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Food allergies are hypersensitivity immune responses triggered by (traces of) allergenic compounds in foods and drinks. The recent trend towards plant-based and lactose-free diets has driven an increased consumption of plant -based milks (PBMs) with the risk of cross-contamination of various allergenic plant-based proteins during the food manufacturing process. Conventional allergen screening is usually performed in the laboratory, but portable biosensors for on-site screening of food allergens at the production site could improve quality control and food safety. Here, we developed a portable smartphone imaging surface plasmon resonance (iSPR) biosensor composed of a 3D-printed microfluidic SPR chip for the detection of total hazelnut protein (THP) in commercial PBMs and compared its instrumentation and analytical performance with a conventional benchtop SPR. The smartphone iSPR shows similar characteristic sensorgrams compared with the benchtop SPR and enables the detection of trace levels of THP in spiked PBMs with the lowest tested concentration of 0.625 mu g/mL THP. The smartphone iSPR achieved LoDs of 0.53, 0.16, 0.14, 0.06, and 0.04 mu g/mL THP in 10x-diluted soy, oat, rice, coconut, and almond PBMs, respectively, with good correlation with the conventional benchtop SPR system (R2 0.950-0.991). The portability and miniaturized characteristics of the smartphone iSPR biosensor platform make it promising for the future on-site detection of food allergens by food producers., Funding Agencies|European Unions Horizon 2020 [720325]

A new radially expanding conducting polymer microactuator is presented. The radially expanding micro-actuators are used as electroactive gates in an electrically controlled microparticle sieve. A novel configuration to dynamically filter particles of different sizes in a microfluidic chip is conceptualized. Micropillars of SU-8 combined with conducting polymers to provide the radial actuation are positioned in a microfluidic chip with a specifically designed 3D printed housing to allow for selective filtration of microparticles with varied sizes. These pillar-shaped microactuators of polypyrrole actuate radially to function as dynamic gates for the fluidic channel, controlling the porosity of the filter allowing for the filtration of specific size of microparticles. This sieve design provides user defined channel width modulation with external stimuli. Photolithography and electrochemical polymerizations are combined with additive manufacturing to fabricate the individual func-tional parts of the microfluidic filter. To demonstrate the new conceptual filter design, we have shown filtration of microparticles of the sizes 60, 80, 90 and 100 mu m by electrically actuating micropillars of the dynamic gate. The flow and aggregation of the microparticles were analysed at the dynamic gates to characterize the perfor-mance of the filter., Funding Agencies|EU Marie Sklodowska-Curie Actions Initial Training Network MICACT [641822]; Swedish Research Council [2014-3079]; Linkoping University

An innovative modular approach for facile design and construction of flexible microfluidic biosensor platforms based on a dry manufacturing "craft-and-stick" approach is developed. The design and fabrication of the flexible graphene paper electrode (GPE) unit and polyethylene tetraphthalate sheet (PET)6/adhesive fluidic unit are completed by an economic and generic xurographic craft approach. The GPE widths and the microfluidic channels can be constructed down to 300 mu m and 200 mu m, respectively. Both units were assembled by simple double-sided adhesive tapes into a microfluidic integrated GPE (MF-iGPE) that are flexible, thin (<0.5 mm), and lightweight (0.4 g). We further functionalized the iGPE with Prussian blue and glucose oxidase for the fabrication of MF-iGPE glucose biosensors. With a closed-channel PET fluidic pattern, the MF-iGPE glucose biosensors were packaged and sealed to protect the integrated device from moisture for storage and could easily open with scissors for sample loading. Our glucose biosensors showed 2 linear dynamic regions of 0.05-1.0 and 1.0-5.5 mmol L-1 glucose. The MF-iGPE showed good reproducibility for glucose detection (RSD < 6.1%, n = 6) and required only 10 mu L of the analyte. This modular craft-and-stick manufacturing approach could potentially further develop along the concept of paper-crafted model assembly kits suitable for low-resource laboratories or classroom settings., Funding Agencies|Royal Golden Jubilee Ph.D. Scholarship from the Thailand Research Fund under the Office of the Prime Ministry, the Royal Thai Government [PHD/0213/2560]

