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Sildenafil is used to treat erectile dysfunction and pulmonary arterial hypertension but is often illicitly added to energy drinks and chocolates. This study introduces a lateral flow strip test using aptamers specific to sildenafil for detecting its illegal presence in food. The process involved using graphene oxide SELEX to identify high-affinity aptamers, which were then converted into molecular gate structures on mesoporous silica nanoparticles, creating a unique signaling system. This system was integrated into lateral flow chromatography strips and tested on buffers and chocolate samples containing sildenafil. The method simplifies the lateral flow assay (LFA) for small molecules and provides a tool for signal amplification. The detection limit for these strips was found to be 68.2 nM (31.8 µg/kg) in spiked food samples.

Background: Sildenafil (SIL) is regarded as an illegal adulterant in functional foods. Some functional foods doped with SIL have posed significant concern about their safety risks. However, the facile colorimetric detection of SIL is rarely investigated., Results: Herein, we prepared a monodispersed spherical composite nanozyme (Fe 3 O 4 -NH 2 /GONRs), possessing excellent peroxidase-like (POD-like) and catalase-like (CAT-like) activities and strong superparamagnetic property. The enzyme-like activities of Fe 3 O 4 -NH 2 /GONRs can be selectively inhibited by SIL due to the synergistic effect of hydrogen bonds and π-π stacking between Fe 3 O 4 -NH 2 /GONRs and SIL. Leveraging this mechanism, a highly sensitive and selective colorimetric detection for SIL with a detection limit (LOD) of 0.26 ng/mL was developed. In addition, we prepared a three-dimensional paper-based analytical device (3D-PAD) for SIL colorimetric detection with naked-eyes and the semi-quantitative analysis with a LOD of 88 ng/mL., Significance: The proposed colorimetric and PAD detections demonstrated the advantages of low-cost, highly sensitive and selective, thus have promise application potential in the rapid detection of adulterated functional foods., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Due to intrinsic defect of fire hazard security, improving the flame retardant capacity of paper is still insufficient in case of precombustion. Herein, we integrate the flame retardant with flame detection performance on the surface of paper, the restricts of graphene oxide (GO) are overcome between high thermoelectric performance and flexibility. A flexible lamellar thermoelectric composite (GO-LA-HP) is constructed through the co-assembly of GO, ascorbic acid (LA), and phenoxycycloposphazene (HP), lamellar GO-LA-HP avoid GO's toughness decline after modification, but also enhance fire sensitivity and flame resistance. The composite could significantly decrease the temperature rise stage (<150 °C), and trigger the fire-warning within 2 s. The hybrid coating composed of phytic acid/phosphoric acid (PyA/PA) and modified thermoelectric GO-LA-HP becomes excellent compatibility on the surface of the modified paper (GPP). GPP is able to extinguish itself immediately after leaving the fire in the vertical combustion, and display the excellent flame resistance. Furthermore, GPP's alarm signal could be timely generated as little as 3 s of contacting the flame, and the response time can exceed 600 s. According to the structure observation and analysis, the related synergistic fire detection reinforcing and flame-retardant mechanisms are also proposed and clarified., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier B.V.)

Easy, economical, and swift detecting tools are very demanded for assaying various chemical species. The introduction of label-free paper-based read-out devices has significantly reached the demand of analytical science for target analytes assays. Herein, a facile, and disposable inexpensive paper-based sensing tool was fabricated for sensing As 3+ ion using graphene quantum dots (GQDs) as a fluorescent reader. The CA-GQDs were synthesized using citric acid (CA) as a precursor via the pyrolysis method, further physisorbed on the cellulose substrate for sensing of As 3+ via aggregation-based fluorescence "turn-off" mechanism. The linear range for quantitating As 3+ ion is in the range of 0.05-50 μM with a detection limit of 10 nM. The practical application of the CA-GQDs-based analytical platform was verified by assaying As 3+ ion in water samples. The CA-GQDs-embedded paper strip can be easily extended for assaying of As 3+ ion, which meets the demand for monitoring of As 3+ ion in real samples., (© 2024 John Wiley & Sons, Ltd.)

Timely and rapid detection of antibiotic residues in the environment is conducive to safeguarding human health and promoting an ecological virtuous cycle. A foldable paper-based photoelectrochemical (PEC) sensor was successfully developed for the detection of ampicillin (AMP) based on glutathione/zirconium dioxide hollow nanorods/aptamer (GSH@ZrO 2 HS@apt) modified cellulose paper as a reactive zone with laser direct-writing lead sulfide/cadmium sulfide/graphene (PbS/CdS/LIG) as photoelectrode and cobalt hydroxide (CoOOH) as a photoresist material. Initially, AMP was introduced into the paper-based reaction zone as a biogate aptamer, which specifically recognized the target and then left the ZrO 2 HS surface, releasing glutathione (GSH) encapsulated inside. Subsequently, the introduction of GSH into the reaction region and etching of CoOOH nanosheets to expose the PbS/CdS/LIG photosensitive material increased photocurrent. Under optimal conditions, the paper-based PEC biosensor showed a linear response to AMP in the range of 5.0 - 2 × 10 4 pM with a detection limit of 1.36 pM (S/N = 3). In addition, the constructed PEC sensing platform has excellent selectivity, high stability and favorable reproducibility, and can be used to assess AMP residue levels in various real water samples (milk, tap water, river water), indicating its promising application in environmental antibiotic detection., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Background: Okadaic acid (OA), as a diarrhetic shellfish poisoning, can increase the risk of acute carcinogenic or teratogenic effects for the ingestion of OA contaminated shellfish. At present, much effort has been made to graft immunoassay onto a paper substrate to make paper-based sensors for rapid and simple detection of shellfish toxin. However, the complicated washing steps and low protein fixation efficiency on the paper substrate need to be further addressed., Results: A novel paper-tip immunosensor for detecting OA was developed combined with smartphone and naked eye readout. The trapezoid paper tip was consisted of quantitative and qualitative detection zones. To improve the OA antigen immobilization efficiency on the paper substrate, graphene oxide (GO)-assisted protein immobilization method was introduced. Meanwhile, Au nanoparticles composite probe combined with the lateral flow washing was developed to simplify the washing step. The OA antigen-immobilized zone, as the detection zone Ⅰ, was used for quantitative assay by smartphone imaging. The paper-tip front, as the detection zone Ⅱ, which could qualitatively differentiate OA pollution level within 45 min using the naked eye. The competitive immunoassay on the paper tip exhibited a wide linear range for detecting OA (0.02-50 ng∙mL -1 ) with low detection limit of 0.02 ng∙mL -1 . The recovery of OA in spiked shellfish samples was in the range of 90.3 %-113.%., Significance: These results demonstrated that the proposed paper-tip immunosensor could provide a simple, low-cost and high-sensitivity test for OA detection without the need for additional large-scale equipment or expertise. We anticipate that this paper-tip immunosensor will be a flexible and versatile tool for on-site detecting the pollution of marine products., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

A one-shot CO 2 laser-based strategy to generate conductive reduced graphene oxide (rGO) decorated with nanoceria (nCe) is proposed. The 2D/0D rGO-nCe films, integrated as catalytic sensing layers in paper-based sensors, were employed for on-site monitoring of indoor fogging treatments against Listeria monocytogenes (Lm), a ubiquitous pathogenic bacterium. The rGO-nCe laser-assisted synthesis was optimized to preserve the rGO film morphological and electron-transfer features and simultaneously integrate catalytic nCe. The films were characterized by microscopical (SEM), spectroscopical (EDX, Raman, and FTIR), and electrochemical techniques. The most performing film was integrated into a nitrocellulose substrate, and the complete sensor was assembled via a combination of xurography and stencil printing. The rGO-nCe sensor's catalytic activity was proved toward the detection of H 2 O 2 , obtaining sensitive determination (LOD = 0.3 µM) and an extended linear range (0.5-1500 µM). Eventually, the rGO-nCe sensor was challenged for the real-time continuous monitoring of hydrogen peroxide aerosol during no-touch fogging treatment conducted following the EU's recommendation for biocidal product use. Treatment effectiveness was proved toward three Lm strains characterized by different origins, i.e., type strain ATCC 7644, clinical strain 338, and food strain 641/6II. The sensor allows for discrimination and quantification treatments at different environmental biocidal amounts and fogging times, and correlates with the microbiological inhibition, promoting the proposed sensor as a useful tool to modulate and monitor no-touch treatments., (© 2024. The Author(s).)

