Recent advances in 2D hexagonal boron nitride (2D-hBN) applied as the basis of electrochemical sensing platforms.

2D hexagonal boron nitride (2D-hBN) is a lesser utilised material than other 2D counterparts in electrochemistry due to initial reports of it being non-conductive. As we will demonstrate in this review, this common misconception is being challenged, and researchers are starting to utilise 2D-hBN in the field of electrochemistry, particularly as the basis of electroanalytical sensing platforms. In this critical review, we overview the use of 2D-hBN as an electroanalytical sensing platform summarising recent developments and trends and highlight future developments of this interesting, often overlooked, 2D material

Graphene Oxide Bulk-Modified Screen-Printed Electrodes Provide Beneficial Electroanalytical Sensing Capabilities

We demonstrate a facile methodology for the mass production of graphene oxide (GO) bulk-modified screen-printed electrodes (GO-SPEs) that are economical, highly reproducible and provide analytically useful outputs. Through fabricating GO-SPEs with varying percentage mass incorporations (2.5%, 5%, 7.5% and 10%) of GO, an electrocatalytic effect towards the chosen electroanalytical probes is observed, which increases with greater GO incorporated compared to bare/graphite SPEs. The optimum mass ratio of 10% GO to 90% carbon ink produces an electroanalytical signal towards dopamine (DA) and uric acid (UA) which is ca. ×10 greater in magnitude than that achievable at a bare/unmodified graphite SPE. Furthermore, 10% GO-SPEs exhibit a competitively low limit of detection (3σ) towards DA at ca. 81 nM, which is superior to that of a bare/unmodified graphite SPE at ca. 780 nM. The improved analytical response is attributed to the large number of oxygenated species inhabiting the edge and defect sites of the GO nanosheets, which are able to exhibit electrocatalytic responses towards inner-sphere electrochemical analytes. Our reported methodology is simple, scalable, and cost effective for the fabrication of GO-SPEs that display highly competitive LODs and are of significant interest for use in commercial and medicinal applications

2D‐Hexagonal Boron Nitride Screen‐Printed Bulk‐Modified Electrochemical Platforms Explored towards Oxygen Reduction Reactions

A low‐cost, scalable and reproducible approach for the mass production of screen‐printed electrode (SPE) platforms that have varying percentage mass incorporations of 2D hexagonal boron nitride (2D‐hBN) (2D‐hBN/SPEs) is demonstrated herein. These novel 2D‐hBN/SPEs are explored as a potential metal‐free electrocatalysts towards oxygen reduction reactions (ORRs) within acidic media where their performance is evaluated. A 5% mass incorporation of 2D‐hBN into the SPEs resulted in the most beneficial ORR catalysis, reducing the ORR onset potential by ca. 200 mV in comparison to bare/unmodified SPEs. Furthermore, an increase in the achievable current of 83% is also exhibited upon the utilisation of a 2D‐hBN/SPE in comparison to its unmodified equivalent. The screen‐printed fabrication approach replaces the less‐reproducible and time‐consuming dropcasting technique of 2D‐hBN and provides an alternative approach for the large‐scale manufacture of novel electrode platforms that can be utilised in a variety of application

Recent advances in portable heavy metal electrochemical sensing platforms

This Review explores the parameters to be engineered to design in situ electrochemical sensor platforms capable of meeting new EU regulation

Tailoring the electrochemical properties of 2D-hBN via physical linear defects: physicochemical, computational and electrochemical characterisation

Monolayer hexagonal-boron nitride films (2D-hBN) are typically reported within the literature to be electrochemically inactive due to their considerable band gap (ca. 5.2–5.8 eV). It is demonstrated herein that introducing physical linear defects (PLDs) upon the basal plane surface of 2D-hBN gives rise to electrochemically useful signatures. The reason for this transformation from insulator to semiconductor (inferred from physicochemical and computational characterisation) is likely due to full hydrogenation and oxygen passivation of the boron and/or nitrogen at edge sites. This results in a decrease in the band gap (from ca. 6.11 to 2.36/2.84 eV; theoretical calculated values, for the fully hydrogenated oxygen passivation at the N or B respectively). The 2D-hBN films are shown to be tailored through the introduction of PLDs, with the electrochemical behaviour dependent upon the surface coverage of edge plane-sites/defects, which is correlated with electrochemical performance towards redox probes (hexaammineruthenium(III) chloride and Fe2+/3+) and the hydrogen evolution reaction. This manuscript de-convolutes, for the first time, the fundamental electron transfer properties of 2D-hBN, demonstrating that through implementation of PLDs, one can beneficially tailor the electrochemical properties of this nanomateria