We developed a fully integrated smart sensing device for on-site testing of food to detect trace formaldehyde (FA). A nano-palladium grafted laser-induced graphene (nanoPd@LIG) composite was synthesized by one-step laser irradiation of a symbolscript precursor. The composite was synthesized in the form of a three-electrode sensor on a polymer substrate. The electrochemical properties and morphology of the fabricated composite were characterized and the electrochemical kinetics of FA oxidation at the nanoPd@LIG electrode were investigated. The nanoPd@LIG electrode was combined with a smart electrochemical sensing (SES) device to determine FA electrochemically. The proposed SES device uses near field communication (NFC) to receive power and transfer data between a smartphone interface and a battery-free sensor. The proposed FA sensor exhibited a linear detection range from 0.01 to 4.0 mM, a limit of detection of 6.4 mu M, good reproducibility (RSDs between 2.0 and 10.1%) and good anti-interference properties for FA detection. The proposed system was used to detect FA in real food samples and the results correlated well with the results from a commercial potentiostat and a spectrophotometric analysis., Funding Agencies|International Research Network (IRN) [IRN62W0002]; Center of Excellence for Trace Analysis and Biosensor; Forensic Science Innovation and Service Center, Center of Excellence for Innovation in Chemistry (PERCH-CIC) , Ministry of Higher Education, Science, Research and Innovation, Graduate School, Division of Health and Applied Sciences, Division of Physical Sc; Forensic Science Innovation and Service Center; Center of Excellence for Innovation in Chemistry (PERCH-CIC); Ministry of Higher Education, Science, Research and Innovation, Graduate School, Division of Health and Applied Sciences, Division of Physical Science, Faculty of Science, Prince of Songkla University, Hat Yai, Thailand

The design of a smartphone imaging surface plasmon resonance (Smart-iSPR) system integrated with an affordable 3D-printed microfluidic SPR chip fabricated via a facile manufacturing approach could pave the way towards the development of miniaturized and integrated smartphone iSPR biosensors for emerging point-of-use applications. Conventional smartphone-based SPR systems using soft photolithography for the fabrication of microfluidics SPR chips are costly, labour-intensive and required a specially-equipped light-controlled environment, that is inadequate and mismatched with the consumer-based smartphone detection platform. Herein, we report the design, fabrication and testing of an innovative print-and-stick unibody microfluidics coupled SPR chip for smartphone iSPR. The 3Dprinted microfluidics (~V0.006) is assembled via an aptly-sized adhesive tape with the gold SPR sensing surface. Such a simple integrated microfluidic SPR chip with the print-and-stick configuration has a high resistance to fluid leakages at the channel-to-sensor interface with pressure up to 66.9 Pa and the tubingto-inset interfaces with pressure up to 86.9 Pa. The smartphone iSPR platform weighs 138 g and with a dimension of around 70 x 60 x 40 mm3, and its performance was characterized using a standard Biacore (R) 02-microglobulin calibration kit. The sensorgrams obtained by the smartphone iSPR show all the typical characteristics for surface functionalization, association and dissociation events. The smartphone iSPR responds linearly to 02-microglobulin within the range of 10-200 nM (R2 = 0.986) with a limit-ofdetection (LOD) of 1.5 nM. Given the miniaturized feature and simple camera-based imaging smartphone iSPR, the analytical performance is satisfactory when compared with the analytical dynamic range of 2 -32 nM described in the Biacore (R) protocol.(c) 2022 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/b, Funding Agencies|European UnionEuropean Commission [720325]

We present a low-cost, accessible, and rapid fabrication process for electrochemical microfluidic sensors. This work leverages the accessibility of consumer-grade electronic craft cutters as the primary tool for patterning of sensor electrodes and microfluidic circuits, while commodity materials such as gold leaf, silver ink pen, double-sided tape, plastic transparency films, and fabric adhesives are used as its base structural materials. The device consists of three layers, the silver reference electrode layer at the top, the PET fluidic circuits in the middle and the gold sensing electrodes at the bottom. Separation of the silver reference electrode from the gold sensing electrodes reduces the possibility of cross-contamination during surface modification. A novel approach in mesoscale patterning of gold leaf electrodes can produce generic designs with dimensions as small as 250 mu m. Silver electrodes with dimensions as small as 385 mu m were drawn using a plotter and a silver ink pen, and fluid microchannels as small as 300 mu m were fabricated using a sandwich of iron-on adhesives and PET. Device layers are then fused together using an office laminator. The integrated microfluidic electrochemical platform has electrode kinetics/performance of Delta E-p = 91.3 mV, I-pa/I-pc = 0.905, characterized by cyclic voltammetry using a standard ferrocyanide redox probe, and this was compared against a commercial screen-printed gold electrode (Delta E-p = 68.9 mV, I-pa/I-pc = 0.984). To validate the performance of the integrated microfluidic electrochemical platform, a catalytic hydrogen peroxide sensor and enzyme-coupled glucose biosensors were developed as demonstrators. Hydrogen peroxide quantitation achieves a limit of detection of 0.713 mM and sensitivity of 78.37 mu A mM(-1) cm(-2), while glucose has a limit of detection of 0.111 mM and sensitivity of 12.68 mu A mM(-1) cm(-2). This rapid process allows an iterative design-build-test cycle in under 2 hours. The upfron, Funding Agencies|Ministry of Higher Education, MalaysiaMinistry of Education, Malaysia [FRGS17-030-0596]; Asian Office of Aerospace Research and Development (AOARD) [FA23861814105, FA23861814048]