The exploration into nanomaterial-based nonenzymatic biosensors with superb performance in terms of good sensitivity and anti-interference ability in disease marker monitoring has always attained undoubted priority in sensing systems. In this work, we report the design and synthesis of a highly active nanocatalyst, i.e., palladium and platinum nanoparticles (Pt&Pd-NPs) decorated ultrathin nanoporous gold (NPG) film, which is modified on a homemade graphene paper (GP) to develop a high-performance freestanding and flexible nanohybrid electrode. Owing to the structural characteristics the robust GP electrode substrate, and high electrochemically catalytic activities and durability of the permeable NPG support and ultrafine and high-density Pt&Pd-NPs on it, the resultant Pt&Pd-NPs-NPG/GP electrode exhibits excellent sensing performance of low detection limitation, high sensitivity and anti-interference capability, good reproducibility and long-term stability for the detection of small molecular biomarkers hydrogen peroxide (H 2 O 2 ) and glucose (Glu), and has been applied to the monitoring of H 2 O 2 in different types of live cells and Glu in body fluids such as urine and fingertip blood, which is of great significance for the clinical diagnosis and prognosis in point-of-care testing.

Laser-induced graphene (LIG) has gained preponderance in recent years, as a very attractive material for the fabrication and patterning of graphitic structures and electrodes, for multiple applications in electronics. Typically, polymeric substrates, such as polyimide, have been used as precursor materials, but other organic, more sustainable, and accessible precursor materials have emerged as viable alternatives, including cellulose substrates. However, these substrates have lacked the conductive and chemical properties achieved by conventional LIG precursor substrates and have not been translated into fully flexible, wearable scenarios. In this work, we expand the conductive properties of paper-based LIG, by boosting the graphitization potential of paper, through the introduction of external aromatic moieties and meticulous control of laser fluence. Colored wax printing over the paper substrates introduces aromatic chemical structures, allowing for the synthesis of LIG chemical structures with sheet resistances as low as 5 Ω·sq -1 , translating to an apparent conductivity as high as 28.2 S·cm -1 . Regarding chemical properties, I D ratios of 0.28 showcase low defect densities of LIG chemical structures and improve on previous reports on paper-based LIG, where sheet resistance has been limited to values around 30 Ω·sq I , with more defect dense and less crystalline chemical structures. With these improved properties, a simple transfer methodology was developed, based on a water-induced peel-off process that efficiently separates patterned LIG structures from the native paper substrates to conformable, flexible substrates, harnessing the multifunctional capabilities of LIG toward multiple applications in wearable electronics. Proof-of concept electrodes for electrochemical sensors, strain sensors, and in-plane microsupercapacitors were patterned, transferred, and characterized, using paper as a high-value LIG precursor for multiples scenarios in wearable technologies, for improved sustainability and accessibility of such applications.G ratios of 0.28 showcase low defect densities of LIG chemical structures and improve on previous reports on paper-based LIG, where sheet resistance has been limited to values around 30 Ω·sq -1 , with more defect dense and less crystalline chemical structures. With these improved properties, a simple transfer methodology was developed, based on a water-induced peel-off process that efficiently separates patterned LIG structures from the native paper substrates to conformable, flexible substrates, harnessing the multifunctional capabilities of LIG toward multiple applications in wearable electronics. Proof-of concept electrodes for electrochemical sensors, strain sensors, and in-plane microsupercapacitors were patterned, transferred, and characterized, using paper as a high-value LIG precursor for multiples scenarios in wearable technologies, for improved sustainability and accessibility of such applications.

The exact fabrication of precise three-dimensional structures for piezoresistive sensors necessitates superior manufacturing methods or tooling, which are accompanied by time-consuming processes and the potential for environmental harm. Herein, we demonstrated a method for in situ synthesis of zinc oxide nanorod (ZnO NR) arrays on graphene-treated cotton and paper substrates and constructed highly sensitive, flexible, wearable, and chemically stable strain sensors. Based on the structure of pine trees and needles in nature, the hybrid sensing layer consisted of graphene-attached cotton or paper fibers and ZnO NRs, and the results showed a high sensitivity of 0.389, 0.095, and 0.029 kPa -1 and an ultra-wide linear range of 0-100 kPa of this sensor under optimal conditions. Our study found that water absorption and swelling of graphene fibers and the associated reduction of pore size and growth of zinc oxide were detrimental to pressure sensor performance. A random line model was developed to examine the effects of different hydrothermal times on sensor performance. Meanwhile, pulse detection, respiration detection, speech recognition, and motion detection, including finger movements, walking, and throat movements, were used to show their practical application in human health activity monitoring. In addition, monolithically grown ZnO NRs on graphene cotton sheets had been integrated into a flexible sensing platform for outdoor UV photo-indication, which is, to our knowledge, the first successful case of an integrated UV photo-detector and motion sensor. Due to its excellent strain detection and UV detection abilities, these strategies are a step forward in developing wearable sensors that are cost-controllable and high-performance.

Graphene paper (GP), a macroscopic self-supporting material, has exceptional flexibility and preserves the excellent physical and chemical properties of graphene nanomaterials. But its applications in regenerative medicine remain to be further explored. Here, we biologically functionalized GP with hydroxyapatite (HA) nanorods by the use of GP-binding peptides as an affinity linker. This strategy solved two daunting challenges for regenerative medicine applications of GP: the lack of good hydrophilicity for supporting cell growth and the difficulty in forming composites by binding with nanobiomaterials. Briefly, we first screened a high-affinity GP-binding peptide (TWWNPRLVYFDY) by the phage display technique. Then we chemically conjugated the GP-binding peptide to the synthetic HA nanorods. The GP-binding peptide on the resultant HA nanorods enabled them to be bound and assembled onto the GP substrate with high affinity, forming a GP-peptide-HA composite with significantly improved hydrophilicity of GP. The composite promoted the attachment and proliferation of mesenchymal stem cells (MSCs), demonstrating its outstanding biocompatibility. Due to the unique compositions of the composite, it was also found to induce osteogenic differentiation of MSCs in vitro in the absence of other inducers in the medium, by verifying the expression of the osteogenic markers including collagen-1, bone morphogenetic proteins 2, runx-related transcription factor 2, osteocalcin, and alkaline phosphatase. Our work suggests that the GP-binding peptide can be used to link inorganic nanoparticles onto GP to facilitate the biomedical applications of GP.

