Nanotopology-Enabled On-Site Pathogen Detection for Managing Atopic Dermatitis.

Atopic dermatitis (AD), a prevalent skin condition often complicated by microbial infection, poses a significant challenge in identifying the responsible pathogen for its effective management. However, a reliable, safe tool for pinpointing the source of these infections remains elusive. In this study, a novel on-site pathogen detection that combines chemically functionalized nanotopology with genetic analysis is proposed to capture and analyze pathogens closely associated with severe atopic dermatitis. The chemically functionalized nanotopology features a 3D hierarchical nanopillar array (HNA) with a functional polymer coating, tailored to isolate target pathogens from infected skin. This innovative nanotopology demonstrates superior pathogenic capture efficiency, favorable entrapment patterns, and non-cytotoxicity. An HNA-assembled stick is utilized to directly retrieve bacteria from infected skin samples, followed by extraction-free quantitative loop-mediated isothermal amplification (direct qLAMP) for validation. To mimic human skin conditions, porcine skin is employed to successfully capture Staphylococcus aureus, a common bacterium exacerbating AD cases. The on-site detection method exhibits an impressive detection limit of 103 cells mL-1 . The HNA-assembled stick represents a promising tool for on-site detection of bacteria associated with atopic dermatitis. This innovative approach enables to deepen the understanding of AD pathogenesis and open avenues for more effective management strategies for chronic skin conditions.

Polyaniline-based 3D network structure promotes entrapment and detection of drug-resistant bacteria.

Sensitive and accurate capture, enrichment, and identification of drug-resistant bacteria on human skin are important for early-stage diagnosis and treatment of patients. Herein, we constructed a three-dimensional hierarchically structured polyaniline nanoweb (3D HPN) to capture, enrich, and detect drug-resistant bacteria on-site by rubbing infected skins. These unique hierarchical nanostructures enhance bacteria capture efficiency and help severely deform the surface of the bacteria entrapped on them. Therefore, 3D HPN significantly contributes to the effective and reliable recovery of drug-resistant bacteria from the infected skin and the prevention of potential secondary infection. The recovered bacteria were successfully identified by subsequent real-time polymerase chain reaction (PCR) analysis after the lysis process. The molecular analysis results based on a real-time PCR exhibit excellent sensitivity to detecting target bacteria of concentrations ranging from 102 to 107 CFU/mL without any fluorescent signal interruption. To confirm the field applicability of 3D HPN, it was tested with a drug-resistant model consisting of micropig skin similar to human skin and Klebsiella pneumoniae carbapenemase-producing carbapenem-resistant Enterobacteriaceae (KPC-CRE). The results show that the detection sensitivity of this assay is 102 CFU/mL. Therefore, 3D HPN can be extended to on-site pathogen detection systems, along with rapid molecular diagnostics through a simple method, to recover KPC-CRE from the skin.

Highly Stretchable Sensor Based on Fluid Dynamics-Assisted Graphene Inks for Real-Time Monitoring of Sweat.

Graphene inks have recently attracted attention for the development of printed wearable and flexible electronics and sensors not only because of their high conductivity and low cost but also because they are suitable for high-speed printing. Although reliable and scalable printing technologies are well established, further improvement in graphene inks in terms of electrical conductivity, stretchability/flexibility, and mass production is necessary for sensors for real-time monitoring. Herein, highly stretchable and conductive graphene inks were prepared by an efficient and scalable fluid dynamics-assisted exfoliation of graphite and a mixing process with elastomeric Ecoflex. After printing inks onto textile substrates, the serpentine-patterned conductors exhibited high conductivity and stable resistance even under a mechanically stretched state (a strain of 150%). Electrochemical sensors that detect sodium ions were fabricated on this conducting platform. These sensors indicated high potentiometric sensing ability under different mechanical deformations. To demonstrate the on-body performance of the developed sensors, real-time monitoring of sodium-ion concentration in the sweat of a human subject was carried out during an indoor stationary cycling exercise.

Touchable 3D hierarchically structured polyaniline nanoweb for capture and detection of pathogenic bacteria.