Tailoring conducting polymers (CPs) such as polyaniline (PANI) to deliver the appropriate morphology, electrochemical properties and processability is essential for the development of effective polymer-based electrochemical sensors and biosensors. Composite PANI electrodes for the detection of ammonium (NH4+) have been previously reported, but have been limited by their reliance on the electrocatalytic reaction between NH4+ and a metal/nano-catalyst. We report an advanced processable and nanofibrous polyaniline:polystyrene-sulphonate (nano-PANI:PSS) as a functional ink for the fabrication of catalyst-free NH4+ sensors and enzyme-coupled urea biosensors. The PSS provides both a soft-template for nanofibre formation and a poly-anionic charge compensator, enabling the detection of NH4+ based on an intrinsic doping/de-doping mechanism. The nanostructured morphology, chemical characteristics and electrochemical properties of the nano-PANI:PSS were characterised. We fabricated 3D-hierarchical sensor interfaces composed of inter-connected nano-PANI:PSS fibres (diameter of similar to 50.3 +/- 4.8 nm) for the detection of NH4+ with a wide linear range of 0.1-11.5 mM (R-2 = 0.996) and high sensitivity of 10(6) mA M-1 cm(-2). We further demonstrated the coupling of the enzyme urease with the nanoPANI:PSS to create a urea biosensor with an innovative biocatalytic product-to-dopant relay mechanism for the detection of urea, with a linear range of 0.2-0.9 mM (R-2 = 0.971) and high sensitivity of 41 mA M-1 cm(-2). Moreover, the nano-PANI:PSS-based sensors show good selectivity for the detection of NH4+ and urea in a urine model containing common interfering molecules. This processable and fibrous nano-PANI:PSS provides new advance on CP-based transducer materials in the emerging field of printed organic sensors and biosensors., Funding Agencies|TUBITAKTurkiye Bilimsel ve Teknolojik Arastirma Kurumu (TUBITAK) [2214A]

Extracellular matrix (ECM) components govern a range of cell functions, such as migration, proliferation, maintenance of stemness, and differentiation. Cell niches that harbor stem-/progenitor cells, with matching ECM, have been shown in a range of organs, although their presence in the heart is still under debate. Determining niches depends on a range of in vitro and in vivo models and techniques, where animal models are powerful tools for studying cell-ECM dynamics; however, they are costly and time-consuming to use. In vitro models based on recombinant ECM proteins lack the complexity of the in vivo ECM. To address these issues, we present the spatiotemporal extracellular matrix model for studies of cell-ECM dynamics, such as cell niches. This model combines gentle decellularization and sectioning of cardiac tissue, allowing retention of a complex ECM, with recellularization and subsequent image processing using image stitching, segmentation, automatic binning, and generation of cluster maps. We have thereby developed an in situ representation of the cardiac ECM that is useful for assessment of repopulation dynamics and to study the effect of local ECM composition on phenotype preservation of reseeded mesenchymal progenitor cells. This model provides a platform for studies of organ-specific cell-ECM dynamics and identification of potential cell niches.

Flexible electronics have gained more attention for emerging electronic devices such as sensors, biosensors, and batteries with advantageous properties including being thin, lightweight, flexible, and low-cost. The development of various forms of allotropic carbon papers provided a new dry-manufacturing route for the fabrication of flexible and wearable electronics, while the electrochemical performance and the bending stability are largely influenced by the bulk morphology and the micro-/nanostructured domains of the carbon papers. Here, we evaluate systematically the intrinsic physicoelectrochemical properties of allotropic carbon-based conducting papers as flexible electrodes including carbon-nanotubes-paper (CNTs-paper), graphene-paper (GR-paper), and carbon-fiber-paper (CF-paper), followed by functionalization of the allotropic carbon papers for the fabrication of flexible electrodes. The morphology, chemical structure, and defects originating from the allotropic nanostructured carbon materials were characterized by scanning electron microscopy (SEM) and Raman spectroscopy, followed by evaluating the electrochemical performance of the corresponding flexible electrodes by cyclic voltammetry and electrochemical impedance spectroscopy. The electron-transfer rate constants of the CNTs-paper and GR-paper electrodes were similar to 14 times higher compared with the CF-paper electrode. The CNTs-paper and GR-paper electrodes composed of nanostructured carbon showed significantly higher bending stabilities of 5.61 and 4.96 times compared with the CF-paper. The carbon-paper flexible electrodes were further functionalized with an inorganic catalyst, Prussian blue (PB), forming the PB-carbon-paper catalytic electrode and an organic conducting polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), forming the PEDOT-carbon-paper capacitive electrode. The intrinsic attribute of different allotropic carbon electrodes affects the deposition of PB and PEDOT, leading to different ele, Funding Agencies|Swedish Research CouncilSwedish Research CouncilEuropean Commission [VR-2015-04434]; Royal Golden Jubilee Ph.D. program (RGJ) from the Thailand Research Fund [PHD/0212/2560]

