Durable, Photostable Omniphobic Synthetic Leather Surfaces with Anti-Biofouling Properties for Hygienic Applications.

Globally, the public health domain is increasingly emphasizing the need for surfaces that can resist bacterial contamination, as the consumption of bacteria-infected substance may cause illnesses. Thus, this study aimed to modify polyurethane (PU) synthetic leather surfaces by coating their upper layer with fluorine-functionalized nano-silica particles (FNPs). This simple modification imparted omniphobic characteristics, realizing anti-biofouling and self-cleaning properties. The effectiveness in preventing bacterial adhesion was confirmed by the dip-inoculation method using Escherichia coli O157:H7 and Staphylococcus epidermidis. Bacterial adhesion was evaluated based on bacterial counts using the pour plate method and by directly enumerating from scanning electron microscopy images. The attachment of bacteria to the modified omniphobic FNPs-coated PU leather surface decreased by over 98.2% compared to that on the bare surface. We expect that the method developed in this study will significantly reduce or even eliminate the potential risks associated with various biological cross-contamination scenarios, thereby enhancing hygiene standards.

Durable Surface Modification of Low-Density Polyethylene/Nano-Silica Composite Films with Bacterial Antifouling and Liquid-Repelling Properties for Food Hygiene and Safety.

The growing prevalence of antimicrobial resistance in bacterial strains has increased the demand for preventing biological deterioration on the surfaces of films used in applications involving food contact materials (FCMs). Herein, we prepared superhydrophobic film surfaces using a casting process that involved the combination of low-density polyethylene (LDPE) with solutions containing surface energy-reducing silica (SRS). The bacterial antifouling properties of the modified film surfaces were evaluated using Escherichia coli O157:H7 and Staphylococcus epidermidis via the dip-inoculation technique. The reduction in bacterial populations on the LDPE film embedded with SRS was confirmed to be more than 2 log-units, which equates to over 99%, when compared to the bare LDPE film. Additionally, the modified film demonstrated liquid-repelling properties against food-related contaminants, such as blood, beverages, and sauces. Moreover, the modified film demonstrated enhanced durability and robustness compared to one of the prevalent industry methods, dip-coating. We anticipate that the developed LDPE/nano-silica composite film represents a promising advancement in the multidisciplinary aspects of food hygiene and safety within the food industry, particularly concerning FCMs.

Silica Nanoparticle-Infused Omniphobic Polyurethane Foam with Bacterial Anti-Adhesion and Antifouling Properties for Hygiene Purposes.

In this study, a method for preventing cross-infection through the surface coating treatment of polyurethane (PU) foam using functionalized silica nanoparticles was developed. Experimental results confirmed that the fabricated PU foam exhibited omniphobic characteristics, demonstrating strong resistance to both polar and nonpolar contaminants. Additionally, quantitative analysis using the pour plate method and direct counting with a scanning electron microscope determined that the treated material exhibited anti-adhesion properties against bacteria. The fabricated PU foam also demonstrated a high level of resistance to the absorption of liquids commonly found in medical facilities, including blood, 0.9% sodium chloride solution, and 50% glycerol. Mechanical durability and stability were verified through repeated compression tests and chemical leaching tests, respectively. The proposed coated PU foam is highly effective at preventing fouling from polar and nonpolar fluids as well as bacteria, making it well-suited for use in a range of fields requiring strict hygiene standards, including the medical, food, and environmental industries.

Influence of Surface Roughness, Nanostructure, and Wetting on Bacterial Adhesion.

