Paper electrochemical immunosensor for the rapid screening of Galectin-3 patients with heart failure.

A paper electrochemical immunosensor for the combined binding and quantification of the heart failure (HF) biomarker Galectin-3 has been developed. The simple design of the new sensor is comprised of paper material that is decorated with gold nanostructures, to maximize its electroactive surface area, and functionalized with target-specific recognition molecules to selectively bind the protein from aqueous solutions. The binding of the protein caused the blockage of the electron flow to the sensor electroactive surface, thus causing its oxidation potential to shift and the corresponding current to reduce quantitatively with the increase in the protein concentration within the working range of 0.5ng/mL-8ng/mL (LOQ-0.5 ng/mL). This novel sensor was able to quantify Galectin-3 concentration in saliva samples from HF patients and healthy controls within 20 min with good reproducibility (RSD = 3.64%), without the need for complex sample processing steps. The electrochemical measurements of the patient samples were cross validated by ELISA where the percent agreement between the two methods was found to be 92.7% (RSD = 7.20%). Therefore, the new paper immunosensor sensor has a strong potential for rapid and cost-effective screening of the Galectin 3 biomarker at points of care, thus supporting the timely diagnosis of heart failure.

Highly Sensitive NO2 Gas Sensors Based on MoS2@MoO3 Magnetic Heterostructure.

Recently, two-dimensional (2D) materials and their heterostructures have attracted considerable attention in gas sensing applications. In this work, we synthesized 2D MoS2@MoO3 heterostructures through post-sulfurization of α-MoO3 nanoribbons grown via vapor phase transport (VPT) and demonstrated highly sensitive NO2 gas sensors based on the hybrid heterostructures. The morphological, structural, and compositional properties of the MoS2@MoO3 hybrids were studied by a combination of advanced characterization techniques revealing a core-shell structure with the coexistence of 2H-MoS2 multilayers and intermediate molybdenum oxysulfides on the surface of α-MoO3. The MoS2@MoO3 hybrids also exhibit room-temperature ferromagnetism, revealed by vibrating sample magnetometry (VSM), as a result of the sulfurization process. The MoS2@MoO3 gas sensors display a p-type-like response towards NO2 with a detection limit of 0.15 ppm at a working temperature of 125 °C, as well as superb selectivity and reversibility. This p-type-like sensing behavior is attributed to the heterointerface of MoS2-MoO3 where interfacial charge transfer leads to a p-type inversion layer in MoS2, and is enhanced by magnetic dipole interactions between the paramagnetic NO2 and the ferromagnetic sensing layer. Our study demonstrates the promising application of 2D molybdenum hybrid compounds in gas sensing applications with a unique combination of electronic and magnetic properties.

Surface Treatment of Inorganic CsPbI3 Nanocrystals with Guanidinium Iodide for Efficient Perovskite Light-Emitting Diodes with High Brightness.

The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material. In particular, nanocrystals (NCs) of inorganic perovskites have demonstrated excellent performance for light-emitting and display applications. However, the presence of surface defects on the NCs negatively impacts their performance in devices. Herein, we report a compatible facial post-treatment of CsPbI3 nanocrystals using guanidinium iodide (GuI). It is found that the GuI treatment effectively passivated the halide vacancy defects on the surface of the NCs while offering effective surface protection and exciton confinement thanks to the beneficial contribution of iodide and guanidinium cation. As a consequence, the film of treated CsPbI3 nanocrystals exhibited significantly enhanced luminescence and charge transport properties, leading to high-performance light-emitting diode with maximum external quantum efficiency of 13.8% with high brightness (peak luminance of 7039 cd m-2 and a peak current density of 10.8 cd A-1). The EQE is over threefold higher than performance of untreated device (EQE: 3.8%). The operational half-lifetime of the treated devices also was significantly improved with T50 of 20 min (at current density of 25 mA cm-2), outperforming the untreated devices (T50 ~ 6 min).

Effects of Nanopillar Size and Spacing on Mechanical Perturbation and Bactericidal Killing Efficiency.

Nanopatterned surfaces administer antibacterial activity through contact-induced mechanical stresses and strains, which can be modulated by changing the nanopattern's radius, spacing and height. However, due to conflicting recommendations throughout the theoretical literature with poor agreement to reported experimental trends, it remains unclear whether these key dimensions-particularly radius and spacing-should be increased or decreased to maximize bactericidal efficiency. It is shown here that a potential failure of biophysical models lies in neglecting any out-of-plane effects of nanopattern contact. To highlight this, stresses induced by a nanopattern were studied via an analytical model based on minimization of strain and adhesion energy. The in-plane (areal) and out-of-plane (contact pressure) stresses at equilibrium were derived, as well as a combined stress (von Mises), which comprises both. Contour plots were produced to illustrate which nanopatterns elicited the highest stresses over all combinations of tip radius between 0 and 100 nm and center spacing between 0 and 200 nm. Considering both the in-plane and out-of-plane stresses drastically transformed the contour plots from those when only in-plane stress was evaluated, clearly favoring small tipped, tightly packed nanopatterns. In addition, the effect of changes to radius and spacing in terms of the combined stress showed the best qualitative agreement with previous reported trends in killing efficiency. Together, the results affirm that the killing efficiency of a nanopattern can be maximized by simultaneous reduction in tip radius and increase in nanopattern packing ratio (i.e., radius/spacing). These findings provide a guide for the design of highly bactericidal nanopatterned surfaces.