Flexible skin patch biosensors are promising for the noninvasive determination of physiological parameters in perspiration for fitness and health monitoring. However, various prerequisites need to be met for the development of such biosensors, including the creation of a flexible conductive platform, bending/contact stability, fast electrochemical kinetics, and immobilization of biomolecules. Here, we describe a conducting polymer-reinforced laser-irradiated graphene (LIG) network as a heterostructured three-dimensional (3D) transducer for flexible skin patch biosensors. LIG with a hierarchically interconnected graphene structure is geometrically patterned on polyimide via localized laser irradiation as a flexible conductive platform, which is then reinforced by poly(3,4-ethylenedioxythiophene) (PEDOT) as a conductive binder (PEDOT/LIG) with improved structural/contact stability and electrochemical kinetics. The interconnected pores of the reinforced PEDOT/LIG function as a 3D host matrix for high loading of "artificial" (Prussian blue, PB) and natural enzymes (lactate oxidase, LOx), forming a compact and heterostructured 3D transducer (LOx/PB-PEDOT/LIG) for lactate biosensing with excellent sensitivity (11.83 mu A mM-1). We demonstrated the fabrication of flexible skin patch biosensors comprising a custom-built integrated three-electrode system achieve amperometric detection of lactate in artificial sweat over a wide physiological linear range of 0-18 mM. The advantage of this facile and versatile transducer is further illustrated by the development of a folded 3D wristband lactate biosensor and a dual channel biosensors for simultaneous monitoring of lactate and glucose. This innovative design concept of a heterostructured transducer for flexible biosensors combined with a versatile fabrication approach could potentially drive the development of new wearable and skin-mountable biosensors for monitoring various physiological parameters in biofluids for noninvasive, Funding Agencies|Swedish Research CouncilSwedish Research CouncilEuropean Commission [VR-2015-04434]

Diabetes has become a major health problem in society. Invasive glucometers, although precise, only provide discrete measurements at specific times and are unsuitable for long-term monitoring due to the injuries caused on skin and the prohibitive cost of disposables. Remote, continuous, self-monitoring of blood sugar levels allows for active and better management of diabetics. In this work, we present a radio frequency (RF) sensor based on a stepped impedance resonator for remote blood glucose monitoring. When placed on top of a human hand, this RF interdigital sensor allows detection of variation in blood sugar levels by monitoring the changes in the dielectric constant of the material underneath. The designed stepped impedance resonator operates at 3.528 GHz with a Q factor of 1455. A microfluidic device structure that imitates the blood veins in the human hand was fabricated in PDMS to validate that the sensor can measure changes in glucose concentrations. To test the RF sensor, glucose solutions with concentrations ranging from 0 to 240 mg/dL were injected into the fluidic channels and placed underneath the RF sensor. The shifts in the resonance frequencies of the RF sensor were measured using a network analyzer via its S-11 parameters. Based on the change in resonance frequencies, the sensitivity of the biosensor was found to be 264.2 kHz/mg center dot dL(-1) and its LOD was calculated to be 29.89 mg/dL.

Precise and high-resolution coupling of functional proteins with micro-transducers is critical for the manufacture of miniaturized bioelectronic devices. Moreover, electrochemistry on microelectrodes has had a major impact on electrochemical analysis and sensor technologies, since the small size of microelectrode affects the radial diffusion flux of the analyte to deliver enhanced mass transport and electrode kinetics. However, a large technology gap has existed between the process technology associated with such microelectronics and the conventional bio-conjugation techniques that are generally used. Here, we report on a high-resolution and rapid geometric protein self-patterning (GPS) method using solvent-assisted protein-micelle adsorption printing to couple biomolecules onto microelectrodes with a minimum feature size of 5 mu m and a printing time of about a minute. The GPS method is versatile for micropatterning various biomolecules including enzymes, antibodies and avidin-biotinylated proteins, delivering good geometric alignment and preserving biological functionality. We further demonstrated that enzyme-coupled microelectrodes for glucose detection exhibited good electrochemical performance which benefited from the GPS method to maximize effective signal transduction at the bio-interface. These microelectrode arrays maintained fast convergent analyte diffusion displaying typical steady-state characteristics, fast response times, good linear sensitivity (0.103 nA mm(-2) mM(-1), R-2 = 0.995) and an ultra-wide linear dynamic range (2-100 mM). Our findings provide a new technical solution for the precise and accurate coupling of biomolecules to a microelectronic array with important implications for the scaleup and manufacture of diagnostics, biofuel cells and bioelectronic devices that could not be realized economically by other existing techniques., Funding Agencies|JSPS KAKENHIMinistry of Education, Culture, Sports, Science and Technology, Japan (MEXT)Japan Society for the Promotion of ScienceGrants-in-Aid for Scientific Research (KAKENHI) [JP19H02587]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [VR-2015-04434]

