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Graphene exhibits excellent physical, electronic, and chemical properties that are highly desirable for biosensing applications. However, most graphene biosensors are based on graphene lying flat on a substrate and therefore do not utilize its maximum specific surface area for ultrasensitive detection. Herein, we report the novel use of photonic annealing on a flexographically printed graphene-ethyl cellulose composite to produce vertically aligned graphene (VAG) biosensors for ultrasensitive detection of algal toxins in drinking water. These VAG structures, which maximized the specific surface area of graphene, were formed by partial removal of the polymeric binder upon applying intense pulsed light on the printed graphene. A label-free and low-cost VAG biosensor based on a non-faradaic electrochemical impedance spectroscopy technique was fabricated. The biosensor exhibited a limit of detection of 1.2 ng/L for microcystin-LR in local tap water. Such an ultrasensitive VAG biosensor is suitable for low-cost mass production using an integrated roll-to-roll flexographic printing with rapid photonic annealing technique.

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A comprehensive study was carried out on the dynamic viscosity of X30 silica dispersions at both high and low volume fractions of colloidal silica particles at various electrolyte ionic strength and pH values. Booth and Ruiz-Reina and Carrique theoretical models (R-R&C) were compared in predicting the primary electroviscous effect (PEE) for viscosity at low volume fractions. To this respect the colloidal dispersion was well characterised with regards to electrolyte properties such as the Debye length, κ-1, calculated from the ionic strength, and zeta potential, ζ, calculated from the electrophoretic mobility using the full numerical model by O'Brien and White (O'B&W). R-R&C hard sphere model (which is a modified version of Simha hard sphere model that includes a boundary condition by Happel on the outer radius of the cell) and the semi-empirical Krieger-Dougherty (K-D) models were fitted to the experimental data at high volume fractions. At both low and high volume fractions the viscosity increased with pH and decreased with ionic strength. At low volume fractions both theoretical models significantly underestimated the experimental dynamic viscosities obtained in this work. This could be attributed to the fuzzy structures for silica particles in aqueous conditions reported previously in the literature, where a significantly larger electroviscous parameter, p, was obtained experimentally for silica particles. The experimental electroviscous parameter, pexp, in this work was found to be roughly an order of magnitude up to 26 times larger than that predicted by Booth and around 5 ±â€¯1 times larger than the predicted p by R-R&C model allowing the introduction of a correction factor in the PEE coefficient obtained from R-R&C model enabling good prediction for X30 silica dispersions by the latter model. The significant improvement of the electroviscous effect predictions by R-R&C model compared to Booth model may be attributed to the limitations invalidating the Booth model at the electrolyte conditions in this study. At high volume fractions, the R-R&C hard sphere cell model, gave a much better fit to the experimental data compared to the K-D model, which also had the advantage of being only dependent on a coefficient that linearly relates an effective volume fraction postulated for the fuzzy silica particles to the experimental. The K-D model however, depends on the intrinsic viscosity, [η], which requires the calculation of the experimental slope of the dynamic viscosity against volume fraction in the dilute limit, and also on a maximum packing fraction as a fitting parameter. Due to the effect of the fuzzy structures on the viscosity, the latter effective volume fraction ϕeff was calculated using two approaches: (i) as a fitting parameter by fitting the R-R&C hard sphere model to the experimental viscosity data over the entire volume fraction range, and (ii) by fitting only the linear part of the experimental viscosity at low volume fractions, It is concluded that the R-R&C hard sphere model with the effective volume fraction accounting for the fuzzy structures fits reasonably well the full range of experimental results at low and high volume fractions. When the model was used with the Adamczyk effective volume fraction (i.e., considering only the dilute region in the fitting procedure), the predictions became worse at high volume fractions where significant deviations from the experimental results were found upon the increase of pH.

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In this study, a uniformly mixed sensing layer of typically immiscible compounds, such as tetrathiafulvalene (TTF) mediator and glucose oxidase (GOx) enzyme, was developed using a simultaneous spray deposition technique ideal for mass production of glucose sensors at low cost while exhibiting enhanced amperometric response. For comparison, the sensors were fabricated via three different methods: conventional drop-cast of TTF and GOx compounds in subsequent layers (DL), spray deposition of the compounds in subsequent layers (SL), and spray mixing of the compounds as one uniform layer (SM). Uniformity of the sensing layers was investigated via Scanning Electron Microscopy (SEM) and Energy Dispersive X-Ray Spectroscopy (EDX) techniques demonstrating an even distribution of the TTF and GOx throughout the sensing layer for the SM sensors. The amperometric studies showed a significantly larger maximum current response, Imax and sensitivity for the SM sensors as compared to the SL and DL sensors. The significantly better performance of the SM sensors correlated well with the even distribution of TTF and GOx throughout the sensing layer, resulting in enhanced electron transfer and redox reaction between GOx and TTF. The SM spray technique was then applied to deposit a uniformly mixed sensing layer on to 3D microneedle arrays to provide minimally invasive continuous glucose monitoring (CGM). In-vivo studies showed amperometric response from the microneedle CGM device was compatible to changes in blood glucose levels measured via the standard finger prick tests. Importantly, the deposition technique is suitable for mass production of the microneedle CGM at very low cost.

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In this work, the formation of a nanotextured surface is reported on flexographic printed zinc oxide thin films which provide an excellent platform for low-cost, highly sensitive biosensing applications. The ability to produce nanotextured surfaces using a high-throughput, roll-to-roll production method directly from precursor ink without any complicated processes is commercially attractive for biosensors that are suitable for large-scale screening of diseases at low cost. The zinc oxide thin film was formed by printing a zinc acetate precursor ink solution and annealing at 300 °C. An intricate nanotexturing of the film surface was achieved through 150 °C drying process between multiple prints. These surface nanostructures were found to be in the range of 100 to 700 nm in length with a width of 58 ± 18 nm and a height of between 20 and 60 nm. Such structures significantly increase the surface area to volume ratio of the biosensing material, which is essential to high sensitivity detection of diseases. Nonfaradaic electrochemical impedance spectroscopy measurements were carried out to detect the pp65-antigen of the human cytomegalovirus using the printed device, which has a low limit of detection of 5 pg/mL.

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