MicroRNAs (miRNAs), found in blood and body fluids, have emerged as potential non-invasive biomarkers for disease and injury. miRNAs are quantitatively evaluated using typical RNA analysis methods such as the quantitative reverse transcription polymerase chain reaction, microarrays, and Northern blot, all of which require complex procedures and expensive reagents. To utilize miRNAs as practical biomarkers, it will be helpful to develop simple and user-friendly sensors. In this study, a paper-based miRNA sensor was developed by combining two methods: (1) target-recycled DNAzyme (Dz) amplification and (2) graphene oxide-assisted Dz blotting on paper. The Dz spots on paper caused a miRNA-dependent color change in presence of colorimetric reagents and facilitated the quantification of absolute amount of the target miRNA, irrespective of the volume, with high reproducibility. This approach is technologically straightforward and enables quantification of as low as 7.75 fmol miRNA using a portable smartphone., (© 2021. The Author(s), under exclusive licence to Springer-Verlag GmbH Austria, part of Springer Nature.)

In this study, carbon papers and aerogels were prepared from chitosan and graphene layers with aldehydic edge functional groups (G-CHO) able to form chemical bonds with chitosan and thus to form a crosslinked network. A high surface area graphite was edge functionalized with hydroxyl groups (G-OH) through the reaction with KOH. G-CHO, with 4.5 mmol/g of functional group, was prepared from G-OH by means of the Reimer-Tieman reaction. Characterization of the graphitic materials was performed with elemental analysis, titration, X-ray analysis, Raman spectroscopy and by estimating their Hansen solubility parameters. CS and G-CHO were mixed with mortar and pestle and carbon papers and aerogels were obtained from a stable acidic water suspension through casting and liophilization, respectively. Free standing and foldable carbon papers and monolithic aerogels based on a continuous covalent network between G-CHO and CS were prepared. G-CHO, which had about 22 stacked layers, was extensively exfoliated in the carbon paper, as confirmed by the absence of the 002 reflection of the graphitic crystallites in the XRD pattern. Carbon paper was found to be resistant to solvents and to be stable for pH ⩾ 7. Composites revealed electrical conductivity. The covalent network between the graphene layers and CS, suggested by the IR findings, accounts for these results. This work demonstrates the effectiveness of a continuous covalent network between chitosan and graphene layers edge functionalized with tailor made functional groups for the preparation of carbon papers and aerogels and paves the way for the scale up of such a type of composites.

Hybrid nanomaterials fabricated by the heterogeneous integration of 1D (carbon nanotubes) and 2D (graphene oxide) nanomaterials showed synergy in electrical and mechanical properties. Here, we reported the infiltration of carboxylic functionalized single-walled carbon nanotubes (C-SWNT) into free-standing graphene oxide (GO) paper for better electrical and mechanical properties than native GO. The stacking arrangement of GO sheets and its alteration in the presence of C-SWNT were comprehensively explored through scanning electron microscopy, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction. The C-SWNTs bridges between different GO sheets produce a pathway for the flow of electrical charges and provide a tougher hybrid system. The nanoscopic surface potential map reveals a higher work function of the individual functionalised SWNTs than surrounded GO sheets showing efficient charge exchange. We observed the enhanced conductivity up to 50 times and capacitance up to 3.5 times of the hybrid structure than the GO-paper. The laminate of polystyrene composites provided higher elastic modulus and mechanical strength when hybrid paper is used, thus paving the way for the exploitation of hybrid filler formulation in designing polymer composites.

Herein, a three-dimensional graphene wall (GWs) and nano-Cu 2 O modified carbon fiber paper (CFP) electrode were used to develop a disposable and sensitive non-enzymatic glucose sensor. This sensing interface of GWs/Cu 2 O consists of an interlaced CFP on which intercrossed graphene walls (GWs) were vertically tethered in situ by radio frequency plasma enhanced chemical vapor deposition (RF-PECVD), and Cu 2 O nanoparticles (NPs) were evenly grew on the 3D GWs layer and skeleton through the complete thermal decomposition of copper acetate (Cu (CH 3 COO) 2 ) at high temperature. The CFP/GWs/Cu 2 O shows a large specific surface area and rich solution diffusion channels, which can expose more catalytic active sites without Nafion fixation film, thus greatly improving the electrocatalytic performance of this glucose sensor. The CFP/GWs/Cu 2 O sensor shows excellent catalytic performance to glucose with a linear detection range of 0.5 μM-5166 μM, LOD of 0.21 μM, and response time <4 s. This kind of disposable and sensitive electrode can capable of controlling uniform growth and accurate quantification, and has great development potential in the field of medical detection and the commercialization of wearable sensors., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

A simple and effective ratiometric fluorescence sensor of CdTe QDs/GCNNs for on-site and rapid analysis of Cu 2+ has been established by mixing physically CdTe QDs and graphite carbon nitride (GCNNs). Two emissions peaks of CdTe QDs at 572 nm and GCNNs at 436 nm are both excitated at 340 nm. Under a UV lamp, fluorescent of traffic yellow CdTe QDs is linearly quenched by Cu 2+ (as the detection signal), while blue GCNNs remains unchanged (as the reference), resulting in a distinguishable color change gradually from pink yellow to blue. The limit of detection (LOD) of this new sensor for Cu 2+ is as low as 0.47 ng mL -1 with 1.4 % RSD. The established method has been successfully applied to detection of Cu 2+ in various drinks with satisfactory results. Moreover, a paper-based sensor, which has been prepared by soaking cellulose acetate membrane in CdTe QDs/GCNNs sensor solution, has a wide semiquantitative detection range for Cu 2+ (0.01 ~ 5.0 μg mL -1 ). It has realized successfully on-site and rapid determination of Cu 2+ in red wine without any pretreatment procedure and is of great promotion and application value in determination of Cu 2+ in liquid samples., (© 2020 American Society for Photobiology.)

Pencils and papers are ubiquitous in our society and have been widely used for writing and drawing, because they are easy to use, low-cost, widely accessible, and disposable. However, their applications in emerging skin-interfaced health monitoring and interventions are still not well explored. Herein, we report a variety of pencil-paper-based on-skin electronic devices, including biophysical (temperature, biopotential) sensors, sweat biochemical (pH, uric acid, glucose) sensors, thermal stimulators, and humidity energy harvesters. Among these devices, pencil-drawn graphite patterns (or combined with other compounds) serve as conductive traces and sensing electrodes, and office-copy papers work as flexible supporting substrates. The enabled devices can perform real-time, continuous, and high-fidelity monitoring of a range of vital biophysical and biochemical signals from human bodies, including skin temperatures, electrocardiograms, electromyograms, alpha, beta, and theta rhythms, instantaneous heart rates, respiratory rates, and sweat pH, uric acid, and glucose, as well as deliver programmed thermal stimulations. Notably, the qualities of recorded signals are comparable to those measured with conventional methods. Moreover, humidity energy harvesters are prepared by creating a gradient distribution of oxygen-containing groups on office-copy papers between pencil-drawn electrodes. One single-unit device (0.87 cm 2 ) can generate a sustained voltage of up to 480 mV for over 2 h from ambient humidity. Furthermore, a self-powered on-skin iontophoretic transdermal drug-delivery system is developed as an on-skin chemical intervention example. In addition, pencil-paper-based antennas, two-dimensional (2D) and three-dimensional (3D) circuits with light-emitting diodes (LEDs) and batteries, reconfigurable assembly and biodegradable electronics (based on water-soluble papers) are explored., Competing Interests: The authors declare no competing interest.