This paper presents the current progress towards a lab-on-chip biosensor for early dengue detection, consisting of an integrated sensor with dual-function working electrode that enables in-situ measurements of both electrochemical impedance spectroscopy (EIS) and quartz crystal microbalance (QCM) enclosed in a miniaturized 3D-printed package equipped with electrical contacts and sample fluid delivery to the quartz biosensor array. The sensors consist of an array of three 10 MI-lz IEQCM biosensors on a single quartz substrate. Early validation is performed for future dengue sensing application. We report the design, optimisation, and fabrication of the sensors, as well as early optimisation and validation of surface bioconjugation of antibodies. This lab-on-chip has the potential to provide accurate dengue detection due to its high sensitivity and dynamic range, as well as providing rapid and early dengue detection in point-of-care settings., Funding Agencies|Swedish Research CouncilSwedish Research CouncilEuropean Commission [2014-4254]; Malaysian Ministry of Higher Education [FRGS15-217-0458]; French National Research Agency under the Investments for the Future programFrench National Research Agency (ANR) [ANR-10-LABX-0074-01]

Polypyrrole magnetic microspheres were synthesized and used to extract carbaryl, carbofuran, and methomyl before analysis by a high-performance liquid chromatography with diode array detection. Under optimal conditions, four times the preconcentration was achieved with the use of only 1.2 mL of sample. Good linearity with ranges of 3.0–7.5 × 103, 6.0–4.5 × 103, and 15–3.0 × 103 ng kg−1 and limits of detection of 1.37 ± 0.10, 4.7 ± 1.2, and 10.1 ± 5.7 ng kg−1 were obtained, respectively. Good reproducibility (RSDs < 5%) was achieved over 24 cycles of extraction and regeneration. Good accuracy (recoveries 81.6 ± 1.5%–108.3 ± 2.2%) and good precision (RSDs 0.11%–4.5%) were obtained. Carbaryl was detected in apple (2.75 ± 0.23 ng kg−1), carbofuran in tomato (11.34 ± 0.61 ng kg−1), and methomyl in watermelon (34.7 ± 1.7 ng kg−1). The relative expanded uncertainty of the measurement method was less than 14% for all three pesticides., Funding agencies: The Center of Excellence for Innovation in Chemistry (PERCH-CIC), Ministry of Higher Eduation, Science, Research and Innovation (MHESI), Thailand.

The rapidly emerging field of organic bioelectronics has witnessed the wide use of conducting polymers (CPs) to fabricate advanced chemically modified electrodes (CMEs) for biosensors and biomedical devices. The electrochemical performance of the CPs in such devices is closely related to the quality and physiochemical nature of the dopants. A bi-functional graphene oxide derivative with high reduction degree and negatively-charged sulphonate functionality, i.e. sulphonate-coupled reduced graphene oxide (S-RGO), was developed and used as an efficient dopant for a CP with enhanced electrochemical performance. The S-RGO was synthesised via a facile one-pot hydrothermal reaction using 4-hydrazinobenzosulphonic acid (4-HBS) as reductant and sulphonate precursor simultaneously. The resulting S-RGO possesses high aqueous dispersion stability (more than 6 months), high electrical conductivity (1493.0 S m−1) and sulphonate functionality. Due to these specific properties, S-RGO demonstrated improved electropolymerisation efficiency for poly(3,4-ethylenedioxythiophene) (PEDOT) proving an effective dopant for the preparation of a PEDOT:S-RGO film (5 mC) with faster polymerisation time (37 s) compared to the conventional 2D dopants GO (PEDOT:GO, 129 s) and RGO (PEDOT:RGO, 66 s). The resulting PEDOT:S-RGO appeared as a homogenous film with uniformly distributed S-RGO dopant, low equivalent series resistance and low charge transfer resistance. Moreover, the electrochemical transduction performance of the PEDOT:S-RGO interface was evaluated with 4 different analytes, including ferric/ferrocyanide redox probe, dopamine, nicotinamide adenine dinucleotide and hydrogen peroxide. As a result of the synergistic effect of S-RGO and PEDOT, the PEDOT:S-RGO demonstrated enhanced electrochemical performance with respect to faster electrode kinetics (smaller ΔEp), ∼2 and ∼4 times increased current responses, and lower peak potentials compared to PEDOT:GO and PEDOT:RGO. This bi-functional S-RGO, Funding agencies: Swedish Research CouncilSwedish Research Council [VR-2015-04434]; China Scholarship CouncilChina Scholarship Council [201606910036]