Bacterial fouling is a persistent problem causing the deterioration and failure of functional surfaces for industrial equipment/components; numerous human, animal, and plant infections/diseases; and energy waste due to the inefficiencies at internal and external geometries of transport systems. This work gains new insights into the effect of surface roughness on bacterial fouling by systematically studying bacterial adhesion on model hydrophobic (methyl-terminated) surfaces with roughness scales spanning from ∼2 nm to ∼390 nm. Additionally, a surface energy integration framework is developed to elucidate the role of surface roughness on the energetics of bacteria and substrate interactions. For a given bacteria type and surface chemistry; the extent of bacterial fouling was found to demonstrate up to a 75-fold variation with surface roughness. For the cases showing hydrophobic wetting behavior, both increased effective surface area with increasing roughness and decreased activation energy with increased surface roughness was concluded to enhance the extent of bacterial adhesion. For the cases of superhydrophobic surfaces, the combination of factors including (i) the surpassing of Laplace pressure force of interstitial air over bacterial adhesive force, (ii) the reduced effective substrate area for bacteria wall due to air gaps to have direct/solid contact, and (iii) the reduction of attractive van der Waals force that holds adhering bacteria on the substrate were summarized to weaken the bacterial adhesion. Overall, this study is significant in the context of designing antifouling coatings and systems as well as explaining variations in bacterial contamination and biofilm formation processes on functional surfaces.

Gold-Nanoparticle-Coated Magnetic Beads for ALP-Enzyme-Based Electrochemical Immunosensing in Human Plasma.

A simple and sensitive AuNP-coated magnetic beads (AMB)-based electrochemical biosensor platform was fabricated for bioassay. In this study, AuNP-conjugated magnetic particles were successfully prepared using biotin-streptavidin conjugation. The morphology and structure of the nanocomplex were characterized by scanning electron microscopy (SEM) with energy-dispersive X-ray analysis (EDX) and UV-visible spectroscopy. Moreover, cyclic voltammetry (CV) was used to investigate the effect of AuNP-MB on alkaline phosphatase (ALP) for electrochemical signal enhancement. An ALP-based electrochemical (EC) immunoassay was performed on the developed AuNP-MB complex with indium tin oxide (ITO) electrodes. Subsequently, the concentration of capture antibodies was well-optimized on the AMB complex via biotin-avidin conjugation. Lastly, the developed AuNP-MB immunoassay platform was verified with extracellular vesicle (EV) detection via immune response by showing the existence of EGFR proteins on glioblastoma multiforme (GBM)-derived EVs (108 particle/mL) spiked in human plasma. Therefore, the signal-enhanced ALP-based EC biosensor on AuNP-MB was favorably utilized as an immunoassay platform, revealing the potential application of biosensors in immunoassays in biological environments.

Enhanced Chemical and Electrochemical Stability of Polyaniline-Based Layer-by-Layer Films.

Polyaniline (PANI) has been widely used as an electroactive material in various applications including sensors, electrochromic devices, solar cells, electroluminescence, and electrochemical energy storage, owing to PANI's unique redox properties. However, the chemical and electrochemical stability of PANI-based materials is not sufficiently high to maintain the performance of devices under many practical applications. Herein, we report a route to enhancing the chemical and electrochemical stability of PANI through layer-by-layer (LbL) assembly. PANI was assembled with different types of polyelectrolytes, and a comparative study between three different PANI-based layer-by-layer (LbL) films is presented here. Polyacids of different acidity and molecular structure, i.e., poly(acrylic acid) (PAA), polystyrene sulfonate (PSS), and tannic acid (TA), were used. The effect of polyacids' acidity on film growth, conductivity, and chemical and electrochemical stability of PANI was investigated. The results showed that the film growth of the LbL system depended on the acidic strength of the polyacids. All LbL films exhibited improved chemical and electrochemical stability compared to PANI films. The doping level of PANI was strongly affected by the type of dopants, resulting in different chemical and electrochemical properties; the strongest polyacid (PSS) can provide the highest conductivity and chemical stability of conductive PANI. However, the electrochemical stability of PANI/PAA was found to be better than all the other films.

Nanotoxicity of 2D Molybdenum Disulfide, MoS2, Nanosheets on Beneficial Soil Bacteria, Bacillus cereus and Pseudomonas aeruginosa.