A sonication of graphite in polysaccharide (pullulan, chitosan and alginate) is one of the viable methods for the preparation of few-layer graphene. However, the effect of these adsorbed polysaccharides on the electrical performance of the produced graphene so far is not yet clear. In order to investigate the present effect of pullulan, chitosan and alginate on the electrical characteristic of resulted graphene, we have produced few-layer graphene using bath sonication of graphite in pullulan, chitosan and alginate medium for the application as electrical conductive ink in strain-sensitive. Data from the TEM reveals the appearance of folded few-layer graphene flakes after sonication for 150 min while the XPS data shows that the chitosan-based graphene possesses the highest carbon-oxygen ratio of 7.2 as compared to that of the pullulan and alginate-based graphene. By subjecting the produced graphene as the ink for paper-based strain sensor, we have discovered that the chitosan-graphene has the best resistivity value (1.66 × 10 -3 Ω⋅cm) and demonstrate the highest sensitivity towards strain (GF: 18.6). This result interestingly implies the potential of the reported chitosan-based conductive ink as a strain-sensitive material for future food packaging., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Troponin T, which is a biomarker of cardiovascular disease, is vital for acute myocardial infarction (AMI). AMI is the most well-known cause of death in the world. In the present work, we designed a novel immunosensor using disposable, cheap, and very conductive graphite paper electrodes (GP). The proposed immunosensor was modified with hydrochloric acid (HCl) for immobilization of anti-TnT antibody. After carboxyl group formation on the surface, the GP electrodes were incubated with EDC/NHS pair as a cross-linker. Electrochemical impedance spectroscopy (EIS), single frequency impedance (SFI), cyclic voltammetry (CV) and square wave voltammetry (SWV) techniques were used for electrochemical characterization of the label-free immunosensor. Furthermore, the fabrication process of the proposed immunosensor was examined by using scanning electron microscopy (SEM). The proposed electrochemical immunosensor had a wide detection range (0.5 fg - 1000 fg/mL), and low limit of detection (LOD) and low limit of quantification (LOQ) at 1.28 fg/mL and 4.29 fg/mL, respectively. The designed immunosensor exhibited very good sensitivity, reproducibility, repeatability, reusability and long storage life. Additionally, the immunosensor was successfully applied to detection of TnT in human serum., (Copyright © 2020 Elsevier B.V. All rights reserved.)

The demand for high-quality graphene for electronic applications is increasing due to its high carrier mobility and electrical conductivity. In this connection, printing technology is a reliable method towards the fabrication of conductive, disposable graphene-based electrode for low-cost sensor application. Herein, we aimed to report the synthesis of high-quality graphene nanosheets obtained by electrochemical exfoliation of biomass-derived from corn cob. The conductive ink was prepared from this exfoliated graphene and was utilized for the preparation of paper-based graphene electrode towards double stranded DNA (dsDNA) sensor application. This paper, based graphene electrode opens the possibility of direct electrochemical analysis of analyte without any sample preparation. In this study, two irreversible oxide peaks were obtained from paper-based printed graphene electrode, corresponds to oxidation of guanine (G) and adenine (A) of dsDNA in the linear range of 0.2 pg mL -1 to 5 pg mL -1 with the detection limit of 0.68 pg mL -1 and the sensitivity of 0.00656 mA pg -1 cm -2 . Further, a small-scale printable circuit is fabricated using this graphene shows good conductivity of 1.145x10 3 (S/m)., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Norovirus is one of the leading causes of gastroenteritis, acute vomiting, intense diarrhoea, acute pain in the stomach, high fever, headaches, and body pain. Conventional methods of detection gave us very promising results but had disadvantages such as low sensitivity, cost ineffectiveness, reduced specificity and selectivity, etc. Therefore, biosensors can be a viable alternative device which can overcome all setbacks associated with the conventional method. An electrochemical sensor based on oxidized graphitic carbon nitride (Ox-g-C 3 N 4 ) modified electrochemical paper-based analytical device (ePAD) was fabricated for the detection of norovirus DNA. The synthesized Ox-g-C 3 N 4 nanosheets were characterized by field emission scanning electron microscopy (FESEM), X-ray Diffraction (XRD), UV-Vis spectroscopy and X-Ray Photoelectron Spectroscopy. The capture probe DNA (PDNA) modified electrodes were characterized by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). These two characterization techniques were also employed to find the optimal scan rate, response time and temperature of the fabricated sensor. The fabricated biosensor showed a limit of detection (LOD) of 100 fM. Furthermore, the specificity of the reported biosensor was affirmed by testing the response of capture probe DNA with oxidized graphitic carbon nitride (PDNA/Ox-g-C 3 N 4 ) modified ePAD on the introduction of a non-complimentary DNA. The fabricated ePAD sensor is easy to fabricate, cost effective and specific, and requires a minimum analysis time of 5 s.

We developed a paper-based analytical device based on the electropolymerization of poly (3,4-ethylenedioxythipohene) (PEDOT) and graphene oxide (GO) composites on the ITO substrate for the detection of uric acid (UA) in authentic human saliva. Scanning electron microscopy, UV-vis spectrum and X-ray diffraction confirmed the formation of porous PEDOT combined with GO film during the electropolymerization process. The nanocomposite based sensor showed an enhanced electrocatalytic activity toward UA with high sensitivity and stability. We demonstrate that UA can be directly detected in undiluted saliva using the paper-based electroanalytical device with no interference from ascorbic acid and dopamine that are normally present in biological fluids. The results indicated that the developed device is promising for non-invasive monitoring of salivary UA in human body., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2019 Elsevier B.V. All rights reserved.)

We propose a flexible, binder-free and free-standing carbonaceous paper fabricated via electrostatic spray deposition using reduced graphene oxide/carbon nanotube (rGO/CNT) as a promising electrode material for flexible sodium-ion batteries (NIBs). The as-prepared rGO/CNT paper exhibits a three-dimensional (3D) layered structure by employing rGO as conductive frameworks to provide sodium-storage active sites and CNT as spacer to increase rGO interlayer distance and benefit the diffusion kinetics of sodium ions. Consequently, the rGO/CNT paper delivers an enhanced sodium ion storage capacity of 166.8 mAh g -1 at 50 mA g -1 , retaining an average capacity of 101.4 mAh g -1 when current density sets back 100 mA g -1 after cycling at various current rates. An average capacity of 50 mAh g -1 at 200 mA g -1 was stabilized when cycling up to 300 cycles. The well-maintained electrochemical performance of free-standing rGO/CNT paper is due to the well-established hybrid 3D nanostructures, which demonstrates our carbon based material fabricated by a facile approach can be applied as one of the high-performance and low-cost electrode materials for applications in flexible energy storage devices., Competing Interests: The authors declare no conflicts of interest.

Many studies have shown that urokinase plasminogen activator (uPA) is causally involved in promoting cancer invasion and metastasis. Thus, monitoring uPA levels could be very useful in cancer diagnosis, identification of initial metastasis, and guiding cancer treatment. Here, the authors developed a novel and scalable uPA sensor based on a graphene-gold nanoparticle platform that uses fluorescence of quantum dots to rapidly (<1 h) detect uPA up to 100 pM. Indeed, the authors' sensor is highly selective and showed an ability to sense up to 100 pM uPA even in the presence of complex biological milieu such as the fetal bovine serum.