This paper highlights the design, simulation and fabrication of an array of twelve integrated electrochemical - quartz crystal microbalance (IEQCM) sensors on a single substrate for liquid sensing. Integration of both measurement techniques is made possible by combining the three electrode electrochemical device with the top and bottom electrodes for the microbalance. Important design parameters such as the working electrode radius and gap spacing, were studied using both theoretical calculations and COMSOL Multiphysics® finite element simulations. The sensor’s working electrode radius affects the magnitude of the frequency response while the gap affects the capacitance and current density which are important for electrochemical measurements. It was found that the best values for the working electrode radius was 2 mm and gap spacing was 0.5 mm. The sensors were fabricated using microfabrication techniques for the gold electrode and screen printing techniques for the reference electrode. Water contact angle, atomic force microscopy, and scanning electron microscope were utilized to study the surface roughness of the IEQCM sensor. IEQCM has a low contact angle of 53.0 ± 1° and low surface roughness of 1.92nm. For liquid sensing, an array of circular chambers were fabricated using polydimethylsiloxane (PDMS) and placed on top of the quartz substrate for liquid testing. Electrochemical measurements and cyclic voltammetry were performed using the sensor in ferri-ferrocyanide and phosphate buffered saline solution to study the function of scan rates on the peak current with respect to the potential difference. For mass sensing measurements, liquid water droplets of 1uL - 10 uL were placed onto the sensing surface and the change in resonance frequencies of the sensors were measured. These resonance frequency changes can be converted in mass change/area in accordance to the advanced Sauerbrey equation. The multichannel IEQCM sensor shows good potential as a parallel sens, Funding agencies: Swedish Research CouncilSwedish Research Council [VR-2014-43058]; Malaysian Ministry of Higher Education [FRGS15-217-0458]

The oxygen reduction reaction (ORR) is an essential process in electrocatalysis limiting the commercialization of sustainable energy conversion technologies, such as fuel cells. The use of conducting polymers as molecular porous and conducting catalysts obtained from the high abundance elements enables the route towards low cost and high-throughput fabrication of disposable plastic electrodes of fuel cells. Poly(3,4-ethylenedioxythiophene) (PEDOT) is a 2-electron ORR electrocatalyst yielding specifically hydrogen peroxide that limits the full utilization of chemical energy of oxygen. Here, we demonstrated an innovative product-to-intermediate relay approach achieving complete oxygen reduction reaction (cORR) with Prussian blue (PB) integrated microporous PEDOT cathode in fuel cells. The microporous structured PEDOT electrode prepared via a simple cryosynthesis allows the bulk integration and stabilization of the poor conducting PB co-catalyst into the PEDOT ion-electron conductor, while the microporous PEDOT allows effective oxygen diffusion into the matrix. We evaluated systematically the effect of sequential PEDOT 2-electron ORR followed by PB co-catalysis launching hydrogen peroxide reduction reaction (HPRR) into H2O. This resulted in the establishment of electronic and ionic transport between PEDOT and PB catalyst enabling the combination of enhanced ORR electrocatalysis by means of the ORR course extension from 2to 4-electron reduction to achieve cORR. The cORR performance delivered by the product-to-intermediate relay between microporous PEDOT and PB co-catalysis led to a four times increase in power density of model proton-exchange membrane fuel cell (PEMFC) assembled from the polymer-based air breathing cathode., Funding Agencies|National Science and Technology Development Agency (NSTDA); Ministry of Science and Technology of Thailand; Swedish Research CouncilSwedish Research Council [VR 2019-05577, VR 2015-04434]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO Mat LiU) [2009 00971]

Conducting polymers that possess good electrochemical properties, nanostructured morphology and functionality for bioconjugation are essential to realise the concept of all-polymer-based biosensors that do not depend on traditional nanocatalysts such as carbon materials, metal, metal oxides or dyes. In this research, we demonstrated a facile approach for the simultaneous preparation of a bi-functional PEDOT interface with a tunable 3D nanofibmus network and carboxylic acid groups (i.e. Nano-PEDOT-COOH) via controlled co-polymerisation of EDOT and EDOT-COOH monomers, using tetrabutylammonium perchlorate as a soft-template. By tuning the ratio between EDOT and EDOT-COOH monomer, the nanofibmus structure and carboxylic acid functionalisation of Nano-PEDOT-COOH were varied over a fibre diameter range of 15.6 +/- 3.7 to 70.0 +/- 9.5 nm and a carboxylic acid group density from 0.03 to 0.18 mu mol cm(-2). The nanofibres assembled into a three-dimensional network with a high specific surface area, which contributed to low charge transfer resistance and high transduction activity towards the co-enzyme NADH, delivering a wide linear range of 20-960 jiM and a high sensitivity of 0.224 mu A mu M-1 cm(-2) at the Nano-PEDOT-COOH50% interface. Furthermore, the carboxylic acid groups provide an anchoring site for the stable immobilisation of an NADH-dependent dehydmgenase (i.e. lactate dehydrogenase), via EDC/S-NHS chemistry, for the fabrication of a Bio-Nano-PEDOT-based biosensor for lactate detection which had a response time of less than 10 s over the range of 0.05-1.8 mM. Our developed bio-Nano-PEDOT interface shows future potential for coupling with multi-biorecognition molecules via carboxylic acid groups for the development of a range of advanced all-polymer biosensors., Funding Agencies|Swedish Research CouncilSwedish Research Council [VR-2015-04434]; China Scholarship CouncilChina Scholarship Council [201606910036]

