Antidelaminating, Thermally Stable, and Cost-Effective Flexible Kapton Platforms for Nitrate Sensors, Mercury Aptasensors, Protein Sensors, and p-Type Organic Thin-Film Transistors.

The inkjet printing of metal electrodes on polymer films is a desirable manufacturing process due to its simplicity but is limited by the lack of thermal stability and serious delaminating flaws in various aqueous and organic solutions. Kapton, adopted worldwide due to its superior thermal durability, allows the high-temperature sintering of nanoparticle-based metal inks. By carefully selecting inks (Ag and Au) and Kapton substrates (Kapton HN films with a thickness of 135 µm and a thermal resistance of up to 400 °C) with optimal printing parameters and simplified post-treatments (sintering), outstanding film integrity, thermal stability, and antidelaminating features were obtained in both aqueous and organic solutions without any pretreatment strategy (surface modification). These films were applied in four novel devices: a solid-state ion-selective (IS) nitrate (NO3-) sensor, a single-stranded DNA (ssDNA)-based mercury (Hg2+) aptasensor, a low-cost protein printed circuit board (PCB) sensor, and a long-lasting organic thin-film transistor (OTFT). The IS NO3- sensor displayed a linear sensitivity range between 10-4.5 and 10-1 M (r2 = 0.9912), with a limit of detection of 2 ppm for NO3-. The Hg2+ sensor exhibited a linear correlation (r2 = 0.8806) between the change in the transfer resistance (RCT) and the increasing concentration of Hg2+. The protein PCB sensor provided a label-free method for protein detection. Finally, the OTFT demonstrated stable performance, with mobility values in the linear (µlin) and saturation (µsat) regimes of 0.0083 ± 0.0026 and 0.0237 ± 0.0079 cm2 V-1 S-1, respectively, and a threshold voltage (Vth) of -6.75 ± 3.89 V.

Ionic Strength Influences on Biofunctional Au-Decorated Microparticles for Enhanced Performance in Multiplexed Colorimetric Sensors.

The rising development of biosensors offers a great potential for health, food, and environmental monitoring. However, in many colorimetric platforms, there is a performance limitation stemming from the tendency of traditional Au nanoparticles toward nonspecific aggregation in response to changing ionic strength (salt concentration). This work puts forward a new type of colorimetric aptamer-functionalized labeling of microparticles, which allows to leverage an increase in ionic strength as a positive driver of enhanced detection performance of analytical targets. The resulting device is a cost-effective, instrument-free, portable, and reliable aptasensor that serves as basis for the fabrication of universal paper-based colorimetric platforms with the capability of multiplex, multireplicates and provides quantitative colorimetric detection. A controlled fabrication process was demonstrated by keeping 90% of the signal obtained from the as-fabricated devices (n = 40) within ± 1 standard deviation (SD) (relative SD = 5.69%) and following a mesokurtic normal-like distribution (p = 0.385). We propose for the first time a salt-induced aggregation mechanism for highly stable multilayered label particles (ssDNA-PEI-Au-PS) as the basis of the detection scheme. The use of DNA aptamers as capture biomolecules and PEI as an encapsulating agent allows for a sensitive and highly specific colorimetric response. As a proof of concept, multiplexed detection of mercury (Hg2+) and arsenic (As3+) was demonstrated. In addition, we introduced a robust image analysis algorithm for testing zone segmentation and color signal quantification that allowed for analytical detection, reaching a limit of detection of 1 ppm for both targeted analytes, with enough evidence (p > 0.05) to prove the high specificity of the fabricated device versus a pool of possible interferent ions.

Competitive heavy metal adsorption onto new and aged polyethylene under various drinking water conditions.

The study goal was to identify factors that influence copper (Cu), iron (Fe), lead (Pb), manganese (Mn), and zinc (Zn) loading on new and aged low-density polyethylene (LDPE) under various drinking water conditions. The applied aging procedure increased LDPE surface area, hydrophilicity and the number of oxygen containing functional groups. Aged LDPE adsorbed up to a 5 fold greater metals than the new LDPE: Cu > Pb, Zn > Mn. Water pH (5.5 to 10.5) significantly altered LDPE surface metal loading. The organic carbon leached from plastic pipes inhibited Cu adsorption (-43.8%), but other metals were less impacted (-5.7% to -9.1%). The addition of free chlorine and corrosion inhibitor retarded metal adsorption to suspended LDPE materials. Overall, by changing water conditions total metal loadings (i.e., Cu, Mn, Pb and Zn) were altered 20.1 to 35.4%. When Fe was present, Cu (-4.0%) and Pb (-4.5%) loadings were reduced, while lesser impacts were found for Mn and Zn. Cu2+, Pb2+ and Zn2+ hydroxides and oxides were identified as the major metal deposit forms on the LDPE surface by XPS. To better predict metal fate in plastic piping systems, plastic surface characteristics, dissolved organics, water pH, hydraulic conditions and microbial growth should be considered.

Nisin infusion into surface cracks in oxide coatings to create an antibacterial metallic surface.

The efficacy of surface topology and chemistry on the ability for a surface to retain antimicrobial performance via the immobilization of a peptide was evaluated. A nanosecond pulsed laser was used to create oxide films on Ti-6Al-4V and 304L stainless steel. The laser conditions employed created a mudflat cracked surface on titanium, but no cracks on the steel. An antimicrobial peptide, nisin, was infused into the cracked and uncracked oxide surfaces to provide antimicrobial activity against Gram-positive bacteria; Listeria monocytogenes was chosen as the model microorganism. Release tests in distilled water at room temperature show that nisin is slowly liberated from the uncracked stainless steel surface, while there was no evidence of nisin liberation from the cracked titanium alloy surfaces, likely due to immobilization of the peptide into the artificially created micro-cracks on the surface of this alloy. Surfaces treated with nisin became active and exhibit anti-microbial performance against L. monocytogenes; this behavior is mostly retained after scrubbing/washing and simple immersion in water.

