoplexes should be kept low in order to maintain optimal nanoplex efficiency.
Foam has been employed as an improved or enhanced oil recovery method to overcome gravity override and the channeling and fingering of the injected gas, which arises because of the low density and viscosity of the injected fluid combined with the rock heterogeneity. A major challenge, however, is the stability of the generated foam when it contacts the oil. In this study we investigate the feasibility of using inexpensive nanoparticles made of coal fly ash, an abundantly available waste product of coal power plants, as a foam booster. We investigate the viability of reducing the size of fly ash particles to 100−200 nm using high-frequency ultrasonic grinding. We also study the foaminess (foamability), strength, and stability of the foams made with minor concentrations of fly ash nanoparticles and surfactant, both in bulk and porous media. The effect of monovalent and divalent ion concentration on the foaminess of the nanoash suspension combined with very low concentrations of a commercial alpha olefin sulfonate (AOS) surfactant, in the presence and absence of oil, is studied. We observe that bulk foam that contains very small amounts of nanoash particles shows a higher stability in the presence of model oils. Furthermore, experiments in porous media exhibit remarkably stronger foam with mixtures of nanoash and surfactant, such that the amount of produced liquids from the cores significantly increases. For the first time we show that nanoash can be used to stabilize nitrogen foam in the presence of crude oil at high temperature and pressure. In the presence of oil, the nanoash−AOS foam shows a higher stability, although crude oil tends to form stable emulsions in water in the presence of nanoash.
At the beginning of 2022, Frontiers in Bioengineering and Biotechnology - Biomaterials Section has published a Research Topic on “Functional Surfaces and Biomaterials.” The aim of this Research Topic is to summarize the current state of research and development in the field of functional surfaces and biomaterials with a particular focus on biotechnological and medical applications.
The guest editorial team would like to thank all colleagues from around the world who submitted their reviews and research articles for the Research Topic. By the end of August 2022, we have successfully collected 20 articles by 138 participating authors following the peer review process. We also tried to select manuscripts from different research areas to cover the most relevant Research Topic of interest, from drug delivery systems to bone tissue engineering to biosensors and general aspects in biomedicine. By the end of December, the 20 articles had been viewed for more than 21000 times with downloads more than 4,000 times, and 11 articles have reached more than 1,000 views.
High moisture permeability, excellent mechanical properties in a wet state, high water-holding capability, and high exudate absorption make bacterial nanocellulose (BNC) a favorable candidate for biomedical device production, especially wound dressings. The lack of antibacterial activity and healing-promoting ability are the main drawbacks that limit its wide application. Pullulan (Pul) is a nontoxic polymer that can promote wound healing. Zinc oxide nanoparticles (ZnO-NPs) are well-known as a safe antibacterial agent. In this study, aminoalkylsilane was chemically grafted on a BNC membrane (A-g-BNC) and used as a bridge to combine BNC with Pul-ZnO-NPs hybrid electrospun nanofibers. FTIR results confirmed the successful production of A-g-BNC/Pul-ZnO. The obtained dressing demonstrated blood clotting performance better than that of BNC. The dressing showed an ability to release ZnO, and its antibacterial activity was up to 5 log values higher than that of BNC. The cytotoxicity of the dressing toward L929 fibroblast cells clearly showed safety due to the proliferation of fibroblast cells. The animal test in a rat model indicated faster healing and re-epithelialization, small blood vessel formation, and collagen synthesis in the wounds covered by A-g-BNC/Pul-ZnO. The new functional dressing, fabricated with a cost-effective and easy method, not only showed excellent antibacterial activity but could also accelerate wound healing.
The effect of Hofmeister anions on the surface properties of polyelectrolyte multilayers built from hyaluronan and chitosan by layer-by-layer deposition is studied by ellipsometry and atomic force microscopy. The thickness, roughness and morphology of the resulting coatings were found to depend on the type of the anion. Relationship between the surface properties and the biological response of the polyelectrolyte multilayers is established by assessing the degree of protein (albumin) adsorption.
Concrete is significant for construction. A problem in application is the appearance of cracks that will damage its strength. An autogenous crack-healing mechanism based on bacteria receives increasing attention in recent years. The bacteria are able to form calcium carbonate (CaCO3) precipitations in suitable conditions to protect and reinforce the concrete. However, a large number of spores are crushed in aged specimens, resulting in a loss of viability. A new kind of hydrogel crosslinked by alginate, chitosan and calcium ions was introduced in this study. It was observed that the addition of chitosan improved the swelling properties of calcium alginate. Opposite pH response to calcium alginate was observed when the chitosan content in the solution reached 1.0%. With an addition of 1.0% chitosan in hydrogel beads, 10.28% increase of compressive strength and 13.79% increase of flexural strength to the control were observed. The results reveal self-healing properties of concretes. A healing crack of 4 cm length and 1 mm width was observed when using cement PO325, with the addition of bacterial spores (2.54–3.07 × 105/cm3 concrete) encapsulated by hydrogel containing no chitosan.
Papermaking waste liquid (black liquor) is a serious source of water pollution worldwide. The subsequent treatment of it is very difficult cause it contains a large amount of lignin, inorganic salts, organic matter, and pigments, which lead to serious water pollution. Lignin is the main by-product of the paper industry and is the only natural aromatic recyclable resource. Its effective utilization rate is currently less than 3%. Therefore, how to effectively recycle lignin in papermaking waste liquid and further synthesize industrialized products is of great significance to the sustainable development and environmental protection. Besides, based on the shortage of petroleum resources in recent years, the application of biomass resources instead of petroleum resources in the industry is also an important issue. In this article, we explored the best optimal conditions for the oxypropylation and esterification of lignin, and prepared bio-bitumen based on modified lignin, and then applied it to the waterproof coating sheets. FTIR and mechanical properties (softening point, low-temperature flexibility, peel strength, etc.) were tested on the obtained waterproof coating sheets. The results show that the addition of modified lignin reduced the softening point and peel strength of the coating sheets. Interestingly, both oxypropylated lignin (OL) and esterified lignin (OEL) were very beneficial to resist the decrease in peel strength during the aging process, showing a significant improvement in the performance of the coating sheets after aging compared to the control.