Modulation of chemical functional groups on conducting polymers (CPs) provides an effective way to tailor the physicochemical properties and electrochemical performance of CPs, as well as serves as a functional interface for stable integration of CPs with biomolecules for organic bioelectronics (OBEs). Herein, we introduced a facile approach to modulate the carboxylate functional groups on the PEDOT interface through a systematic evaluation on the effect of a series of carboxylate-containing molecules as counterion dopant integrated into the PEDOT backbone, including acetate as monocarboxylate (mono-COO-), malate as dicarboxylate (di-COO-), citrate as tricarboxylate (tri-COO-), and poly(acrylamide-co-acrylate) as polycarboxylate (poly-COO-) bearing different amounts of molecular carboxylate moieties to create tunable PEDOT:COO- interfaces with improved polymerization efficiency. We demonstrated the modulation of PEDOT:COO- interfaces with various granulated morphologies from 0.33 to 0.11 mu m, tunable surface carboxylate densities from 0.56 to 3.6 mu M cm(-2), and with improved electrochemical kinetics and cycling stability. We further demonstrated the effective and stable coupling of an enzyme model lactate dehydrogenase (LDH) with the optimized PEDOT:poly-COO- interface via simple covalent chemistry to develop biofunctionalized PEDOT (Bio-PEDOT) as a lactate biosensor. The biosensing mechanism is driven by a sequential bioelectrochemical signal transduction between the bio-organic LDH and organic PEDOT toward the concept of all-polymer-based OBEs with a high sensitivity of 8.38 mu A mM(-1) cm(-2) and good reproducibility. Moreover, we utilized the LDH-PEDOT biosensor for the detection of lactate in spiked serum samples with a high recovery value of 91-96% and relatively small RSD in the range of 2.1-3.1%. Our findings provide a new insight into the design and optimization of functional CPs, leading to the development of new OBEs for sensing, biosensing, bioenginee, Funding Agencies|Swedish Research CouncilSwedish Research Council [VR-2015-04434]; Thailand Science Research and Innovation (TSRI) [IRN62W0002]; Royal Golden Jubilee Ph.D program (RGJ) from the Thailand Research Fund [PHD/0212/2559]; Development and Promotion of Science and Technology Talents projects (DPST) from the Royal Thai Government

The rapidly developing field of conducting polymers in organic electronics has many implications for bioelectronics. For biosensing applications, tailoring the functionalities of the conducting polymers surface is an efficient approach to improve both sensitivity and selectivity. Here, we demonstrated a facile and economic approach for the fabrication of a high-density, negatively charged carboxylic-acid-group-functionalized PEDOT (PEDOT:COOH) using an inexpensive ternary carboxylic acid, citrate, as a dopant. The polymerization efficiency was significantly improved by the addition of LiClO4 as a supporting electrolyte yielding a dense PEDOT:COOH sensing interface. The resulting PEDOT:COOH interface had a high surface density of carboxylic acid groups of 0.129 mu mol/cm(2) as quantified by the toluidine blue O (TBO) staining technique. The dopamine response measured with the PEDOT:COOH sensing interface was characterized by cyclic voltammetry with a significantly reduced Delta E-p of 90 mV and a 3-fold increase in the I-pa value compared with those of the nonfunctionalized PEDOT sensing interface. Moreover, the cyclic voltammetry and electrochemical impedance spectroscopy results demonstrated the increased electrode kinetics and highly selective discrimination of dopamine (DA) in the presence of the interferents ascorbic acid (AA) and uric acid (UA), which resulted from the introduction of negatively charged carboxylic acid groups. The negatively charged carboxylic acid groups could favor the transfer, preconcentration, and permeation of positively charged DA to deliver improved sensing performance while repelling the negatively charged AA and UA interferents. The PEDOT:COOH interface facilitated measurement of dopamine over the range of 1-85 mu M, with a sensitivity of 0.228 mu A mu M-1, which is 4.1 times higher than that of a nonfunctionalized PEDOT electrode (0.055 mu A mu M-1). Our results demonstrate the feasibility of a simple and economic fabrication of a hi, Funding Agencies|Swedish Research CouncilSwedish Research Council [VR-2015-04434]; China Scholarship CouncilChina Scholarship Council [201606910036]

The nitrocellulose (NC) membrane based lateral flow immunoassay device (LFID) is one of the most important and widely used biosensor platforms for point-of-care (PoC) diagnostics. However, the analytical performance of LFID has limitations and its optimization is restricted to the bioassay chemistry, the membrane porosity, and the choice of biolabel system. These bottom neck technical issues resulted from the fact that the conventional LFID design principle has not evolved for many years, which limited the LFID for advanced biosensor applications. Here we introduce a new dimension for LFID design and optimization based on geometric flow control (GFC) of NC membranes, leading to highly sensitive GFC-LFID. This novel approach enables comprehensive flow control via different membrane geometric features such as the width (w) and the length (l) of a constriction, as well as its input angle (?1) and output angle (?2). The GFC-LFID (w=0.5 mm, l=7 mm, ?1= 60, ?2= 45) attained a 10-fold increase in sensitivity for detection of interleukin-6 (IL-6), compared with conventional LFID, whereas reducing by 10-fold the antibody consumption. The GFC-LFID detects IL-6 over a linear range of 0.1-10?ng/mL with a limit of detection (LoD) of 29?pg/mL, which even outperforms some commercial IL-6 LFIDs. Such significant improvement is attained by pure geometric control of the NC membrane, without additives, that only relaying on a simple high throughput laser ablation procedure suitable for integration on regular large-scale manufacturing of GFC-LFIDs. Our new development on GFC-LFID with the combination of facile scalable fabrication process, tailored flow control, improved analytical performance, and reduced antibodies consumption is likely to have a significant impact on new design concept for the LFID industry.