Concerns arising from accidental and occasional releases of novel industrial nanomaterials to the environment and waterbodies are rapidly increasing as the production and utilization levels of nanomaterials increase every day. In particular, two-dimensional nanosheets are one of the most significant emerging classes of nanomaterials used or considered for use in numerous applications and devices. This study deals with the interactions between 2D molybdenum disulfide (MoS2) nanosheets and beneficial soil bacteria. It was found that the log-reduction in the survival of Gram-positive Bacillus cereus was 2.8 (99.83%) and 4.9 (99.9988%) upon exposure to 16.0 mg/mL bulk MoS2 (macroscale) and 2D MoS2 nanosheets (nanoscale), respectively. For the case of Gram-negative Pseudomonas aeruginosa, the log-reduction values in bacterial survival were 1.9 (98.60%) and 5.4 (99.9996%) for the same concentration of bulk MoS2 and MoS2 nanosheets, respectively. Based on these findings, it is important to consider the potential toxicity of MoS2 nanosheets on beneficial soil bacteria responsible for nitrate reduction and nitrogen fixation, soil formation, decomposition of dead and decayed natural materials, and transformation of toxic compounds into nontoxic compounds to adequately assess the environmental impact of 2D nanosheets and nanomaterials.

Bacterial Antifouling Characteristics of Helicene-Graphene Films.

Herein, we describe interfacially-assembled [7]helicene films that were deposited on graphene monolayer using the Langmuir-Schaefer deposition by utilizing the interactions of nonplanar (helicene) and planar (graphene) π-π interactions as functional antifouling coatings. Bacterial adhesion of Staphylococcus aureus on helicene-graphene films was noticeably lower than that on bare graphene, up to 96.8% reductions in bacterial adhesion. The promising bacterial antifouling characteristics of helicene films was attributed to the unique molecular geometry of helicene, i.e., nano-helix, which can hinder the nanoscale bacterial docking processes on a surface. We envision that helicene-graphene films may eventually be used as protective coatings against bacterial antifouling on the electronic components of clinical and biomedical devices.

Dual-Functional, Superhydrophobic Coatings with Bacterial Anticontact and Antimicrobial Characteristics.

Bacterial pathogens are responsible for millions of cases of illnesses and deaths each year throughout the world. The development of novel surfaces and coatings that effectively inhibit and prevent bacterial attachment, proliferation, and growth is one of the crucial steps for tackling this global challenge. Herein, we report a dual-functional coating for aluminum surfaces that relies on the controlled immobilization of lysozyme enzyme (muramidase) into interstitial spaces of presintered, nanostructured thin film based on ∼200 nm silica nanoparticles and the sequential chemisorption of an organofluorosilane to the available interfacial areas. The mean diameter of the resultant lysozyme microdomains was 3.1 ± 2.5 µm with an average spacing of 8.01 ± 6.8 µm, leading to a surface coverage of 15.32%. The coating had an overall root-mean-square (rms) roughness of 539 ± 137 nm and roughness factor of 1.50 ± 0.1, and demonstrated static, advancing, and receding water contact angles of 159.0 ± 1.0°, 155.4 ± 0.6°, and 154.4 ± 0.6°, respectively. Compared to the planar aluminum, the coated surfaces produced a 6.5 ± 0.1 (>99.99997%) and 4.0 ± 0.1 (>99.99%) log-cycle reductions in bacterial surfaces colonization against Gram-negative Salmonella Typhimurium LT2 and Gram-positive Listeria innocua, respectively. We anticipate that the implementation of such a coating strategy on healthcare environments and surfaces and food-contact surfaces can significantly reduce or eliminate potential risks associated with various contamination and cross-contamination scenarios.

Antimicrobial Activities of Thermoplastic Polyurethane/Clay Nanocomposites against Pathogenic Bacteria.

As a thermoplastic polymer with an impressive combination of mechanical properties and biological compatibility, thermoplastic polyurethane (TPU) is one of the important polymers used in various applications such as biomaterials, conducting materials, and tissue engineering. Nanocomposites made of TPUs with nanoclays were prepared by melt-compounding, and the effects of clay on antibacterial activities and physical properties of nanocomposites were investigated. X-ray powder diffraction, water contact angle, and TEM results were analyzed to investigate the effects of dispersion and modification of clays in TPU/clay nanocomposites. Using the pour plating method, scanning electron microscopy technique, and disk diffusion test, TPU/clay nanocomposites were observed to show contact killing activity against bacteria. The antibacterial activities of TPU/clay nanocomposites were found to be affected by the dispersion state and amount of organic modifier of clays. TPU nanocomposites containing 5 wt % organically modified clay showed 98.5% killing efficiency against Gram-negative Escherichia coli and 99.9% against Gram-positive Staphylococcus aureus, while neat TPU showed almost none. The positively charged quaternary ammonium salt groups of clay in TPU/clay nanocomposites interacted with the negatively charged cytoplasmic membrane of bacteria, and the dead bacteria were eliminated by weakened adhesion on hydrophobic backbone surfaces.