Mass-Producible 2D-MoS2‑Impregnated Screen-Printed Electrodes

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsami.7b05104Two-dimensional molybdenum disulfide (2D-MoS2) screen-printed electrodes (2D-MoS2-SPEs) have been designed, fabricated, and evaluated toward the electrochemical oxygen reduction reaction (ORR) within acidic aqueous media. A screen-printable ink has been developed that allows for the tailoring of the 2D-MoS2 content/mass used in the fabrication of the 2D-MoS2-SPEs, which critically affects the observed ORR performance. In comparison to the graphite SPEs (G-SPEs), the 2D-MoS2-SPEs are shown to exhibit an electrocatalytic behavior toward the ORR which is found, critically, to be reliant upon the percentage mass incorporation of 2D-MoS2 in the 2D-MoS2-SPEs; a greater percentage mass of 2D-MoS2 incorporated into the 2D-MoS2-SPEs results in a significantly less electronegative ORR onset potential and a greater signal output (current density). Using optimally fabricated 2D-MoS2-SPEs, an ORR onset and a peak current of approximately +0.16 V [vs saturated calomel electrode (SCE)] and −1.62 mA cm–2, respectively, are observed, which exceeds the −0.53 V (vs SCE) and −635 μA cm–2 performance of unmodified G-SPEs, indicating an electrocatalytic response toward the ORR utilizing the 2D-MoS2-SPEs. An investigation of the underlying electrochemical reaction mechanism of the ORR within acidic aqueous solutions reveals that the reaction proceeds via a direct four-electron process for all of the 2D-MoS2-SPE variants studied herein, where oxygen is electrochemically favorably reduced to water. The fabricated 2D-MoS2-SPEs are found to exhibit no degradation in the observed achievable current over the course of 1000 repeat scans. The production of such inks and the resultant mass-producible 2D-MoS2-SPEs mitigates the need to modify post hoc an electrode via the drop-casting technique that has been previously shown to result in a loss of achievable current over the course of 1000 repeat scans. The 2D-MoS2-SPEs designed, fabricated, and tested herein could have commercial viability as electrocatalytic fuel cell electrodes because of being economical as a result of their scales of economy and inherent tailorability. The technique utilized herein to produce the 2D-MoS2-SPEs could be adapted for the incorporation of different 2D nanomaterials, resulting in SPEs with the inherent advantages identified above

Nanodiamond based surface modified screen-printed electrodes for the simultaneous voltammetric determination of dopamine and uric acid.

From Europe PMC via Jisc Publications RouterHistory: ppub 2019-02-01, epub 2019-02-22Publication status: PublishedThe electroanalytical detection of the neurotransmitter dopamine (DA) in the presence of uric acid (UA) is explored for the first time using commercially procured nanodiamonds (NDs). These are electrically wired via surface modification upon screen-printed graphite macroelectrodes (SPEs). The surface coverage of the NDs on the SPEs was explored in order to optimize electroanalytical outputs to result in well-resolved signals and in low limits of detection. The (electro)analytical outputs are observed to be more sensitive than those achieved at bare (unmodified) SPEs. Such responses, previously reported in the academic literature have been reported to be electrocatalytic and have been previously attributed to the presence of surface sp2 carbon and oxygenated species on the surface of the NDs. However, XPS analysis reveals the commercial NDs to be solely composed of nonconductive sp3 carbon. The low/negligible electroconductivity of the NDs was further confirmed when ND paste electrodes were fabricated and found to exhibit no electrochemical activity. The electroanalytical enhancement, when using NDs electronically wired upon SPEs, is attributed not to the NDs themselves being electrocatalytic, as reported previously, but rather changes in mass transport where the inert NDs block the underlying electroactive SPEs and create a random array of graphite microelectrodes. The electrode was applied to simultaneous sensing of DA and UA at pH 5.5. Figures of merit include (a) low working potentials of around 0.27 and 0.35 V (vs. Ag/AgCl); and (b) detection limits of 5.7 × 10-7 and 8.9 × 10-7 M for DA and UA, respectively. Graphical abstract The electroanalytical enhancement of screen-printed electrodes modified with inert/non-conductive nanodiamonds is due to a change in mass transfer where the inert nanodiamonds facilitate the production of a random microelectrode array