Resolving Bio-Nano Interactions of E. coli Bacteria-Dragonfly Wing Interface with Helium Ion and 3D-Structured Illumination Microscopy to Understand Bacterial Death on Nanotopography.

Obtaining a comprehensive understanding of the bactericidal mechanisms of natural nanotextured surfaces is crucial for the development of fabricated nanotextured surfaces with efficient bactericidal activity. However, the scale, nature, and speed of bacteria-nanotextured surface interactions make the characterization of the interaction a challenging task. There are currently several different opinions regarding the possible mechanisms by which bacterial membrane damage occurs upon interacting with nanotextured surfaces. Advanced imaging methods could clarify this by enabling visualization of the interaction. Charged particle microscopes can achieve the required nanoscale resolution but are limited to dry samples. In contrast, light-based methods enable the characterization of living (hydrated) samples but are limited by the resolution achievable. Here we utilized both helium ion microscopy (HIM) and 3D structured illumination microscopy (3D-SIM) techniques to understand the interaction of Gram-negative bacterial membranes with nanopillars such as those found on dragonfly wings. Helium ion microscopy enables cutting and imaging at nanoscale resolution, while 3D-SIM is a super-resolution optical microscopy technique that allows visualization of live, unfixed bacteria at ∼100 nm resolution. Upon bacteria-nanopillar interaction, the energy stored due to the bending of natural nanopillars was estimated and compared with fabricated vertically aligned carbon nanotubes. With the same deflection, shorter dragonfly wing nanopillars store slightly higher energy compared to carbon nanotubes. This indicates that fabricated surfaces may achieve similar bactericidal efficiency as dragonfly wings. This study reports in situ characterization of bacteria-nanopillar interactions in real-time close to its natural state. These microscopic approaches will help further understanding of bacterial membrane interactions with nanotextured surfaces and the bactericidal mechanisms of nanotopographies so that more efficient bactericidal nanotextured surfaces can be designed and fabricated, and their bacteria-nanotopography interactions can be assessed in situ.

Ultrathin Ni1- x Co x S2 nanoflakes as high energy density electrode materials for asymmetric supercapacitors.

Transition metal compounds such as nickel cobalt sulfides (Ni-Co-S) are promising electrode materials for energy storage devices such as supercapacitors owing to their high electrochemical performance and good electrical conductivity. Developing ultrathin nanostructured materials is critical to achieving high electrochemical performance, because they possess rich active sites for electrochemical reactions, shortening the transport path of ions in the electrolyte during the charge/discharge processes. This paper describes the synthesis of ultrathin (around 10 nm) flower-like Ni1- x Co x S2 nanoflakes by using templated NiCo oxides. The as-prepared Ni1- x Co x S2 material retained the morphology of the initial NiCo oxide material and exhibited a much improved electrochemical performance. The Ni1- x Co x S2 electrode material exhibited a maximum specific capacity of 1066.8 F·g-1 (533.4 C·g-1) at 0.5 A·g-1 and a capacity retention of 63.4% at 20 A·g-1 in an asymmetric supercapacitor (ASC). The ASC showed a superior energy density of 100.5 Wh·kg-1 (at a power density of 1.5 kW·kg-1), an ultrahigh power density of 30 kW·kg-1 (at an energy density of 67.5 Wh·kg-1) and excellent cycling stability. This approach can be a low-cost way to mass-produce high-performance electrode materials for supercapacitors.

Bacteria Death and Osteoblast Metabolic Activity Correlated to Hydrothermally Synthesised TiO2 Surface Properties.