A bacteria-capturing platform is a critical function of accurate, quantitative, and sensitive identification of bacterial pathogens for potential usage in the detection of foodborne diseases. Despite the development of various nanostructures and their surface chemical modification strategies, relative to the principal physical contact propagation of bacterial infections, mechanically robust and nanostructured platforms that are available to capture bacteria remain a significant problem. Here, a three-dimensional (3D) hierarchically structured polyaniline nanoweb film is developed for the efficient capture of bacterial pathogens by hand-touching. This unique nanostructure ensures sufficient mechanical resistance when exposed to compression and shear forces and facilitates the 3D interfacial interactions between bacterial extracellular organelles and polyaniline surfaces. The bacterial pathogens (Escherichia coli O157:H7, Salmonella enteritidis, and Staphylococcus aureus) are efficiently captured through finger-touching, as verified by the polymerase chain reaction (PCR) analysis. Moreover, the real-time PCR results of finger-touched cells on a 3D nanoweb film show a highly sensitive detection of bacteria, which is similar to those of the real-time PCR using cultured cells without the capturing step without any interfering of fluorescence signal and structural deformation during thermal cycling.

3D Hierarchical Polyaniline-Metal Hybrid Nanopillars: Morphological Control and Its Antibacterial Application.

Effective and reliable antibacterial surfaces are in high demand in modern society. Although recent works have shown excellent antibacterial performance by combining unique hierarchical nanotopological structures with functional polymer coating, determining the antibacterial performance arising from morphological changes is necessary. In this work, three-dimensional (3D) hierarchical polyaniline-gold (PANI/Au) hybrid nanopillars were successfully fabricated via chemical polymerization (i.e., dilute method). The morphology and structures of the PANI/Au nanopillars were controlled by the reaction time (10 min to 60 h) and the molar concentrations of the monomer (0.01, 0.1, and 1 M aniline), oxidant (0.002, 0.0067, 0.01, and 0.02 M ammonium persulfate), and acid (0.01, 0.1, 1, and 2 M perchloric acid). These complex combinations allow controlling the hierarchical micro- to nanostructure of PANI on a nanopillar array (NPA). Furthermore, the surface of the 3D PANI/Au hierarchical nanostructure can be chemically treated while maintaining the structure using initiated chemical vapor deposition. Moreover, the excellent antibacterial performance of the 3D PANI/Au hierarchical nanostructure (HNS) exceeds 99% after functional polymer coating. The excellent antibacterial performance of the obtained 3D PANI/Au HNS is mainly because of the complex topological and physicochemical surface modification. Thus, these 3D PANI/Au hierarchical nanostructures are promising high-performance antibacterial materials.

Highly Concentrated, Conductive, Defect-free Graphene Ink for Screen-Printed Sensor Application.

HIGHLIGHTS: Ultrathin and defect-free graphene ink is prepared through a high-throughput fluid dynamics process, resulting in a high exfoliation yield (53.5%) and a high concentration (47.5 mg mL-1). A screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 104 S m-1 and good mechanical flexibility. An electrochemical sodium ion sensor based on graphene ink exhibits an excellent potentiometric sensing performance in a mechanically bent state. Real-time monitoring of sodium ion concentration in sweat is demonstrated. Conductive inks based on graphene materials have received significant attention for the fabrication of a wide range of printed and flexible devices. However, the application of graphene fillers is limited by their restricted mass production and the low concentration of their suspensions. In this study, a highly concentrated and conductive ink based on defect-free graphene was developed by a scalable fluid dynamics process. A high shear exfoliation and mixing process enabled the production of graphene at a high concentration of 47.5 mg mL-1 for graphene ink. The screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 104 S m-1 and maintains high conductivity under mechanical bending, compressing, and fatigue tests. Based on the as-prepared graphene ink, a printed electrochemical sodium ion (Na+) sensor that shows high potentiometric sensing performance was fabricated. Further, by integrating a wireless electronic module, a prototype Na+-sensing watch is demonstrated for the real-time monitoring of the sodium ion concentration in human sweat during the indoor exercise of a volunteer. The scalable and efficient procedure for the preparation of graphene ink presented in this work is very promising for the low-cost, reproducible, and large-scale printing of flexible and wearable electronic devices.