Aptamer-based SERS biosensor for whole cell analytical detection of E. coli O157:H7.

Infectious outbreaks caused by foodborne pathogens such as E. coli O157:H7 are still imposing a heavy burden for global food safety, causing acute illnesses and significant industrial impact worldwide. Despite the growth of biosensors as a research field, continuous innovation on detection strategies, novel materials and enhanced limits of detection, most of the platforms developed at the laboratory scale never will get to meet the market. The use of aptamers as capture biomolecules has been proposed as a promising alternative to overcome the harsh environmental conditions of industrial manufacturing processes, and to enhance the performance under real, complex, conditions. In this work, we present the feasibility of using aptameric DNA sequences, covalently conjugated to 4-aminothiophenol-gold nanoparticle complexes for the sensitive and highly specific detection of E. coli O157:H7 via surface enhanced Raman spectroscopy (SERS) analysis. Low concentrations of E. coli O157:H7 were detected and quantified within 20 min in both pure culture (∼101 CFU mL-1) and ground beef samples (∼102 CFU mL-1). The SERS intensity response showed a strong negative linear correlation (r2 = 0.995) with increasing concentrations of E. coli O157:H7 (ranging from 102 to 106 CFU mL-1). High specificity was achieved at genus (L. monocytogenes, S. aureus S. typhimurium) species (E. coli B1201) and serotype (E. coli O55:H7) level, demonstrating with 95% of confidence that the interferent microorganisms tested generated a Raman signal response not significantly different from the background (p = 0.786). This work evaluates the incorporation of aptameric DNA sequences as bio capture molecules exclusively. The successful performance presented using non-modified citrate reduced GNPs, is promising for potential low-cost, high-throughput applications. The findings might be applied simultaneously to the detection of a wide variety of foodborne pathogens in a multiplexed fashion employing unique Raman probes and strain-specific aptamer sequences.

Corrosion of upstream metal plumbing components impact downstream PEX pipe surface deposits and degradation.

Plastic pipes have been and are being installed downstream of metal drinking water plumbing components. Prior research has suggested that such pipe configurations may induce plastic pipe degradation and even system failure. To explore the impact of upstream metal plumbing components on downstream plastic pipes, field- and bench-scale experiments were conducted. Six month old galvanized iron pipes (GIPs) and downstream crosslinked polyethylene (PEX) pipes were exhumed from a residential home. Calcium, iron, manganese, phosphorous, and zinc were the most abundant elements on both GIPs and PEX pipes. Black and yellow deposits were found on some of the exhumed PEX pipe inner walls, which were mainly copper, iron, and manganese oxides (CuO, Cu(OH)2, Fe2O3, FeOOH and MnO2). Follow-up bench-scale experiments revealed that metal levels in the drinking water did not always predict metal loadings on plastic pipe surfaces. The pH 4 water resulted in a greater amount of metals released into the bulk water, but the pH 7.5 water resulted in a greater amount of metals deposited on the PEX pipe surfaces. Hot water (55 °C) induced a greater amount of organics released and higher metal loadings on PEX pipe surfaces at pH 7.5. ATR-FTIR analysis showed that at 55 °C, PEX pipes connected to copper and brass components had the greatest oxidation functional group peak intensity (COOC, CO, and COC). This study highlights potential downstream plastic pipe degradation and metal deposition, which may cause plumbing problems and failures for building owners, inhabitants, and water utilities.

Inkjet Printed Nanopatterned Aptamer-Based Sensors for Improved Optical Detection of Foodborne Pathogens.

The increasing incidence of infectious outbreaks from contaminated food and water supply continues imposing a global burden for food safety, creating a market demand for on-site, disposable, easy-to-use, and cost-efficient devices. Despite of the rapid growth of biosensors field and the generation of breakthrough technologies, more than 80% of the platforms developed at lab-scale never will get to meet the market. This work aims to provide a cost-efficient, reliable, and repeatable approach for the detection of foodborne pathogens in real samples. For the first time an optimized inkjet printing platform is proposed taking advantage of a carefully controlled nanopatterning of novel carboxyl-functionalized aptameric ink on a nitrocellulose substrate for the highly efficient detection of E. coli O157:H7 (25 colony forming units (CFU) mL-1 in pure culture and 233 CFU mL-1 in ground beef) demonstrating the ability to control the variation within ±1 SD for at least 75% of the data collected even at very low concentrations. From the best of the knowledge this work reports the lowest limit of detection of the state of the art for paper-based optical detection of E. coli O157:H7, with enough evidence (p > 0.05) to prove its high specificity at genus, species, strain, and serotype level.

Hybrid plasmonic Au-TiN vertically aligned nanocomposites: a nanoscale platform towards tunable optical sensing.

Tunable plasmonic structure at the nanometer scale presents enormous opportunities for various photonic devices. In this work, we present a hybrid plasmonic thin film platform: i.e., a vertically aligned Au nanopillar array grown inside a TiN matrix with controllable Au pillar density. Compared to single phase plasmonic materials, the presented tunable hybrid nanostructures attain optical flexibility including gradual tuning and anisotropic behavior of the complex dielectric function, resonant peak shifting and change of surface plasmon resonances (SPRs) in the UV-visible range, all confirmed by numerical simulations. The tailorable hybrid platform also demonstrates enhanced surface plasmon Raman response for Fourier-transform infrared spectroscopy (FTIR) and photoluminescence (PL) measurements, and presents great potentials as designable hybrid platforms for tunable optical-based chemical sensing applications.