Current electrochemical biosensors for multiple miRNAs require tedious immobilization of various nucleic acid probes. Here, we demonstrate an innovative approach using a generic neutravidin biosensor combined with electrochemically encoded responsive nanolabels for facile and simultaneous multiplexed detection of miRNA-21 and miRNA-141. The selectivity of the biosensor arises from the intrinsic properties of the electrochemically encoded responsive nanolabels, comprising biotinylated molecular beacons (biotin-MB) and metal nanoparticles (metal-NPs). The procedure is a simple one-pot assay, where the targeted miRNA causes the opening of biotin-MB followed by capturing of the biotin-MB-metal-NPs by the neutravidin biosensor and simultaneous detection of the captured metal-NPs by stripping square-wave voltammetry (SSWV). The multiplexed detection of miRNA-21 and miRNA-141 is achieved by differentiation of the electrochemical signature (i.e., the peak current) for the different metal-NP labels. The biosensor delivers simultaneous detection of miRNAs with a linear range of 0.5-1000 pM for miRNA-21 and a limit of detection of 0.3 pM (3 sigma/sensitivity, n = 3), and a range of 50-1000 pM for miRNA-141, with a limit of detection of 10 pM. Furthermore, we demonstrate multiplexed detection of miRNA-21 and miRNA-141 in a spiked serum sample., Funding Agencies|EU-FP7 project [PIRSES-GA-2012-318053]

Conducting polymers, with unique ion/electron transfer capability, reversible doping/dedoping and controllable chemical and electrochemical properties, have received many attention as advanced interfaces in electronic and bioelectronic devices. Recent advancement is focus on fine-tailoring the conducting polymer interfaces with addition functionality and controlled morphology with enhanced performance beyond its intrinsic properties. Here, we demonstrate the tailoring of physico-chemical properties of poly (3,4-ethylenedioxythiophene) (PEDOT) with high density carboxyl functionality and tailored nano-structure, and its application in dopamine sensing and lactate biosensing with enhanced selectivity and sensitivity. For dopamine sensing, we developed a high-density negatively-charged carboxyl functionalized PEDOT interface using a low-cost organic acid citrate as dopant. Citrate contains a high content of carboxyl functionality and small size allowing well distribution of the citrate dopant within the PEDOT with a high surface carboxyl density upto 26 µM/cm2. The carboxyl confined PEDOT interface with nano-globular structure showed increased electrode kinetics and increased discriminationof dopamine from interferences (ascorbic acid and uric acid). For lactate biosensing, we further developed a nano-fibrillar carboxyl PEDOT interface that can detect dihydronicotinamide adenine dinucleotide (NADH) at low potential at ~0.43 V. Based on the post-immobilisation of NAD-dependent lactate dehydrogenase via carboxyl coupling, lactate biosensor was developed with good analytical performance and low operation potential to reduce interferences. These results demonstrated tailoring of physico-chemical properties of PEDOT interface with improved sensing performance, thus could potentially applied for next generation bioelectronic devices such as wearable and flexible sensors and biosensors.

Dengue is an infectious mosquito-borne viral disease that affects approximately 50 million people annually worldwide and is prevalent mostly in the tropics. Severe cases of dengue can be fatal, making early detection and fast diagnosis crucial towards improving patient care and survival rates. Currently, early detection can be achieved through detection of NS1 protein, using ELISA technique. Unfortunately, ELISA is an expensive method, making it unsuitable as a screening technique, especially in low-resource settings. In this work, we present a prototype device and its early validation studies, of an integrated electrochemical and mass-sensor for dengue NS1 antigen. The sensor is connected to open source mass-sensing software and hardware, OpenQCM which makes it easily portable. Having dual-measurement capabilities (mass and impedance) increases the sensitivity of the sensor. Preliminary studies suggest that the prototype could achieve ultralow limit of detection as low as 10 ng mL-1, dual-sensing cross-validation capability, portable size, time of less than 30 minutes, and parallelization of multiple assays. This work could lead to early and accurate dengue detection in routine point-of-care settings.

This work describes the development of a miniaturized sensing system for continuous and real time monitoring of adenosine triphosphate (ATP) bioluminescence based on highly sensitive Silicon Photomultiplier (SiPM) coupled to highly versatile 3D printed lab-on-chip (LoC).