Preparation and Comparison of Hydrolase-Coated Plastics

Polypropylene and polyethylene were coated with alpha-Chymotrypsin (a-CT) or subtilisin Carlsberg (SubC) or Burkholderia cepacia lipase (lipase BC) by different immobilization procedures, such as physical adsorption and covalent linking. This latter procedure was based on the chemical functionalization of the plastic surface by oxygen gas plasma treatment. Immobilization of the enzyme was carried out by using as cross-linking agent i) glutaraldehyde (GA) or ii) N’-diisopropylcarbodiimide (DIC) and N-hydroxysuccinimide (NHS). The effects of duration of the plasma treatment and the type of the immobilization procedure on the transesterification activity of the enzyme were investigated. In general polypropylene resulted a better support than polyethylene. Moreover, a-CT showed higher transesterification activity when immobilized with GA, while for SubC, DIC and NHS were better cross-linking agents than GA. No activity was observed with these enzymes when immobilization was carried out by physical adsorption. On the contrary, lipase BC immobilized by physical adsorption was even more active than the free enzyme. Concerning thermal stability, immobilized SubC was less stable than the free enzyme. Overall, these results show that plastics endowed with biocatalytic properties could be obtained by simple immobilization protocols and that optimal immobilization conditions depend on the type of starting plastic, plasma treatment, cross-linking method, and the nature of the enzyme

Single-use disposable electrochemical label-free immunosensor for detection of glycated hemoglobin (HbA1c) using differential pulse voltammetry (DPV)

A single-use disposable in vitro electrochemical immunosensor for the detection of HbA1c in undiluted human serum using differential pulse voltammetry (DPV) was developed. A three-electrode configuration electrochemical biosensor consisted of 10-nm-thin gold film working and counter electrodes and a thick-film printed Ag/AgCl reference electrode was fabricated on a polyethylene terephthalate (PET) substrate. Micro-fabrication techniques including sputtering vapor deposition and thick-film printing were used to fabricate the biosensor. This was a roll-to-roll cost-effective manufacturing process making the single-use disposable in vitro HbA1c biosensor a reality. Self-assembled monolayers of 3-Mercaptopropionic acid (MPA) were employed to covalently immobilize anti-HbA1c on the surface of gold electrodes. Electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS) confirmed the excellent coverage of MPA-SAM and the upward orientation of carboxylic groups. The hindering effect of HbA1c on the ferricyanide/ferrocyanide electron transfer reaction was exploited as the HbA1c detection mechanism. The biosensor showed a linear range of 7.5-20 μg/mL of HbA1c in 0.1 M PBS. Using undiluted human serum as the test medium, the biosensor presented an excellent linear behavior (R2 = 0.999) in the range of 0.1-0.25 mg/mL of HbA1c. The potential application of this biosensor for in vitro measurement of HbA1c for diabetic management was demonstrated

Synergic photocatalytic effect between TiO2 and a fluorinated transparent ionomeric material in the oxidation of hydrosoluble pollutants in turbid suspensions

The crystal violet (CV) dye has been chosen to study the photooxidation activity of titanium dioxide immobilized into a transparent fluoropolymeric matrix toward organic pollutants. The photoactive matrix was directly coated on the UV source by applying a TiO2 containing fluorinated ionomeric dispersion and a perfluorinated transparent amorphous polymer in an appropriate sequence. The photocatalytic activity of the multilayered coating towards the hydrosoluble organic CV dye was evaluated in transparent solution and in highly turbid suspension. The turbidity was obtained by dispersing insoluble microparticles of calcium sulfate in the polluted aqueous solution. The photoabatement rates obtained in transparent and in turbid conditions were 0.0918 min-1 and 0.0300 min-1, respectively. The TiO2 nanoparticle dispersed in the fluorinated matrix revealed a higher photocatalytic activity than simple dispersed TiO2 in both transparent as well as turbid conditions. The immobilization of the catalyst in a stable fluorinated matrix avoided the TiO2 separation and prevented catalyst losses. The synergism in the activity between the TiO2-based photocatalyst and the fluorinated matrix was particularly evident at low pollutant concentrations

Graphene Flake Self-Assembly Enhancement via Stretchable Platforms and External Mechanical Stimuli

