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In this work, a novel facile closed bipolar electrochemiluminescence (C-BP-ECL) sensor has been developed for highly sensitive detection of glucose based on the integration of chitosan (CS), poly(diallyldimethylammonium chloride)-functioned multi-walled carbon nanotubes (PDDA-MWCNTs) and graphene quantum dots-gold nanoparticles (GQDs-AuNPs) on the wax/carbon ink-screen-printed cloth-based device. When CS, PDDA-MWCNTs and GQDs-AuNPs are successively decorated onto the cathode of closed bipolar electrode (C-BPE), the C-BPE anode can emit much stronger C-BP-ECL signals. Moreover, the cathodic decoration of the C-BPE can generate a stronger ECL signal in comparison with its anodic decoration. Under optimized conditions, glucose can be detected in the range of 0.1-5000 μM, and the limit of detection is estimated to be 64 nM, which is about three orders of magnitude lower than that in case of the bare C-BPE cathode (31 μM). It has been shown that the proposed sensor has high detection sensitivity, wide dynamic range, and as well acceptable reproducibility, selectivity and stability. Finally, the applicability and validity of the C-BP-ECL sensor are demonstrated for the detection of glucose in human serum samples. We believe that this novel highly-sensitive sensor will have potential applications in various areas such as clinical diagnosis, food analysis and environmental monitoring., (Copyright © 2019 Elsevier B.V. All rights reserved.)

This paper introduces a new and simple concept for fabricating low-cost, easy-to-use capillary microchannel (CMC) assisted thread-based microfluidic analytical devices (CMCA-μTADs) for bipolar electrochemiluminescence (BP-ECL) application. The thread with patterns of carbon screen-printed electrodes and bare thread zones (BTZs) is embedded into a CMC. Such CMCA-μTADs can produce a strong and stable BP-ECL signal, and have an extremely low cost ($0.01 per device). Interestingly, the CMCA-μTADs are ultraflexible, and can be bent with a 135° bending angle at the BTZ or with a 150° bending angle at the middle of bipolar electrode (BPE), with no loss of analytical performance. Additionally, the two commonly-used ECL systems of Ru(bpy) 3 2+ /TPA and luminol/H 2 O 2 are applied to demonstrate the quantitative ability of the BP-ECL CMCA-μTADs. It has been shown that the proposed devices have successfully fulfilled the detection of TPA and H 2 O 2 , with detection limits of 0.00432mM and 0.00603mM, respectively. Based on the luminol/H 2 ECL system, the CMCA-μTADs are further applied for the glucose measurement, with the detection limit of 0.0205mM. Finally, the applicability and validity of the CMCA-μTADs are demonstrated for the measurements of H 2 ECL system, the CMCA-μTADs are further applied for the glucose measurement, with the detection limit of 0.0205mM. Finally, the applicability and validity of the CMCA-μTADs are demonstrated for the measurements of H 2 in milk, and glucose in human urine and serum. The results indicate that the proposed devices have the potential to become an important new tool for a wide range of applications.2 in milk, and glucose in human urine and serum. The results indicate that the proposed devices have the potential to become an important new tool for a wide range of applications., (Copyright © 2017 Elsevier B.V. All rights reserved.)

A novel screen-printed microfluidic paper-based analytical device with all-carbon electrode-enabled electrochemical assay (SP-ACE-EC-μPAD) has been developed. The fabrication of these devices involved wax screen-printing, which was simple, low-cost and energy-efficient. The working, counter and reference electrodes were screen-printed using carbon ink on the patterned paper devices. Different wax screen-printing processes were examined and optimized, which led to an improved method with a shorter heating time (~5 s) and a lower heating temperature (75 °C). Different printing screens were examined, with a 300-mesh polyester screen yielding the highest quality wax screen-prints. The carbon electrodes were screen-printed on the μPADs and then examined using cyclic voltammetry. The analytical performance of the SP-ACE-EC-μPADs for the detection of glucose and uric acid in standard solutions was investigated. The results were reproducible, with a linear relationship [R(2) = 0.9987 (glucose) or 0.9997 (uric acid)] within the concentration range of interest, and with detection limits as low as 0.35 mM (glucose) and 0.08 mM (uric acid). To determine the clinical utility of the μPADs, chronoamperometry was used to analyze glucose and uric acid in real urine samples using the standard addition method. Our devices were able to detect the analytes of interest in complex real-world biological samples, and have the potential for use in a wide variety of applications.