A novel 3D paper-based microfluidic screen-printed electrode (SPE) composed of two layers was constructed by photolithography and screen-printing technology. Aldehyde functionalized hydrophilic zone of the counter and reference electrodes layer was prepared for glucose oxidase immobilization. Highly conductive prussian blue deposited reduced graphene oxide-tetraethylene pentamine (rGO-TEPA/PB) modified paper working electrode layer can be used as an electrochemical sensitive membrane for quantitative detection of hydrogen peroxide (H 2 O 2 ), which was the enzyme-catalyzed reaction product. Therefore, this 3D paper-based microfluidic electrochemical biosensor can be used for quantitative detection of glucose. Under optimum conditions, the proposed biosensor can be used for quantitative determination of glucose over a wide linear range of 0.1 mM-25 mM with detection limit of 25 μM. Finally, the 3D paper-based microfluidic electrochemical biosensor was applied to determine glucose in human sweat and blood, and the obtained results were in good consistency with values measured by Roche's blood glucose meter. In addition, the proposed 3D paper-based electrochemical device showed good repeatability, stability, and anti-interference, which would be of great potential to monitor glucose in complex biological fluids., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Despite the green energy generation with low cost compared to conventional fuel cells, microbial fuel cells (MFCs) still suffer with anode related constraints including laborious pretreatment and modification process of conventional electrodes, limited bacterial loading capacity, and inferior extracellular electron transfer efficiency. Accordingly, this investigation explores the waste tissue paper derived three dimensional (3D) carbon aerogel (CA) integrated with cerium dioxide (CeO 2 ) nanotubes decorated nitrogen-doped reduced graphene oxide nanosheets (NRGO) as a competent anode to address these technical complements. The direct growth of NRGO and CeO 2 over CA in the form of freestanding and binder-free NRGO/CeO 2 (1:2)/CA alleviates the significant constrains of conventional anode fabrication. The 3D hierarchical architectures of CA with open porous structure provide easy access of bacteria, thus increases the bacterial colonies per unit volume. Furthermore, the hydrogen bonding between the interfacial oxygen atoms of CeO 2 and lysine residues of the cytochrome c in bacteria yields excellent extracellular electron transfer efficiency. The electrostatic interaction between the NRGO and bacteria cells improves the bacterial adhesion and biofilm formation, leading to the compact biofilm formation for the improved direct electron transference. With the profits of above, the MFC with NRGO/CeO 2 (1:2)/CA demonstrates a maximum power output and good lifespan performances. The present exploration facts thus access advanced avenues to converting waste matters of tissue paper, human urine, and wastewater into profitable constituents for the development of efficient and durable power producing systems.

A paper-based analytical device (PAD) with an integrated composite electrode for non-enzymatic creatinine sensing was developed. The electrode was produced and optimization was efficiently accomplished using a rapid digital dispensing approach. The electrochemical sensor was fabricated using an HP D300 digital dispenser to deliver a copper oxide and ionic liquid composite onto an electrochemically reduced graphene modified screen-printed carbon electrode (CuO/IL/ERGO/SPCE) on a PAD. The modified electrode was characterized using electrochemical and microscopic techniques. Electrochemical detection of creatinine was performed on the SPCE using amperometry at a constant potential. Under optimized conditions, the paper-based sensor exhibited a linear range of 0.01-2.0 mM (R 2  = 0.99) and the limit of detection was 0.22 μM (S/N = 3, IUPAC definition) for creatinine. The simple fabrication process, low cost, and clinically appropriate creatinine sensitivity make this device applicable for point-of-care use., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Hemoglobin A1c (HbA1c) is a standard biomarker to measure long-term average glucose concentration for diagnosis and monitoring of diabetes. Various methods have been reported for measuring HbA1c, however, portable and precise determination is still challenging. Herein, a new highly sensitive electrochemical nanobiosensor is developed for the specific determination of HbA1c. A nanocomposite of reduced graphene oxide (rGO) and gold with hierarchical architecture structure was electrochemically deposited on a cheap and flexible graphite sheet (GS) electrode. The nanocomposite increased the surface area, improved the electron transfer on the electrode surface and augmented the signal. It also provided a suitable substrate for linkage of thiolated DNA aptamer as a bioreceptor on the electrode surface by strong covalent bonding. The quantitative label free detection was carried out by differential pulse voltammetry (DPV) in a phosphate-buffered saline (PBS) solution containing redox probe Fe(CN) 6 3-/4- . The detection is based on insulating the surface in presence of HbA1c and decreasing the current, which is directly related to the HbA1c concentration. The nanobiosensor demonstrated high sensitivity of 269.2 μA. cm -2 , wide linear range of 1 nM-13.83 μM with a low detection limit of 1 nM. The biosensor was successfully used for measuring HbA1c in blood real sample. Furthermore, it is promising to use it as a part of a point of care device for low-invasive screening and management of diabetes., (Copyright © 2019 Elsevier B.V. All rights reserved.)