While the green production and application of 2D functional nanomaterials, such as graphene flakes, in films for stretchable and wearable technologies is a promising platform for advanced technologies, there are still challenges involved in the processing of the deposited material to improve properties such as electrical conductivity. In applications such as wearable biomedical and flexible energy devices, the widely used flexible and stretchable substrate materials are incompatible with high-temperature processing traditionally employed to improve the electrical properties, which necessitates alternative manufacturing approaches and new steps for enhancing the film functionality. We hypothesize that a mechanical stimulus, in the form of substrate straining, may provide such a low-energy approach for modifying deposited film properties through increased flake packing and reorientation. To this end, graphene flakes were exfoliated using an unexplored combination of ethanol and cellulose acetate butyrate for morphological and percolative electrical characterization prior to application on polydimethylsiloxane (PDMS) substrates as a flexible and stretchable electrically conductive platform. The deposited percolative free-standing films on PDMS were characterized via in situ resistance strain monitoring and surface morphology measurements over numerous strain cycles, with parameters extracted describing the dynamic modulation of the film’s electrical properties. A reduction in the film resistance and strain gauge factor was found to correlate with the surface roughness and densification of a sample’s (sub)surface and the applied strain. High surface roughness samples exhibited enhanced reduction in resistance as well as increased sensitivity to strain compared to samples with low surface roughness, corresponding to surface smoothing, which is related to the dynamic settling of graphene flakes on the substrate surface. This procedure of incorporating strain as a mechanical stimulus may find application as a manufacturing tool/step for the routine fabrication of stretchable and wearable devices, as a low energy and compatible approach, for enhancing the properties of such devices for either high sensitivity or low sensitivity of electrical resistance to substrate strain

Nickel Phosphides Fabricated through a Codeposition–Annealing Technique as Low-Cost Electrocatalytic Layers for Efficient Hydrogen Evolution Reaction

Water splitting will be one of the most strategic techniques in the upcoming hydrogen-based economy. In this context, the development of efficient and low-cost Pt-free electrocatalysts is crucial t..

Biocompatible rapid few-layers-graphene synthesis in aqueous lignin solutions

Ultrasonic-Assisted Liquid Phase Exfoliation (UALPE) is considered one of the most promising approaches for the scale-up of graphene production. The process is based on the isolation and stabilization of layers of 2D materials, such as graphene: the selection of a proper stabilizing/exfoliating agent is crucial to achieve a stable Few-Layers-Graphene (FLG) dispersion. In the present work we propose the use of alkali lignin (AL) as a polymeric stabilizing agent for the rapid ( ≤3 hours) synthesis of FLG. Sonication time and graphite-to-lignin (Gr/AL) ratios were investigated as the primary operational parameters to identify the optimal working conditions. Spectroscopical characterization of the samples were employed to assess the quality of the synthesized material: the analysis of the Raman and XPS spectra provided insight on the number of layers and the nature of the limited defects introduced with the exfoliation procedure. Low-defectivity FLG was obtained at Gr/AL = 8 and a sonication time of 3 hours. Furthermore, Scan- ning Electron Microscopy and Dynamic Light Scattering were performed to investigate the size of the exfoliated flakes ( ∼400 nm). The procedure proposed represents a rapid route for the synthesis of FLG, which will be further explored for composites in chemiresistive devices

Multi-dimensional microwave sensing using graphene waveguides

This paper presents an electrolytically gated broadband microwave sensor where atomically-thin graphene layers are integrated into coplanar waveguides and coupled with microfluidic channels. The interaction between a solution under test and the graphene surface causes material and concentration-specific modifications of graphene's DC and AC conductivity. Moreover, wave propagation in the waveguide is modified by the dielectric properties of materials in its close proximity via the fringe field, resulting in a combined sensing mechanism leading to an enhanced S-parameter response compared to metallic microwave sensors. The possibility of further controlling the graphene conductivity via an electrolytic gate enables a new, multi-dimensional approach merging chemical field-effect sensing and microwave measurement methods. By controlling and synchronizing frequency sweeps, electrochemical gating and liquid flow in the microfluidic channel, we generate multidimensional datasets that enable a thorough investigation of the solution under study. As proof of concept, we functionalize the graphene surface in order to identify specific single-stranded DNA sequences dispersed in phosphate buffered saline solution. We achieve a limit of detection of ~1 attomole per litre for a perfect match DNA strand and a sensitivity of ~3 dB/decade for sub-pM concentrations. These results show that our devices represent a new and accurate metrological tool for chemical and biological sensing

Preface—JES focus issue on ubiquitous sensors and systems for IoT

This focus issue of the Journal of The Electrochemical Society (JES) is devoted to Ubiquitous Sensors and Systems for IoT. Ubiquitous sensors are becoming an integral part of Internet of Things (IoT) applications, and progress in this domain can be seen each month. The promise is that everyone and everything will be connected via wireless data collection, and services like healthcare will be brought to everyone, everywhere, anytime, for virtually any need