Spontaneous Nanobelt Formation by Self-Assembly of ß-Benzyl GABA.

We present the formation of a nanobelt by self-assembly of ß-benzyl GABA (γ-aminobutyric acid). This simple γ-amino acid building block self-assembled to form a well-defined nanobelt in chloroform. The nanobelt showed distinct optical properties due to π-π interactions. This new-generation self-assembled single amino acid may serve as a template for functional nanomaterials.

The influence of surface chemistry on the kinetics and thermodynamics of bacterial adhesion.

This work is concerned with investigating the effect of substrate hydrophobicity and zeta potential on the dynamics and kinetics of the initial stages of bacterial adhesion. For this purpose, bacterial pathogens Staphylococcus aureus and Escherichia coli O157:H7 were inoculated on the substrates coated with thin thiol layers (i.e., 1-octanethiol, 1-decanethiol, 1-octadecanethiol, 16-mercaptohexadecanoic acid, and 2-aminoethanethiol hydrochloride) with varying hydrophobicity and surface potential. The time-resolved adhesion data revealed a transformation from an exponential dependence to a square root dependence on time upon changing the substrate from hydrophobic or hydrophilic with a negative zeta potential value to hydrophilic with a negative zeta potential for both pathogens. The dewetting of extracellular polymeric substances (EPS) produced by E. coli O157:H7 was more noticeable on hydrophobic substrates, compared to that of S. aureus, which is attributed to the more amphiphilic nature of staphylococcal EPS. The interplay between the timescale of EPS dewetting and the inverse of the adhesion rate constant modulated the distribution of E. coli O157:H7 within microcolonies and the resultant microcolonial morphology on hydrophobic substrates. Observed trends in the formation of bacterial monolayers rather than multilayers and microcolonies rather than isolated and evenly spaced bacterial cells could be explained by a colloidal model considering van der Waals and electrostatic double-layer interactions only after introducing the contribution of elastic energy due to adhesion-induced deformations at intercellular and substrate-cell interfaces. The gained knowledge is significant in the context of identifying surfaces with greater risk of bacterial contamination and guiding the development of novel surfaces and coatings with superior bacterial antifouling characteristics.

Thermo-responsive gels based on supramolecular assembly of an amidoamine and citric acid.

In this work, we report the formation of a novel, aqueous-based thermo-responsive, supramolecular gelling system prepared by a convenient and efficient self-assembly of a long-chain amino-amide and citric acid. To determine the viscosity behavior and to gain insights into the gelation mechanism, a complementary combination of techniques, including Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), dynamic light scattering (DLS), and sinusoidal oscillatory tests, were used. The supramolecular gelator exhibited remarkably reversible sol-gel transitions induced by temperature at 76 °C. At a concentration of 5 wt%, the zero-frequency viscosity of the supramolecular system increased by about four orders of magnitude (from 4.2 to 12 563 Pa s) by changing the temperature from 23 °C to 76 °C. The viscous nature of the supramolecular gel could be preserved up to 90 °C. The synergistic combination of the hydrogen bonding between amino and carboxylic acid groups and the electrostatic interactions arising from the protonation of the amino-group and the deprotonation of carboxylic acid groups enhanced at higher temperatures is presumably responsible for the thermo-responsive behavior. We anticipate that these supramolecular gelators can be beneficial in various applications such as hydrogel scaffolds for regenerative medicine, personal care products and cosmetics, and enhanced oil recovery as viscosity modifiers.

Structural, tribological, and mechanical properties of the hind leg joint of a jumping insect: Using katydids to inform bioinspired lubrication systems.