3D Hierarchical Nanotopography for On-Site Rapid Capture and Sensitive Detection of Infectious Microbial Pathogens.

Effective capture and rapid detection of pathogenic bacteria causing pandemic/epidemic diseases is an important task for global surveillance and prevention of human health threats. Here, we present an advanced approach for the on-site capture and detection of pathogenic bacteria through the combination of hierarchical nanostructures and a nuclease-responsive DNA probe. The specially designed hierarchical nanocilia and network structures on the pillar arrays, termed 3D bacterial capturing nanotopographical trap, exhibit excellent mechanical reliability and rapid (<30 s) and irreversible bacterial capturability. Moreover, the nuclease-responsive DNA probe enables the highly sensitive and extremely fast (<1 min) detection of bacteria. The bacterial capturing nanotopographical trap (b-CNT) facilitates the on-site capture and detection of notorious infectious pathogens (Escherichia coli O157:H7, Salmonella enteritidis, Staphylococcus aureus, and Bacillus cereus) from kitchen tools and food samples. Accordingly, the usefulness of the b-CNT is confirmed as a simple, fast, sensitive, portable, and robust on-site capture and detection tool for point-of-care testing.

Flexible nanopillar-based immunoelectrochemical biosensor for noninvasive detection of Amyloid beta.

The noninvasive early detection of biomarkers for Alzheimer's disease (AD) is essential for the development of specific treatment strategies. This paper proposes an advanced method for fabricating highly ordered and flexible nanopillar-based electrochemical biosensors by the combination of soft/photolithography and metal evaporation. The nanopillar array (NPA) exhibits high surface area containing 1500 nm height and 500 nm diameter with 3:1 ratio. In regard with physical properties of polyurethane (PU) substrate, the developed NPA is sustainable and durable to external pressure such as bending and twisting. To manipulate the NPA surface to biocompatible, the gold was uniformly deposited on the PU substrate. The thiol chemistry which is stably modified on the gold surface as a form of self-assembled monolayer was employed for fabricating the NPA as a biocompatible chip by covalently immobilize the antibodies. The proposed nanopillar-based immunoelectrochemical biosensor exhibited good and stable electrochemical performance in ß-amyloid (Aß) detection. Moreover, we successfully confirmed the performance of the as-developed sensor using the artificial injection of Aß in human tear, with sensitivity of 0.14 ng/mL and high reproducibility (as a standard deviation below 10%). Our findings show that the developed nanopillar-based sensor exhibits reliable electrochemical characteristics and prove its potential for application as a biosensor platform for testing at the point of care.

Antibacterial Nanopillar Array for an Implantable Intraocular Lens.

Postsurgical intraocular lens (IOL) infection caused by pathogenic bacteria can result in blindness and often requires a secondary operation to replace the contaminated lens. The incorporation of an antibacterial property onto the IOL surface can prevent bacterial infection and postoperative endophthalmitis. This study describes a polymeric nanopillar array (NPA) integrated onto an IOL, which captures and eradicates the bacteria by rupturing the bacterial membrane. This is accomplished by changing the behavior of the elastic nanopillars using bending, restoration, and antibacterial surface modification. The combination of the polymer coating and NPA dimensions can decrease the adhesivity of corneal endothelial cells and posterior capsule opacification without causing cytotoxicity. An ionic antibacterial polymer layer is introduced onto an NPA using an initiated chemical vapor deposition process. This improves bacterial membrane rupture efficiency by increasing the interactions between the bacteria and nanopillars and damages the bacterial membrane using quaternary ammonium compounds. The newly developed ionic polymer-coated NPA exceeds 99% antibacterial efficiency against Staphylococcus aureus, which is achieved through topological and physicochemical surface modification. Thus, this paper provides a novel, efficient strategy to prevent postoperative complications related to bacteria contamination of IOL after cataract surgery.

Highly self-healable and flexible cable-type pH sensors for real-time monitoring of human fluids.