Orthopaedic surgery comes with an inherent risk of bacterial infection, prolonged antibiotic therapy and revision surgery. Recent research has focused on nanostructured surfaces to improve the bactericidal and osseointegrational properties of implants. However, an understanding of the mechanical properties of bactericidal materials is lacking. In this work, the surface properties of hydrothermal TiO2 nanostructured surfaces are investigated for their effect on bactericidal efficiency and cellular metabolic activity of human osteoblast cells. TiO2 nanostructures, approximately 307 nm in height and 14 GPa stiffness, were the most effective structures against both gram-positive (Staphylococcus aureus) and gram-negative (Pseudomonas aeruginosa) bacteria. Statistical analysis significantly correlated structure height to the death of both bacteria strains. In addition, the surface contact angle and Young's modulus were correlated to osteoblast metabolic activity. Hydrophilic surfaces with a contact angle between 35 and 50° produced the highest cellular metabolic activity rates after 24 hours of incubation. The mechanical tests showed that nanostructures retain their mechanical stability and integrity over a long time-period, reaffirming the surfaces' applicability for implants. This work provides a thorough examination of the surface, mechanical and wettability properties of multifunctional hydrothermally synthesised nanostructured materials, capable of killing bacteria whilst improving osteoblast metabolic rates, leading to improved osseointegration and antibacterial properties of orthopaedic implants.

Electronic and optical properties of lead-free hybrid double perovskites for photovoltaic and optoelectronic applications.

Developing of lead-free double perovskites have drawn significant interest for photovoltaics and optoelectronics as the materials have the potential to avoid toxicity and instability issues associated with lead-based organometallic perovskites. In this study, we report the optoelectronic properties of a new group of non-toxic lead-free organic-inorganic halide double perovskites composed of caesium (Cs), methylammonium (MA) or formamidinium (FA) with bismuth (Bi) and metal copper (Cu). We perform density functional theory investigations to calculate the structural, electronic and optical properties of 18 Pb-free compounds, ABiCuX6 [A = Cs2, (MA)2, (FA)2, CsMA, CsFA, MAFA; X = I, Br, Cl] to predict their suitability in photovoltaic and optoelectronic applications. We found that the considered compounds are semiconductors with a tunable band gap characteristics that are suitable for some devices like light emitting diodes. In addition to this, the high dielectric constant, high absorption, high optical conductivity and low reflectivity suggest that the materials have the potential in a wide range of optoelectronic applications including solar cells. Furthermore, we predict that the organic-inorganic hybrid double perovskite (FA)2BiCuI6 is the best candidate in photovoltaic and optoelectronic applications as the material has superior optical and electronic properties.

Multi-biofunctional properties of three species of cicada wings and biomimetic fabrication of nanopatterned titanium pillars.

Recently, multi-biofunctional properties of cicada wings have drawn keen interest for biomedical device applications due to their superhydrophobic, self-cleaning and bactericidal effects. We present a systematic evaluation of bactericidal and cytocompatible properties of cicada wings. We also present biomimetic nanofabrication of a patterned array of titanium nanopillars using electron beam lithography. We have characterized the nanoscale architecture of the wings of three different Australian species of cicadas (Psaltoda claripennis, Aleeta curvicosta and Palapsalta eyrei) using helium ion microscopy (HIM), scanning electron microscopy, atomic force measurement (AFM) and transmission electron microscopy (TEM). The chemical nature of the nanopatterned substrates was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Pseudomonas aeruginosa and Staphylococcus aureus cells were attached to determine the bactericidal activity of the insect wings. Human osteoblast cells were attached to examine the biocompatibility of the insect wings. It was found that all the three cicada species have unique surface topography on their wing membranes and veins. The height, spacing, diameter, density and aspect ratio of the three species varied between the species and between the membrane and the veins. The density and aspect ratio of the nanopillars on the membranes were significantly higher than on the veins. Bacterial attachment investigation confirmed that P. aeruginosa cells and S. aureus cells were damaged by the nanopatterned array of pillars. A significant reduction in colonies of P. aeruginosa cells was found on the wings of the three species compared to the control after 18 hours. A significant reduction of S. aureus cells on the wings was observed at 2 and 4 hours but not at 18 hours compared to the control. The cell morphology of the human osteoblast cells appeared intact after 24 hours of attachment, indicating the biocompatibility of the insect wings. As a proof of concept, patterned nanopillars of titanium have been fabricated using the electron beam lithography technique directly inspired by the cicada wing architecture. The titanium nanopillars were observed to damage the bacterial cells of P. aeruginosa in a manner similar to the cicada wing species and remain compatible to osteoblast cells. The outcomes of this research can help to engineer an optimum nano-patterned surface to enhance the bioactivity and bactericidal effect on biomedical devices.

Tuning the Amount of Oxygen Vacancies in Sputter-Deposited SnOx films for Enhancing the Performance of Perovskite Solar Cells.