This work describes the first approach at combining microfluidic cloth-based analytical devices (μCADs) with electrochemiluminescence (ECL) detection. Wax screen-printing is employed to make cloth-based microfluidic chambers which are patterned with carbon screen-printed electrodes (SPEs) to create truly disposable, simple, inexpensive sensors which can be read with a low-cost, portable charge coupled device (CCD) imaging sensing system. And, the two most commonly used ECL systems of tris(2,2'-bipyridyl)ruthenium(II)/tri-n-propylamine (Ru(bpy)3(2+)/TPA) and 3-aminophthalhydrazide/hydrogen peroxide (luminol/H2O2) are applied to demonstrate the quantitative ability of the ECL μCADs. In this study, the proposed devices have successfully fulfilled the determination of TPA with a linear range from 2.5 to 2500μM with a detection limit of 1.265μM. In addition, the detection of H2O2 can be performed in the linear range of 0.05-2.0mM, with a detection limit of 0.027mM. It has been shown that the ECL emission on the wax-patterned cloth device has an acceptable sensitivity, stability and reproducibility. Finally, the applicability of cloth-based ECL is demonstrated for determination of glucose in phosphate buffer solution (PBS) and artificial urine (AU) samples, with the detection limits of 0.032mM and 0.038mM, respectively. It can be foreseen, therefore, that μCADs with ECL detection could provide a new sensing platform for point-of-care testing, public health, food safety detection and environmental monitoring in remote regions, developing or developed countries., (Copyright © 2015 Elsevier B.V. All rights reserved.)

In this work, we first introduce the fabrication of microfluidic cloth-based analytical devices (μCADs) using a wax screen-printing approach that is suitable for simple, inexpensive, rapid, low-energy-consumption and high-throughput preparation of cloth-based analytical devices. We have carried out a detailed study on the wax screen-printing of μCADs and have obtained some interesting results. Firstly, an analytical model is established for the spreading of molten wax in cloth. Secondly, a new wax screen-printing process has been proposed for fabricating μCADs, where the melting of wax into the cloth is much faster (∼5 s) and the heating temperature is much lower (75 °C). Thirdly, the experimental results show that the patterning effects of the proposed wax screen-printing method depend to a certain extent on types of screens, wax melting temperatures and melting time. Under optimized conditions, the minimum printing width of hydrophobic wax barrier and hydrophilic channel is 100 μm and 1.9 mm, respectively. Importantly, the developed analytical model is also well validated by these experiments. Fourthly, the μCADs fabricated by the presented wax screen-printing method are used to perform a proof-of-concept assay of glucose or protein in artificial urine with rapid high-throughput detection taking place on a 48-chamber cloth-based device and being performed by a visual readout. Overall, the developed cloth-based wax screen-printing and arrayed μCADs should provide a new research direction in the development of advanced sensor arrays for detection of a series of analytes relevant to many diverse applications., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Photoelectrochemical (PEC) detection is a widely used detection method that uses light to stimulate and photocurrent signals to detect the target. Due to the disengagement of the excitation unit and the detection unit, the PEC background signal is reduced, and the detection sensitivity is improved. In this work, we report the first demonstration of PEC detection for microfluidic cloth-based analytical devices (μCADs). Using PEC μCADs integrated with cadmium sulfide quantum dots (CdS QDs) and multiwalled carbon nanotubes (MWCNTs), the nonenzymatic, sensitive and rapid measurement of glucose in saliva has been achieved. For the cloth-based device, the PEC reaction zone and cloth-based electrodes can be fabricated by inexpensive wax-based and carbon ink-based screen-printing, respectively. By the layer-by-layer method, the as-prepared poly (dimethyl diadly ammonium chloride-functionalized) MWCNTs (PDDA-MWCNTs) and CdS QDs are successively adsorbed onto the working electrode surface of the cloth-based device. In the presence of an excitation source and glucose, the CdS QDs generate a strong oxidizing electron hole that can then continuously oxidize glucose to produce an electrical signal for glucose detection. Under optimized conditions, a linear dependence is obtained between the PEC signal and glucose concentrations in the range of 0.05–1000 μM with a detection limit of 15.99 nM. In the detection range, the cloth-based device also shows acceptable selectivity, reproducibility, and long-term stability. Moreover, the method has been implemented for the detection of glucose in real saliva samples, suggesting good potential for biochemical applications. [Display omitted] • The coupling of PEC detection and μCADs has been firstly proposed. • The μCADs are used for non-enzymatic glucose analysis for the first time. • The self-assembly of PDDA-MWCNTs and CdS QDs is firstly used for PEC detection. • The PEC μCADs have been used for detection of glucose in human saliva samples. • The method is highly sensitive (detection limit of 15.99 nM), simple, rapid, and low-cost. [ABSTRACT FROM AUTHOR]