This study investigates the structural properties of the hind leg femur-tibia joint in adult katydids (Orthoptera: Tettigoniidae), including its tribological and mechanical properties. It is of particular interest because the orthopteran (e.g., grasshoppers, crickets, and katydids) hind leg is highly specialized for jumping. We show that the katydid hind leg femur-tibia joint had unique surfaces and textures, with a friction coefficient (µ) at its coupling surface of 0.053±0.001. Importantly, the sheared surfaces at this joint showed no sign of wear or damage, even though it had undergone thousands of external shearing cycles. We attribute its resiliency to a synergistic interaction between the hierarchical surface texture/pattern on the femoral surfaces, a nanograded internal nanostructure of articulating joints, and the presence of lubricating lipids on the surface at the joint interface. The micro/nanopatterned surface of the katydid hind leg femur-tibia joint enables a reduction in the total contact area, and this significantly reduces the adhesive forces between the coupling surfaces. In our katydids, the femur and tibia joint surfaces had a maximum effective elastic modulus (Eeff) value of 2.6GPa and 3.9GPa, respectively. Presumably, the decreased adhesion through the reduction of van der Waals forces prevented adhesive wear, while the contact between the softer textured surface and harder smooth surface avoided abrasive wear. The results from our bioinspired study offer valuable insights that can inform the development of innovative coatings and lubrication systems that are both energy efficient and durable. STATEMENT OF SIGNIFICANCE: Relative to body length, insects can outjump most animals. They also accelerate their bodies at a much faster rate. Orthopterans (e.g., grasshoppers, crickets, and katydids) have hind legs that are specialized for jumping. Over an individual's lifetime, the hind leg joint endures repeated cycles of flexing and extending, including jumping, and its efficiency and durability easily surpass that of most mechanical devices. Although the efficient functioning of insect joints has long been recognized, the mechanism by which insect joints experience friction/adhesion/wear, and operate efficiently/reliably is still largely unknown. Our study on the structural, tribological, and mechanical properties of the orthopteran hind leg joints reveals the potential of katydid bioinspired research leading to more effective coatings and lubrication systems.

Metal-Organic-Inorganic Nanocomposite Thermal Interface Materials with Ultralow Thermal Resistances.

As electronic devices get smaller and more powerful, energy density of energy storage devices increases continuously, and moving components of machinery operate at higher speeds, the need for better thermal management strategies is becoming increasingly important. The removal of heat dissipated during the operation of electronic, electrochemical, and mechanical devices is facilitated by high-performance thermal interface materials (TIMs) which are utilized to couple devices to heat sinks. Herein, we report a new class of TIMs involving the chemical integration of boron nitride nanosheets (BNNS), soft organic linkers, and a copper matrix-which are prepared by the chemisorption-coupled electrodeposition approach. These hybrid nanocomposites demonstrate bulk thermal conductivities ranging from 211 to 277 W/(m K), which are very high considering their relatively low elastic modulus values on the order of 21.2-28.5 GPa. The synergistic combination of these properties led to the ultralow total thermal resistivity values in the range of 0.38-0.56 mm2 K/W for a typical bond-line thickness of 30-50 µm, advancing the current state-of-art transformatively. Moreover, its coefficient of thermal expansion (CTE) is 11 ppm/K, forming a mediation zone with a low thermally induced axial stress due to its close proximity to the CTE of most coupling surfaces needing thermal management.

Nanoporous aerogel as a bacteria repelling hygienic material for healthcare environment.

Healthcare-associated infections (HAIs) caused by pathogenic bacteria are a worldwide problem and responsible for numerous cases of morbidity and mortality. Exogenous cross-contamination is one of the main mechanisms contributing to such infections. This work investigates the potential of hydrophobically modified nanoporous silica aerogel as an antiadhesive hygienic material that can inhibit exogenous bacterial contamination. Nanoporous silica aerogels were synthesized via sol-gel polymerization of tetraethyl orthosilicate and hydrophobized using trimethylsilyl chloride. Bacterial adhesion characteristics were evaluated via dip-inoculation in suspensions of Gram-negative Escherichia coli O157:H7 and Gram-positive Staphylococcus aureus. The attachment of E. coli O157:H7 and S. aureus to hydrophobic nanoporous silica aerogel (HNSA) was found to be significantly lower than that to hydrophilic and hydrophobic nonporous silica materials: 99.91% (E. coli O157:H7) and 99.93% (S. aureus) reduction in comparison to hydrophilic nonporous silica, and 82.95% (E. coli O157:H7) and 84.90% (S. aureus) reduction in comparison to hydrophobic nonporous silica. These results suggest that the use of HNSA as surfaces that come into contact with bacterial pathogens in the healthcare environment can improve bacterial hygiene, and therefore may reduce the rate of HAIs.