A paper-based electrochemical immunosensor was developed for the detection of cancer antigen 125 (CA125) by screen-printing technique. The reduced graphene oxide/thionine/gold nanoparticles (rGO/Thi/AuNPs) nanocomposites were compounded and coated onto the working electrode of immunosensor for CA125 antibody (anti-CA125) immobilization and detection signal amplification. The detection principle was based on the fact that the immunocomplex formed by specify binding of CA125 antibody and antigen could reduce the current response of thionine, which was proportional to the corresponding concentration of CA125 antigen. The immunoassay results showed that the linear range of CA125 was from 0.1 U mL -1 to 200 U mL -1 with the limit of detection (LOD) of 0.01 U mL -1 at signal to noise of 3. Quality control serum samples measured by our proposed immunosensor showed acceptable agreement with traditional ELISA method with the relative error less than 8.05%. The immunosensor exhibited good electrochemical performance with high reproducibility, reliability, stability and accuracy. The proposed immunosensor could be used for the determination of CA125 and had the potential for point-of-care testing (POCT) of other tumor marker., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Allergen genes of the peanut and soybean were selected as model targets. Four hairpin DNA probes, H1, H2, H3, H4 were designed. Cy3-labeled H1 and H2 were used to detect peanut DNA, while FAM-labeled H3 and H4 were used to detect soybean DNA. Graphene oxide (GO) was used as the adsorption material for capturing the hairpin probes, and as a selective fluorescence quencher to reduce the background signal. To develop an allergen gene detection system with a GO-based paper chip format, we integrated the hybridization chain reaction (HCR) with fluorescence resonance energy transfer (FRET) in our design. The results showed that in the absence of peanut DNA (T P ) and soybean DNA (T S ), the detection probes attached to the GO surface, which quenched their fluorescence. In the presence of T P or T S , however, complementary probe binding to the targets initiated HCR, producing long double-stranded DNA products that could not be absorbed onto the GO surface. Hence, a strong red or green fluorescent signal was generated. The detection limit for both peanut and soybean DNA was 1 nM using this method, indicating the high sensitivity of our approach. This method also exhibited good specificity and a single chip could be used to simultaneously detect two different targets., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Graphene-based materials represent advanced platforms for tissue engineering and implantable medical devices. From a clinical standpoint, it is essential that these materials are produced using non-toxic and non-hazardous methods, and have predictable properties and reliable performance under variable physiological conditions; especially when used with a cellular component. Here we describe such a biomaterial, namely smart graphene-cellulose (G-C) paper, and its suitability for traditional planar two-dimensional (2D) or three-dimensional (3D) human cell support, verified by adipose-derived stem cell (ADSC) culture and osteogenic differentiation. G-C paper is prepared using commercially available cellulose tissue paper as a substrate that is coated by immersion-deposition with graphene oxide (GO) followed by reduction to reduced graphene oxide (RGO) without the use of toxic organic solvents. The fabrication process is amenable to large scale production and the resultant papers have low electrical resistivity (up to ∼300 Ω/sq). Importantly, G-C papers can be configured to 3D constructs by lamination with alginate and further modified by folding and rolling for 3D "origami-inspired" cell-laden structures., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Three-dimensional (3-D) graphene was synthesized by the assembly of graphene oxide with phenolic resin, followed by carbonization in argon. The as-synthesized 3-D graphene has excellent conductivity, good thermal stability, large specific surface area (1511 m² g -1 ) and pore volume (0.90 cm 3  g -1 ). By immobilizing the 3-D graphene onto the stainless steel wire (SSW), we obtained a 3-D graphene coated fiber that was then used as a working electrode for electro-enhanced SPME, which shows a 3.2-fold improvement of extraction efficiency for bisphenol A (BPA) over that of traditional SPME. Coupled to gas chromatography, the method was developed to the determination of BPA with good linearity (R 2  = 0.9935) in the range of 0.1-10 μg mL -1 . The limit of detection was calculated to be 0.006 μg mL -1 based on the signal-to-noise of 3. The proposed method was applied for the analysis of three kinds of thermal papers with BPA being detected in all samples (0.696-3.78 mg g -1 ). Recovery tests were performed to validate the reliability of the method, and the recoveries were found between 81.9% and 119% with relative standard deviations lower than 4.8%., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Flexible sensing devices have drawn tremendous attention in the past decades due to their potential applications in future hand-held, potable consumer, and wearable electronics. Here, we firstly developed an ultrasensitive wireless potentiometric aptasensor based on flexible freestanding graphene paper for kanamycin detection. Flexible graphene paper made from a simple vacuum filtration method was used as a biocompatible platform for effective immobilization of aptamer. A nuclease-assisted amplification strategy was introduced into this potentiometric biosensing system in order to significantly improve the detection sensitivity through a classic catalytic recycling reaction of target induced by the nuclease (DNase I). As expected, an ultra-low detection limit of 30.0 fg/mL for kanamycin was achieved. Furthermore, the developed potentiometric enzymatic aptasensor exhibits high selectivity, favorable flexibility, excellent stability and reproducibility, which holds great promising for its routine sensing application., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Point-of-care testing (POCT) devices represent a growing field that aims to develop low-cost, rapid, sensitive diagnostic testing platforms that are portable and self-contained. Surface-enhanced Raman spectroscopy (SERS) is an approach has shown high potential in POCT technology. However, the specificity or ability to uniquely detect a desired biomarker in complex biological samples is a key factor for translating SERS technologies to POCT. Herein, we fabricated cellulose SERS strips (CS) decorated with novel plasmonic nanoparticles, termed graphene-isolated-Au-nanocrystals (GIANs), for the portable detection of complex biological samples. This CS@GIANs SERS strip was used to detect free bilirubin (BR) in the blood of newborns, a biomarker of jaundice, without sample labeling or prepreparation. CS@GIANs showed superior affinity to hydrophobic BR molecules compared to typical SERS substrate, which reduced the steric hindrance effect from the nonspecific binding of BR with serum albumin in blood and improved sensitivity. Meanwhile, with the separation property of cellulose chromatography papers, CS@GIANs showed superior anti-interference to other biomolecules that had been previously adsorbed on the SERS strip. Moreover, the SERS signal from the graphitic shell of GIANs could be used as a stable internal calibration standard, which improved the reproducibility and accuracy of Raman analysis. Such a cellulose SERS strip holds high potential for enhancing current efforts in the development of rapid and low-cost point-of-care diagnostic testing.

Introduction: The PKU is an inborn error of amino acid metabolism, in which phenylalanine (Phe) accumulated in the blood causing alterations at the central nervous system. We report a novel paper-based enzymatic platform coupled to screen printed graphene-modified electrode for the neonatal screening of phenylketonuria (PKU0., Methods: The paper-based analytical device coupled to electrochemical detection (EPAD) is based on the use of paper microzones modified with phenylalanine dehydrogenase enzyme (PheDH). The modified PADs were placed on the surface of an electrode modified with electrochemically reduced graphene (ERGO). PheDH in the presence of NAD + catalyzes the reversible deamination of Phe to form phenylpyruvate, ammonia, and NADH. The electrochemical oxidation of NADH was monitored by differential pulse amperometry (DPA) at 0.6 V. The method was linear in the concentration range from 1 to 600 μmol/L of Phe with a LOQ of 1 μmol/L and LOD of 0.2 μmol/L. Within day precision was 5.7% across 3 levels of control samples. Between-day precision was 8.3%. The comparison with the standard Phe enzyme assay kit showed good agreement. The time required for the overall assay was <5 min. The non-sophisticated equipment required, the short assay time and the appropriate LOQ and LOD achieved by our EPAD make it an attractive and easy to use alternative compared to existing methods applied to the screening of PKU in neonatal samples., (Copyright © 2018 Elsevier B.V. All rights reserved.)

A functionalized paper based on gold nanoparticles (Au NPs) conjugated graphene oxide (GO) was developed for near-infrared (NIR) laser triggered photothermal ablation against infectious bacterial pathogens. Firstly, quaternized carboxymethyl chitosan (QCMC) not only acted as reducing agent to synthesize Au NPs, but also functioned as coupling agent to link up Au NPs with GO. Au-QCMC-GO(+) was supposed to synergistically intensify the photothermal effect, which was then mixed with nanocellulose to form a functionalized paper via vacuum filtration. The photothermal efficiency, antibacterial treatment and mechanical property of Au-QCMC-GO(+)/nanocellulose paper were investigated. Excited by NIR laser irradiation, Au-QCMC-GO(+)/nanocellulose paper generated a temperature rise over 80 °C, sufficient for photothermal ablation upon both Gram-positive bacteria (Bacillus subtilis and Stapylococcus aureus) and Gram-negative bacteria (Escherichia coli and Pseudomonas aeruginosa). Additionally, Au-QCMC-GO(+)/nanocellulose paper showed a remarkable enhancement in tensile strength, bursting index and tear index compared to those of pure nanocellulose paper., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Rapid, disposable, point-of-care (POC) oral fluid testing has gained considerable attention in recent years as saliva contains biomarker and components of the serum proteome that offer important information on both oral and systemic disease. Microfluidic paper-based analytical devices (μPADs) coupled with smartphone reflectance sensing systems have long been considered to be an effective POC tool for the diagnostics of biomarkers in oral fluid. However, the existing portable systems are limited by the poor color distribution in the detection area as well as not being universally applicable. Therefore, using the properties of nanomaterials to our advantage, we present a simple, universally applicable approach that features graphene oxide (GO) coated μPADs coupled with smartphone-based colorimetric detection for the direct quantification of glucose. An integrated portable system is used to implement the approach. Owing to the enhanced reagents absorptivity, reactive efficiency and homogeneity of color distribution from the deposition of GO, the glucose assay performance was improved. Also, by using a self-developed app, the glucose concentrations in physiological range can be automatically quantified. Finally, the approach is universally applicable as the modification of μPADs with GO can be achieved without the use of any linker, binder or retention aid, which avoids possible enzyme cross contamination. The system was first calibrated by standard glucose buffer solutions, and the limit of detection as well as the linear dynamic range were found to be 0.02 mM and 0~1 mM, respectively, which are appropriate for analyzing glucose concentrations in a clinically relevant range. Finally, the system was used for quantifying glucose concentrations in artificial saliva and the results obtained using our portable system showed reasonable agreement with the actual use concentrations. Thus, the utility of the system in sensitively quantifying glucose concentrations in a portable, and repeatable manner is demonstrated.