• A wearable cloth-based electrochemical sensor (WCECS) is proposed. • The good sweat collection channels and sweat transport channel are obtained. • The WCECS is easily fabricated, low-cost, skin-friendly and secure-safe. • The WCECS has an acceptable analytical performance. • The WCECS can be applied for in vitro sweat monitoring and duplex detection. Wearable electrochemical (EC) biosensors have attracted tremendous attention for noninvasive diagnosis and point-of-care testing (POCT) of individual health level. The analysis of glucose concentration in epidermal sweat presents a promising means of noninvasive continuous glucose monitoring for diabetes mellitus. The previous focus has been mainly on pursuing novel EC sensing materials to achieve highly sensitive biosensors. In this work, a novel flexible three-dimensional (3-D) wearable cloth-based EC sensor (WCECS) has been proposed for analysis of glucose in sweat. The WCECS possesses excellent sweat collection channels and cloth-based sweat transport channel. Notably, the transport channel is actuated by the capillary force to absorb the sweat into the cloth-based chip which can be easily and inexpensively fabricated by the screen-printing technology. Under optimized conditions, the WCECS can well measure the concentrations of glucose in sweat over the range of 0.05−1 mM, with an acceptable sensitivity of 105.93 μA mM−1 cm−2. Besides, the WCECS exhibits excellent selectivity, reproducibility and stability. Importantly, the EC responses of the WCECS have a good correlation with those of the glucometer, and are consistent with the results by the glucose kit. Moreover, the WCECS can be applied for constant 9 h wearable monitoring, and for simultaneous detection of lactic acid and glucose in sweat. So, the proposed approach may represent an important step toward the promising application of the cloth-based sensor for daily personalized health monitoring. [ABSTRACT FROM AUTHOR]

Electrochemiluminescence (ECL) chips have been widely used in the field of medical diagnosis. However, most of these chips currently in use are costly and require high amounts of sample. In this work, we present, for the first time, a shared-cathode closed bipolar electrochemiluminescence (SC-CBP-ECL) cloth-based chip, which can be used for multiplex detection. The SC-CBP-ECL chips ($0.03–0.05 for each chip) are manufactured using carbon ink- and wax-based screen-printing techniques, without the need for expensive and complex fabrication equipment. Under optimised conditions, the SC-CBP-ECL chips were successfully used for coinstantaneous detection of glucose in double ECL systems (i.e., Ru(bpy) 3 2+ and luminol), with corresponding linear ranges of 0.05–1 mM and 0.05–10 mM, and detection limits of 0.0382 mM and 0.0422 mM. To our knowledge, this is the first report on the application of fibre material-based closed bipolar electrodes (C-BPE) combined with double ECL systems. Furthermore, the SC-CBP-ECL chips exhibit an acceptable specificity and good reproducibility and stability and can be used for glucose detection in human serum samples with a good agreement compared with the clinical method. Finally, the SC-CBP-ECL chips could be successfully used for simultaneous detection of seven glucose samples and also show potential for simultaneous detection of three different targets (hydrogen peroxide [H 2 O 2 ], glucose, and uric acid [UA]). Therefore, we believe that the chip described in this study has broad potential application in the field of cost-effective multiplex detection. [Display omitted] • A shared-cathode closed bipolar electrochemiluminescence (SC-CBP-ECL) is reported. • The combination of cloth-based C-BPE and double ECL system is presented. • The SC-CBP-ECL can be used for coinstantaneous detection of seven glucose samples. • The SC-CBP-ECL can be applied for simultaneous detection of three different targets. • The proposed multiplex detection method is cost-effective. [ABSTRACT FROM AUTHOR]