Rapid antibiotic susceptibility testing using resazurin bulk modified screen-printed electrochemical sensing platforms

Urinary tract infections (UTIs) are one of the most common types of bacterial infection. UTIs can be associated with multidrug resistant bacteria and current methods of determining an effective antibiotic for UTIs can take up to 48 hours, which increases the chances of a negative prognosis for the patient. In this paper we report for the first time, the fabrication of resazurin bulk modified screen-printed macroelectrodes (R-SPEs) demonstrating them to be effective platforms for the electrochemical detection of antibiotic susceptibility in complicated UTIs. Using differential pulse voltammetry (DPV), resazurin was able to be detected down to 15.6 μM. R-SPEs were utilised to conduct antibiotic susceptibility testing (AST) of E. coli (ATCC® 25922) to the antibiotic gentamicin sulphate using DPV to detect the relative concentrations of resazurin between antibiotic treated bacteria, and bacteria without antibiotic treatment. Using R-SPEs, antibiotic susceptibility was determined after a total elapsed time of 90 minutes including the inoculation of the artificial urine, preincubation and testing time. The use of electrochemistry as a phenotypic means of identifying an effective antibiotic to treat a complicated UTI offers a rapid and accurate alternative to culture based methods for AST with R-SPEs offering an inexpensive and simpler alternative to other AST methods utilising electrochemical based approaches

3D printed graphene based energy storage devices

The final publication is available at Springer via http://dx.doi.org/10.1038/srep422333D printing technology provides a unique platform for rapid prototyping of numerous applications due to its ability to produce low cost 3D printed platforms. Herein, a graphene-based polylactic acid filament (graphene/PLA) has been 3D printed to fabricate a range of 3D disc electrode (3DE) configurations using a conventional RepRap fused deposition moulding (FDM) 3D printer, which requires no further modification/ex-situ curing step. To provide proof-of-concept, these 3D printed electrode architectures are characterised both electrochemically and physicochemically and are advantageously applied as freestanding anodes within Li-ion batteries and as solid-state supercapacitors. These freestanding anodes neglect the requirement for a current collector, thus offering a simplistic and cheaper alternative to traditional Li-ion based setups. Additionally, the ability of these devices’ to electrochemically produce hydrogen via the hydrogen evolution reaction (HER) as an alternative to currently utilised platinum based electrodes (with in electrolysers) is also performed. The 3DE demonstrates an unexpectedly high catalytic activity towards the HER (−0.46 V vs. SCE) upon the 1000th cycle, such potential is the closest observed to the desired value of platinum at (−0.25 V vs. SCE). We subsequently suggest that 3D printing of graphene-based conductive filaments allows for the simple fabrication of energy storage devices with bespoke and conceptual designs to be realised

Exploring the role of the connection length of screen-printed electrodes towards the hydrogen and oxygen evolution reactions

Zero-emission hydrogen and oxygen production are critical for the UK to reach net-zero greenhouse gasses by 2050. Electrochemical techniques such as water splitting (electrolysis) coupled with renewables energy can provide a unique approach to achieving zero emissions. Many studies exploring electrocatalysts need to “electrically wire” to their material to measure their performance, which usually involves immobilization upon a solid electrode. We demonstrate that significant differences in the calculated onset potential for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) can be observed when using screen-printed electrodes (SPEs) of differing connection lengths which are immobilized with a range of electrocatalysts. This can lead to false improvements in the reported performance of different electrocatalysts and poor comparisons between the literature. Through the use of electrochemical impedance spectroscopy, uncompensated ohmic resistance can be overcome providing more accurate Tafel analysis