After a long-term toxicity study on Bisphenol A (BPA), the European Union and U.S food and drug administration updating the rules regarding the usage of BPA by extending the prohibition of BPA to include in the production of papers, on February 2018. Therefore, it is essential to establish the trace level BPA detectors in paper samples. In this report, the synthesis of novel ZnO nanoclusters wrapped with reduced graphene oxide (ZnO NCs/rGO) and its application towards the selective electrocatalytic detection of BPA are described. Initially, ZnO NCs/rGO is synthesized by the one-step hydrothermal approach, and various characterizations explain the compound's compositions and structure. The significance of ZnO NCs/rGO together with good electrocatalytic properties leads this material to the platform for electrochemical sensor. Finally, ZnO NCs/rGO was fabricated and validated as an effective sensor for the sensitive detection of BPA. The demonstrated sensor revealed excellent detection of BPA with the very low detection limit (2.1 nM), and also it offered good analytical parameters with more extensive linear range and higher sensitivity. Likewise, the sensor annexes good durability, reproducibility, and selectivity towards the determination of BPA. Due to the nourishing capacity of the prepared ZnO NCs/rGO, it is employed for the detection of BPA in tissue paper samples., (Copyright © 2018 Elsevier Inc. All rights reserved.)

Although significant technological advancements have been made in the development of analytical biosensor chips for detecting bacterial strains (E. coli, S. Mutans and B. Subtilis), critical requirements i.e. limit of detection (LOD), fast time of response, ultra-sensitivity with high reproducibility and good shelf-life with robust sensing capability have yet to be met within a single sensor chip. In order to achieve these criteria, we present an electrically-receptive thermally-responsive (ER-TR) sensor chip comprised of simple filter paper used as substrate coated with composite of poly(N-isopropylacrylamide) polymer (PNIPAm) - graphene nanoplatelet (GR) followed by evaporation of Au electrodes for capturing both Gram-positive (S. mutans and B. subtilis) and Gram-negative (E. coli) bacterial cells in real-time. Autoclave water, tap water, lake water and milk samples were tested with ER-TR chip with and without bacterial strains at varying concentration range 10 1 -10 5 cells/mL. The sensor was integrated with in-house built printed circuit board (PCB) to transmit/receive electrical signals. The interaction of E. coli, S. mutans and B. subtilis cells with fibers of PNIPAm-GR resulted in a change of electrical resistance and the readout was monitored wirelessly in real-time using MATLAB algorithm. Finally, prepared ER-TR chip exhibited the reproducibility of 85-97% with shelf-life of up to four weeks after testing with lake water sample., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Staphylococcus aureus (S. aureus) is a pathogenic bacteria which causes infectious diseases and food poisoning. Current diagnostic methods for infectious disease require sophisticated instruments, long analysis time and expensive reagents which restrict their application in resource-limited settings. Electrochemical paper based analytical device (EPAD) was developed by integrating graphene nano dots (GNDs) and zeolite (Zeo) using specific DNA probe. The ssDNA/GNDs-Zeo modified paper based analytical device (PAD) was characterized using cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The genosensor was optimized at pH7.4 and incubation temperature of 30°C. A linear current response with respect to target DNA concentrations was obtained. The limit of detection (LOD) of the proposed sensor was found out to be 0.1nM. The specificity was confirmed by introducing non-complimentary target DNA to ssDNA/GNDs-Zeo modified PAD. The suitability of the proposed EPAD genosensor was demonstrated with fruit juice samples mixed with S. aureus. The proposed EPAD genosensor is a low cost, highly specific, easy to fabricate diagnostic device for detection of S. aureus bacteria which requires very low sample volume and minimum analysis time of 10s., (Copyright © 2018 Elsevier B.V. All rights reserved.)

We introduce for the first time a paper-based analytical device (PAD) for the non-enzymatic detection of glucose by modifying a screen-printed carbon electrode with cobalt phthalocyanine, graphene and an ionic liquid (CoPc/G/IL/SPCE). The modifying composite was characterized by UV-visible spectroscopy, energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The disposable devices show excellent conductivity and fast electron transfer kinetics. The results demonstrated that the modified electrode on PADs had excellent electrocatalytic activity towards the oxidation of glucose with NaOH as supporting electrolyte (0.1M). The oxidation potential of glucose was negatively shifted to 0.64V vs. the screen-printed carbon pseudo-reference electrode. The paper-based sensor comprised a wide linear concentration range for glucose, from 0.01 to 1.3mM and 1.3-5.0mM for low and high concentration of glucose assay, respectively, with a detection limit of 0.67µM (S/N = 3). Additionally, the PADs were applied to quantify glucose in honey, white wine and human serum. The disposable, efficient, sensitive and low-cost non-enzymatic PAD has great potential for the development of point-of-care testing (POCT) devices that can be applied in healthcare monitoring., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Flexible sweat biosensors are of considerable current interest for the development of wearable smart miniature devices. In this work, we report a novel type of flexible and electrochemical sweat platform fabricated by depositing Cu submicron buds on freestanding graphene paper (GP) carrying MoS 2 nanocrystals monolayer for bio-functional detection of glucose and lactate. Quantitative analysis of glucose and lactate was carried out by using amperometric i-t method. Linear ranges were obtained between 5 and 1775 μM for glucose and 0.01-18.4 mM for lactate, and their corresponding limits of detection were 500 nM and 0.1 μM, respectively. The platform demonstrates fast response, good selectivity, superb reproducibility and outstanding flexibility, which enable its use for monitoring glucose and lactate in human perspiration. The strategy of structurally integrating 3D transition metal, 0D transition metal sulfide and 2D graphene will provide new insight into the design of flexible electrodes for sweat glucose and lactate monitoring and a wider range of applications in biosensing, bioelectronics, and lab-on-a-chip devices., (Copyright © 2017. Published by Elsevier Inc.)

In this study, two-dimensional (2D) and three-dimensional (3D) freestanding reduced graphene oxide-supported Cu 2 O composites (Cu 2 O-rGO) were synthesized via simple and cost-efficient hydrothermal and filtration strategies. The structural characterizations clearly showed that highly porous 3D graphene aerogel-supported Cu 2 O microcrystals (3D Cu 2 O-GA) have been successfully synthesized, and the Cu 2 O microcrystals are uniformly assembled in the 3D GA. Meanwhile, paper-like 2D reduced graphene oxide-supported Cu 2 O nanocrystals (2D Cu 2 O-rGO-P) have also been prepared by a filtration process. It was found that the products prepared from different precursors and methods exhibited different sensing performances for H 2 O 2 detection. The electrochemical measurements demonstrated that the 3D Cu 2 O-GA has high electrocatalytic activity for the H 2 O 2 reduction and excellent sensing performance for the electrochemical detection of H 2 O 2 with a detection limit of 0.37 μM and a linear detection range from 1.0 μM to 1.47 mM. Meanwhile, the 2D Cu 2 O-rGO-P structure also showed good electrochemical sensing performance toward H 2 O 2 detection with a much wider linear response over the concentration range from 5.0 μM to 10.56 mM. Compared to the previously reported sensing materials, the as-obtained 2D and 3D Cu 2 O-rGO materials exhibited higher electrochemical sensing properties toward the detection of H 2 O 2 with high sensitivity and selectivity. The 2D and 3D Cu 2 O-rGO composites also exhibited high sensing performance for the real-time detection of H 2 O 2 in human serum. The present study indicates that 2D and 3D graphene-Cu 2 O composites have promising applications in the fabrication of nonenzymatic electrochemical sensing devices.