Development of sensing technology with wearable chemical sensors is realizing non-invasive, real-time monitoring healthcare and disease diagnostics. The advanced sensor devices should be compact and portable for use in limited space, easy to wear on human body, and low-cost for personalized healthcare markets. Here, we report a highly sensitive, flexible, and autonomously self-healable pH sensor cable developed by weaving together two carbon fiber thread electrodes coated with mechanically robust self-healing polymers. The pH sensor cable showed excellent electrochemical performances of sensitivity, repeatability, and durability. Spontaneous and autonomous sensor healing efficiency of the pH sensor cable was demonstrated by measuring sensitivity during four cycles of cutting and healing process. The pH sensor cable could measure pH in small volumes of real human fluid samples, including urine, saliva, and sweat, and the results were similar to those of a commercial pH meter. Taken together, successful real-time pH monitoring for human sweat was demonstrated by fabricating a wearable sensing system in which the pH sensor cable was knitted into a headband integrated with wireless electronics.

Preparation of ultrathin defect-free graphene sheets from graphite via fluidic delamination for solid-contact ion-to-electron transducers in potentiometric sensors.

In this study, ultrathin and defect-free graphene (Gr) sheets were prepared through a fluid dynamics-induced shear exfoliation method using graphite. The high hydrophobicity and surface area of Gr make it attractive as a solid-contact ion-to-electron transducer for potentiometric K+ sensors, in which the electrodes are fabricated through a screen-printing process. The electrochemical characterization demonstrates that Gr solid contact results in a high double-layer capacitance, potential stability, and strong resistance against water layer, gases, and light. The Gr-based K+ sensors showed a Nernstian slope of 53.53 mV/log[K+] within a linear concentration range of 10-1-10-4 M, a low detection limit of 10-4.28 M, a fast response time of ~8 s, good repeatability, and excellent long-term stability. Moreover, the Gr-based K+ sensors provided accurate ion concentrations in actual samples of human sweat and sports drinks.

Development of zinc oxide-based sub-micro pillar arrays for on-site capture and DNA detection of foodborne pathogen.

Prevention and early detection of bacterial infection caused by foodborne pathogens are the most important task to human society. Although currently available diagnostic technologies have been developed and designed for detection of specific pathogens, suitable capturing tools for the pathogens are rarely studied. In this paper, a new methodology is developed and proposed to realize effective capturing through touchable flexible zinc oxide-based sub-micro pillar arrays through genetic analysis. Zinc oxide coated pillar arrays have a high surface area, flexible, and adheres strongly to bacteria. Therefore, it contributes to enhance the bacterial capturability. An in-depth analysis on the sub-sequential capturing process at the bacterial cell-pillar interface is presented. By carefully observing the structural changes and performing numerical analysis under different reaction times, the results are presented. The resulting zinc oxide coated pillar arrays exhibited comprehensive capturability. These pillars were able to detect pathogenic bacteria due to a combination of complex structures, depletion force, and high surface electrostatics. The developed sub-micro pillars successfully captured and detected infectious foodborne bacteria of Escherichia coli in the range of 106-101 CFU/mL.

Extremely Fast Self-Healable Bio-Based Supramolecular Polymer for Wearable Real-Time Sweat-Monitoring Sensor.

Sensors with autonomous self-healing properties offer enhanced durability, reliability, and stability. Although numerous self-healing polymers have been attempted, achieving sensors with fast and reversible recovery under ambient conditions with high mechanical toughness remains challenging. Here, a highly sensitive wearable sensor made of a robust bio-based supramolecular polymer that is capable of self-healing via hydrogen bonding is presented. The integration of carbon fiber thread into a self-healing polymer matrix provides a new toolset that can easily be knitted into textile items to fabricate wearable sensors that show impressive self-healing efficiency (>97.0%) after 30 s at room temperature for K+/Na+ sensing. The wearable sweat-sensor system-coupled with a wireless electronic circuit board capable of transferring data to a smart phone-successfully monitors electrolyte ions in human perspiration noninvasively in real time, even in the healed state during indoor exercise. Our smart sensors represent an important advance toward futuristic personalized healthcare applications.

Potentiometric performance of flexible pH sensor based on polyaniline nanofiber arrays.