Bacterially Antiadhesive, Optically Transparent Surfaces Inspired from Rice Leaves.

Because of the growing prevalence of antimicrobial resistance strains, there is an increasing need to develop material surfaces that prevent bacterial attachment and contamination in the absence of antibiotic agents. Herein, we present bacterial antiadhesive materials inspired from rice leaves. "Rice leaf-like surfaces" (RLLS) were fabricated by a templateless, self-masking reactive-ion etching approach. Bacterial attachment on RLLS was characterized under both static and dynamic conditions using Gram-negative Escherichia coli O157:H7 and Gram-positive Staphylococcus aureus. RLLS surfaces showed exceptional bacterial antiadhesion properties with a >99.9% adhesion inhibition efficiency. Furthermore, the optical properties of RLLS were investigated using UV-vis-NIR spectrophotometry. In contrast to most other bacterial antiadhesive surfaces, RLLS demonstrated optical-grade transparency (i.e., ≥92% transmission). We anticipate that the combination of bacterial antiadhesion efficiency, optical grade transparency, and the convenient single-step method of preparation makes RLLS a very attractive candidate for the surfaces of biosensors; endoscopes; and microfluidic, bio-optical, lab-on-a-chip, and touchscreen devices.

Preventing adhesion of Escherichia coli O157:H7 and Salmonella Typhimurium LT2 on tomato surfaces via ultrathin polyethylene glycol film.

This work deals with adhesion of Escherichia coli O157:H7 and Salmonella enterica subsp. enterica serovar Typhimurium LT2 (S. Typhimurium LT2) on polyethylene glycol (PEG) coated tomato surfaces. PEG coating was characterized by water contact angle technique, scanning electron microscopy, and secondary ion mass spectrometry. It was shown that PEG films could physisorb on the tomato surfaces after the oxygen plasma treatment, which made some outermost layers of the surfaces hydrophilic. Bacterial adhesion on PEG coated tomato surface was studied by standard plate count, fluorescence microscopy, and scanning electron microscopy techniques. Fully covered PEG film reduced the bacterial attachment 90% or more in comparison to the bare tomato surface. The degree of bacterial attachment decreased exponentially with increasing PEG coverage. When desired, PEG film could be removed by rinsing with water. Overall, this work demonstrates the proof-of-concept that an ultrathin film of polyethylene glycol may be used to effectively inhibit the attachment of pathogenic bacteria on tomato surfaces.

Capillarity induced large area patterning of peptide nanowires.

Peptide nanostructures assembled from an aromatic diphenylalanine have attracted considerable attention because of high thermal and mechanical stabilities of the assembled morphologies. Of diverse assembled structures, liquid crystalline peptide nanowires exhibiting optical and mechanical anisotropies can be a valuable building block for micro- or nano-fluidics, molecular electronics, and biological sensing. In this work, we investigated large scale patterning of liquid crystalline peptide nanowires and pattern transfer. The peptide nanowires could be highly aligned on a substrate by capillary flow over a large area. The high etching resistivity of nanowires to subsequent reactive ion etching process allowed for a successful pattern transfer of the well-aligned nanowire morphology onto the underlying SiO2 substrate.

Hierarchical assembly of diphenylalanine into dendritic nanoarchitectures.

Highly ordered, multi-dimensional dendritic nanoarchitectures were created via self-assembly of diphenylalanine from an acidic buffer solution. The self-similarity of dendritic structures was characterized by examining their fractal dimensions with the box-counting method. The fractal dimension was determined to be 1.7, which demonstrates the fractal dimension of structures generated by diffusion limited aggregation on a two-dimensional substrate surface. By confining the dendritic assembly of diphenylalanine within PDMS microchannels, the self-similar dendritic growth could be hierarchically directed to create linearly assembled nanoarchitectures. Our approach offers a novel pathway for creating and directing hierarchical nanoarchitecture from biomolecular assembly.