In this work, carbon papers and aerogels based on graphene layers and chitosan were prepared. They were obtained by mixing chitosan (CS) and a high surface area nanosized graphite (HSAG) in water in the presence of acetic acid. HSAG/CS water dispersions were stable for months. High resolution transmission electron microscopy revealed the presence of few graphene layers in water suspensions. Casting or lyophilization of such suspensions led to the preparation of carbon paper and aerogel, respectively. In X-ray spectra of both aerogels and carbon paper, peaks due to regular stacks of graphene layers were not detected: graphene with unaltered sp 2 structure was obtained directly from graphite without the use of any chemical reaction. The composites were demonstrated to be electrically conductive thanks to the graphene. Chitosan thus makes it possible to obtain monolithic carbon aerogels and flexible and free-standing graphene papers directly from a nanosized graphite by avoiding oxidation to graphite oxide and successive reduction. Strong interaction between polycationic chitosan and the aromatic substrate appears to be at the origin of the stability of HSAG/CS adducts. Cation-π interaction is hypothesized, also on the basis of X-ray photoelectron spectroscopy findings. This work paves the way for the easy large-scale preparation of carbon papers through a method that has a low environmental impact and is based on a biosourced polymer, graphene, and water.

A paper/poly(methyl methacrylate) (PMMA) hybrid CD-like microfluidic SpinChip integrated with DNA probe-functionalized graphene oxide (GO) nanosensors was developed for multiplex quantitative LAMP detection (mqLAMP). This approach can simply and effectively address a major challenging problem of multiplexing in current LAMP methods.

Pressure sensors should have an excellent sensitivity in the range of 0-20 kPa when applied in wearable applications. Traditional pressure sensors cannot achieve both a high sensitivity and a large working range simultaneously, which results in their limited applications in wearable fields. There is an urgent need to develop a pressure sensor to make a breakthrough in both sensitivity and working range. In this paper, a graphene-paper pressure sensor that shows excellent performance in the range of 0-20 kPa is proposed. Compared to most reported graphene pressure sensors, this work realizes the optimization of sensitivity and working range, which is especially suitable for wearable applications. We also demonstrate that the pressure sensor can be applied in pulse detection, respiratory detection, voice recognition, as well as various intense motion detections. This graphene-paper pressure sensor will have great potentials for smart wearable devices to achieve health monitoring and motion detection.

In this work, aiming at the construction of a disposable, wireless, low-cost and sensitive system for bioassay, we report a closed bipolar electrode electrochemiluminescence (BPE-ECL) sensing platform based on graphite paper as BPE for the first time. Graphite paper is qualified as BPE due to its unique properties such as excellent electrical conductivity, uniform composition and ease of use. This simple BPE-ECL device was applied to the quantitative analysis of oxidant (H 2 O 2 ) and biomarker (CEA) respectively, according to the principle of BPE sensing-charge balance. For the H 2 O 2 analysis, Pt NPs were electrodeposited onto the cathode through a bipolar electrodeposition approach to promote the sensing performance. As a result, this BPE-ECL device exhibited a wide linear range of 0.001-15mM with a low detection limit of 0.5µM (S/N=3) for H 2 O 2 determination. For the determination of CEA, chitosan-multi-walled carbon nanotubes (CS-MWCNTs) were employed to supply a hydrophilic interface for immobilizing primary antibody (Ab 1 ); and Au@Pt nanostructures were conjugated with secondary antibody (Ab 2 ) as catalysts for H 2 O 2 reduction. Under the optimal conditions, the BPE-ECL immunodevice showed a wide linear range of 0.01-60ngmL -1 with a detection limit of 5.0pgmL -1 for CEA. Furthermore, it also displayed satisfactory selectivity, excellent stability and good reproducibility. The developed method opened a new avenue to clinical bioassay., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Simple, inexpensive and rapid sensing systems are very demanded for a myriad of uses. Intrinsic properties of emerging paper-based analytical devices have demonstrated considerable potential to fulfill such demand. This work reports an easy-to-use, low cost, and disposable paper-based sensing device for rapid chemical screening with a smartphone readout. The device comprises luminescent graphene quantum dots (GQDs) sensing probes embedded into a nitrocellulose matrix where the resonance energy transfer phenomenon seems to be the sensing mechanism. The GQDs probes were synthesized from citric acid by a pyrolysis procedure, further physisorbed and confined into small wax-traced spots on the nitrocellulose substrate. The GQDs were excited by an UV LED, this, is powered by a smartphone used as both; energy source and imaging capture. The LED was contained within a 3D-printed dark chamber that isolates the paper platform from external light fluctuations leading to highly reproducible data. The cellulose-based device was proven as a promising screening tool for phenols and polyphenols in environmental and food samples, respectively. It opens up new opportunities for simple and fast screening of organic compounds and offers numerous possibilities for versatile applications. It can be especially useful in remote settings where sophisticated instrumentation is not always available.

The present study was aimed to develop an ultrasensitive technique for electroanalysis of ketamine; a date rape drug. It involved the fabrication of nano-hybrid based electrochemical micro fluidic paper-based analytical device (EμPADs) for electrochemical sensing of ketamine. A paper chip was developed using zeolites nanoflakes and graphene-oxide nanocrystals (Zeo-GO). EμPAD offers many advantages such as facile approach, economical and potential for commercialization. Nanocrystal modified EμPAD showed wide linear range 0.001-5nM/mL and a very low detection limit of 0.001nM/mL. The developed sensor was tested in real time samples like alcoholic and non-alcoholic drinks and found good correlation (99%). The hyphenation of EμPAD integrated with nanocrystalline Zeo-GO for detection of ketamine has immense prospective for field-testing platforms. An extensive development could be made for industrial translation of this fabricated device., (Copyright © 2016 Elsevier B.V. All rights reserved.)

Cortisol has been identified as a biomarker in saliva to monitor psychological stress. In this work, we report a label-free paper-based electrical biosensor chip to quantify salivary cortisol at a point-of-care (POC) level. A high specificity of the sensor chip to detect cortisol with a detection limit of 3 pg/mL was achieved by conjugating anticortisol antibody (anti-CAB) on top of gold (Au) microelectrodes using 3,3'-dithiodipropionic acid di(N-hydroxysuccinimide ester (DTSP) as a self-assembled monolayer (SAM) agent. The electrode design utilized poly(styrene)-block-poly(acrylic acid) (PS 67 -b-PAA 27 ) polymer and graphene nanoplatelets (GP) suspension coated on filter paper to increase the sensitivity of the immune response. A biosensor chip was then integrated with a lab-built low-cost miniaturized printed circuit board (PCB) to provide an electrical connection and to wirelessly transmit/receive electrical signals using MATLAB. This fully integrated proposed hand-held device successfully exhibited a wide cortisol-detection range from 3 pg/mL to 10 μg/mL, with a sensitivity of 50 Ω (pg mL -1 ) -1 . The performance of the proposed cortisol sensor chip was validated using an enzyme-linked immunosorbent assay (ELISA) technique with a regression value of 0.9951. The advantages of the newly developed cortisol immune biosensor over previously reported chips include an improved limit of detection, no need for additional redox medium for electron exchange, faster response to achieve stable data, excellent shelf life, and its economical production.