We report potentiometric performance of a polyaniline nanofiber array-based pH sensor fabricated by combining a dilute chemical polymerization and low-cost and simple screen printing process. The pH sensor had a two-electrode configuration consisting of polyaniline nanofiber array sensing electrode and Ag/AgCl reference electrode. Measurement of electromotive force between sensing and reference electrodes provided various electrochemical properties of pH sensors. The pH sensor show excellent sensor performances of sensitivity of 62.4 mV/pH, repeatability of 97.9% retention, response time of 12.8 s, and durability of 3.0 mV/h. The pH sensor could also measure pH changes as the milk is spoiled, which is similar to those of a commercial pH meter. The pH sensors were highly flexible, and thus can measure the fruit decay on the curved surface of an apple. This flexible and miniature pH sensor opens new opportunities for monitoring of water, product process, human health, and chemical (or bio) reactions even using small volumes of samples.

Fast and Scalable Hydrodynamic Synthesis of MnO2/Defect-Free Graphene Nanocomposites with High Rate Capability and Long Cycle Life.

The integration of metal oxides and carbon materials provides a great potential for enhancing the high energy and power densities of supercapacitors, but the rational design and scalable fabrication of such composite materials still remain a challenge. Herein, we report a fast, scalable, and one-pot hydrodynamic synthesis for preparing ion conductive and defect-free graphene from graphite and MnO2/graphene nanocomposites. The use of this hydrodynamic method using Taylor-Couette flow allows us to efficiently fast shear-exfoliate graphite into large quantities of high-quality graphene sheets. Deposition of MnO2 on graphene is subsequently performed in a fluidic reactor within 10 min. The prepared MnO2/graphene nanocomposite shows outstanding electrochemical performances, such as a high specific capacitance of 679 F/g at 25 mV/s, a high rate capability of 74.7% retention at an extremely high rate of 1000 mV/s, and an excellent cycling characteristic (∼94.7% retention over 20 000 cycles). An asymmetric supercapacitor device is fabricated by assembling an anode of graphene and a cathode of MnO2/graphene, which resulted in high energy (35.2 W h/kg) and power (7.4 kW/kg) densities (accounting for the mass of both electrodes and the electrolyte) with a high rate capability and long cycle life.

Flexible nanopillar-based electrochemical sensors for genetic detection of foodborne pathogens.

Flexible and highly ordered nanopillar arrayed electrodes have brought great interest for many electrochemical applications, especially to the biosensors, because of its unique mechanical and topological properties. Herein, we report an advanced method to fabricate highly ordered nanopillar electrodes produced by soft-/photo-lithography and metal evaporation. The highly ordered nanopillar array exhibited the superior electrochemical and mechanical properties in regard with the wide space to response with electrolytes, enabling the sensitive analysis. As-prepared gold and silver electrodes on nanopillar arrays exhibit great and stable electrochemical performance to detect the amplified gene from foodborne pathogen of Escherichia coli O157:H7. Additionally, lightweight, flexible, and USB-connectable nanopillar-based electrochemical sensor platform improves the connectivity, portability, and sensitivity. Moreover, we successfully confirm the performance of genetic analysis using real food, specially designed intercalator, and amplified gene from foodborne pathogens with high reproducibility (6% standard deviation) and sensitivity (10 × 1.01 CFU) within 25 s based on the square wave voltammetry principle. This study confirmed excellent mechanical and chemical characteristics of nanopillar electrodes have a great and considerable electrochemical activity to apply as genetic biosensor platform in the fields of point-of-care testing (POCT).

Heteroassembled gold nanoparticles with sandwich-immunoassay LSPR chip format for rapid and sensitive detection of hepatitis B virus surface antigen (HBsAg).