This work demonstrates the effect of oxygen vacancies in SnOx thin films on the performance of perovskite solar cells. Various SnOx films with different amounts of oxygen vacancies were deposited by sputtering at different substrate temperatures (25-300 °C). The transmittance of the films decreased from 82 to 66 % with increasing deposition temperature from 25 to 300 °C. Both X-ray photoelectron spectroscopy and electron-spin resonance spectroscopy confirmed that a higher density of oxygen vacancies was created within the SnOx film at a high substrate temperature, which caused narrowing of the SnOx bandgap from 4.1 (25 °C) to 3.74 eV (250 °C). Combined ultraviolet photoelectron spectroscopy and UV/Vis spectroscopy showed an excellent conduction band position alignment between the methylammonium lead iodide perovskite layer (3.90 eV) and the SnOx electron transport layer deposited at 250 °C (3.92 eV). As a result, a significant enhancement of the open-circuit voltage from 0.82 to 1.0 V was achieved, resulting in an increase of the power conversion efficiency of the perovskite solar cells from 11 to 14 %. This research demonstrated a facile approach for controlling the amount of oxygen vacancies in SnOx thin films to achieve a desirable energy alignment with the perovskite absorber layer for enhanced device performance.

Mechanical, bactericidal and osteogenic behaviours of hydrothermally synthesised TiO2 nanowire arrays.

The application of orthopaedic implants is associated with risks of bacterial infection and long-term antibiotic therapy. This problem has led to the study of implants with nano-textured surfaces as a method of inhibiting bacterial adhesion and reducing implant failure due to infection. In this research, various nano-textured surfaces of TiO2 were synthesised using hydrothermal synthesis, by varying NaOH concentration, reaction time and reaction temperature. Their correlations to mechanical, morphological, bactericidal and osteogenic properties of the surfaces were investigated. It was found that high alkaline concentrations produced large nanowire mesh arrays, while short reaction time and low temperature produced comparatively smaller arrays. The highly dense morphology formed at higher NaOH concentrations has resulted in high elastic modulus and hardness values, compared to surfaces produced at lower NaOH concentrations. Viability tests of the TiO2 nanowire array against gram-positive Staphylococcus aureus cells showed a bactericidal efficiency of 54% and 33% after 3 and 18 h, respectively. This nano-textured surface produces an osteoblast cellular metabolic activity of 71% after 24 h, compared to 67% when exposed to a flat Ti control surface. This preliminary work demonstrates an excellent outcome in producing bactericidal surfaces that promoted metabolic activity of human osteoblast cells for potential use in orthopaedic implants.

Towards lead-free perovskite photovoltaics and optoelectronics by ab-initio simulations.

Lead (Pb) free non-toxic perovskite solar cells have become more important in the commercialization of the photovoltaic devices. In this study the structural, electronic, optical and mechanical properties of Pb-free inorganic metal halide cubic perovskites CsBX3 (B = Sn, Ge; X = I, Br, Cl) for perovskite solar cells are simulated using first-principles Density Functional Theory (DFT). These compounds are semiconductors with direct band gap energy and mechanically stable. Results suggest that the materials have high absorption coefficient, low reflectivity and high optical conductivity with potential application in solar cells and other optoelectronic energy devices. On the basis of the optical properties, one can expect that the Germanium (Ge) would be a better replacement of Pb as Ge containing compounds have higher optical absorption and optical conductivity than that of Pb containing compounds. A combinational analysis of the electronic, optical and mechanical properties of the compounds suggests that CsGeI3 based perovskite is the best Pb-free inorganic metal halide semiconductor for the solar cell application. However, the compound with solid solution of CsGe(I0.7Br0.3)3 is found to be mechanically more ductile than CsGeI3. This study will also guide to obtain Pb-free organic perovskites for optoelectronic devices.

Bactericidal Effects of Natural Nanotopography of Dragonfly Wing on Escherichia coli.

Nanotextured surfaces (NTSs) are critical to organisms as self-adaptation and survival tools. These NTSs have been actively mimicked in the process of developing bactericidal surfaces for diverse biomedical and hygiene applications. To design and fabricate bactericidal topographies effectively for various applications, understanding the bactericidal mechanism of NTS in nature is essential. The current mechanistic explanations on natural bactericidal activity of nanopillars have not utilized recent advances in microscopy to study the natural interaction. This research reveals the natural bactericidal interaction between E. coli and a dragonfly wing's (Orthetrum villosovittatum) NTS using advanced microscopy techniques and proposes a model. Contrary to the existing mechanistic models, this experimental approach demonstrated that the NTS of Orthetrum villosovittatum dragonfly wings has two prominent nanopillar populations and the resolved interface shows membrane damage occurred without direct contact of the bacterial cell membrane with the nanopillars. We propose that the bacterial membrane damage is initiated by a combination of strong adhesion between nanopillars and bacterium EPS layer as well as shear force when immobilized bacterium attempts to move on the NTS. These findings could help guide the design of novel biomimetic nanomaterials by maximizing the synergies between biochemical and mechanical bactericidal effects.