This study aimed to develop a more sensitive method for the detection of hepatitis B surface antigen (HBsAg) using heteroassembled gold nanoparticles (AuNPs). A single layered localized surface plasmon resonance (LSPR) chip format was developed with antigen-antibody reaction-based detection symmetry using AuNPs, which detected HBsAg at 10 pg/mL. To further improve the detection limit, a modified detection format was fabricated by fixing a secondary antibody (to form a heteroassembled sandwich format) to the AuNP monolayer, which enhanced the detection sensitivity by about 100 times. The developed heteroassembled AuNPs sandwich-immunoassay LSPR chip format was able to detect as little as 100 fg/mL of HBsAg within 10-15 min. In addition, the heteroassembled AuNPs sandwich-immunoassay LSPR chip format did not show any non-specific binding to other tested antigens, including alpha fetoprotein (AFP), C-reactive protein (CRP), and prostate-specific antigen (PSA). These findings confirm that the proposed detection strategy of heteroassembled AuNPs sandwich-immunoassay LSPR chip format may provide a new platform for early diagnosis of various human diseases.

Sustainable Boron Nitride Nanosheet-Reinforced Cellulose Nanofiber Composite Film with Oxygen Barrier without the Cost of Color and Cytotoxicity.

This paper introduces a boron nitride nanosheet (BNNS)-reinforced cellulose nanofiber (CNF) film as a sustainable oxygen barrier film that can potentially be applied in food packaging. Most commodity plastics are oxygen-permeable. CNF exhibits an ideal oxygen transmission rate (OTR) of <1 cc/m²/day in highly controlled conditions. A CNF film typically fabricated by the air drying of a CNF aqueous solution reveals an OTR of 19.08 cc/m²/day. The addition of 0⁻5 wt % BNNS to the CNF dispersion before drying results in a composite film with highly improved OTR of 4.7 cc/m²/day, which is sufficient for meat and cheese packaging. BNNS as a 2D nanomaterial increases the pathway of oxygen gas and reduces the chances of pinhole formation during film fabrication involving water drying. In addition, BNNS improves the mechanical properties of the CNF films (Young's modulus and tensile strength) without significant elongation reductions, probably due to the good miscibility of CNF and BNNS in the aqueous solution. Addition of BNNS also produces negligible color change, which is important for film aesthetics. An in vitro cell experiment was performed to reveal the low cytotoxicity of the CNF/BNNS composite. This composite film has great potential as a sustainable high-performance food-packaging material.

Fabrication of newspaper-based potentiometric platforms for flexible and disposable ion sensors.

Paper-based materials have attracted a great deal of attention in sensor applications because they are readily available, biodegradable, inexpensive, and mechanically flexible. Although paper-based sensors have been developed, but important obstacles remian, which include the retention of chemical and mechanical stabilities when paper is wetted. Herein, we develop a simple and scalable process for fabrication of newspaper-based platforms by coating of parylene C and patterning of metal layers. As-prepared parylene C-coated newspaper (PC-paper) provides low-cost, disposable, and mechanically and chemically stable electrochemical platforms for the development of potentiometric ion sensors for the detection of electrolyte cations, such as, H+ and K+. The pH and K+ sensors produced show near ideal Nernstian sensitivity, good repeatability, good ion selectivity, and low potential drift. These disposable, flexible ion sensors based on PC-paper platforms could provide new opportunities for the development of point-of-care testing sensors, for diagnostics, healthcare, and environment testing.

High performance electrochemical glucose sensor based on three-dimensional MoS2/graphene aerogel.

Two-dimensional (2D) nanosheets have been extensively explored as electrode materials for the development of high-performance electrochemical biosensors due to their unique structural characteristics. Nevertheless, 2D nanosheets suffer from sheet aggregation issues limiting the electrical conductivity of layered metal sulfides or hydroxides. Here, we report high-performance glucose biosensors based on a three-dimensional (3D) aerogel composed of interconnected 2D MoS2 and graphene sheet. 3D MoS2/graphene aerogel (MGA) provides a large surface area for the effective immobilization of enzymes, and continuous framework of electrically conductive graphene sheets. Flow-injection amperometric evaluation of the glucose biosensor using a 3D MGA electrode exhibits a rapid response (∼4s), a linear detection range from 2 to 20mM, a sensitivity of 3.36µA/mM, and a low limit of detection of 0.29mM. Moreover, the interference response from oxidizable species, such as ascorbic acid, uric acid and dopamine is negligible at an operating potential of -0.45V.