Measurement of sucrose concentration using Imbibition length on paper: A device for equipment-free and environmentally-friendly detection.

The Lucas-Washburn equation is commonly used to predict the distance (L) that a liquid travels through paper. This equation establishes that L2 is linear with time and inversely proportional to the viscosity of the liquid. However, there is currently no theoretical equation connecting the viscosity of a solution to its concentration. In this study, the imbibition flow of a sucrose solution was measured along the length of a horizontal strip of filter paper, featuring a printed, thermometer-shaped hydrophobic boundary. A sample (38 µL) was dispensed onto the bulb area, and the solution's flow was visually tracked using a red dye added to the sample. The imbibition length (L) was measured by a vernier caliper at 10.0 min after the sample addition. An empirical equation, based on literature values of the viscosity (η) and concentration (C) of sucrose solutions, was proposed. By integrating this empirical equation with the Lucas-Washburn equation, the following equation was derived: L = a⋅exp{-(bC + cC2)}, where 'a', 'b' and 'c' are parameters. This equation was fitted to the dataset of L and C, covering C values from 0 to 60 % w/w standard sucrose solutions, resulting in a coefficient of determination of 0.9987. The plot of L against C was observed to closely follow a linear line, with a fitting providing a coefficient of determination of 0.9986. The sucrose contents in samples, such as soft drinks, syrups, and sugarcanes, determined using the imbibition length method and conventional refractometry, were in statistical agreement via the paired t-test at the 95 % confidence level. This method is simple, instrument-free, requiring only a small amount of safe red food dye, and can be conducted on-site.

Simple and Equipment-Free Paper-Based Device for Determination of Mercury in Contaminated Soil.

This work presents a simple and innovative protocol employing a microfluidic paper-based analytical device (µPAD) for equipment-free determination of mercury. In this method, mercury (II) forms an ionic-association complex of tetraiodomercurate (II) ion (HgI42-(aq)) using a known excess amount of iodide. The residual iodide flows by capillary action into a second region of the paper where it is converted to iodine by pre-deposited iodate to liberate I2(g) under acidic condition. Iodine vapor diffuses across the spacer region of the µPAD to form a purple colored of tri-iodide starch complex in a detection zone located in a separate layer of the µPAD. The digital image of the complex is analyzed using ImageJ software. The method has a linear calibration range of 50-350 mg L-1 Hg with the detection limit of 20 mg L-1. The method was successfully applied to the determination of mercury in contaminated soil and water samples which the results agreed well with the ICP-MS method. Three soil samples were highly contaminated with mercury above the acceptable WHO limits (0.05 mg kg-1). To the best of our knowledge, this is the first colorimetric µPAD method that is applicable for soil samples including mercury contaminated soils from gold mining areas.

Paper-based colorimetric biosensor of blood alcohol with in-situ headspace separation of ethanol from whole blood.

This work presents a novel development that exploits the concept of in-situ gas-separation together with a specific enzymatic colorimetric detection to produce a portable biosensor called "Blood Alcohol Micro-pad" for direct quantitation of ethanol in whole blood. The thin square device (25 mm × 25 mm × 1.8 mm) comprises two layers of patterned filter paper held together with a double-sided mounting tape with an 8-mm circular hole (the headspace). In operation, the reagent is deposited on one layer and covered with sticky tape. Then 8 µL of a blood sample is dispensed onto the opposite layer and covered with sticky tape. Diffusion of ethanol across the 1.6 mm narrow headspace permits selective detection of ethanol by the enzymatic reagents deposited on the opposite layer. This reagent zone contains alcohol oxidase, horseradish peroxidase and 2'-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt, as the chromogenic reagent. The color intensity, measured from the recorded digital image, resulting from the enzymatic assay of ethanol, correlates with the concentration of blood alcohol. The results obtained with spiked mice and sheep blood samples, using an external calibration in the range of 1-120 mg dL-1ethanol, gave recoveries of 93.2-104.4% (n = 12). The "Blood Alcohol Micro-pad" gave good precision with %RSD <1 (50 mg dL-1 ethanol, n = 10) and limit of quantification (10SD of intercept/slope) of 11.56 mg dL-1. The method was successfully validated against a headspace gas chromatography-mass spectrometric method. It has good potential for development as a simple and convenient blood alcohol sensor for on-site testing.

T-shirt ink for one-step screen-printing of hydrophobic barriers for 2D- and 3D-microfluidic paper-based analytical devices.

This work presents the use of polyvinyl chloride (PVC) fabric ink, commonly employed for screening t-shirts, as new and versatile material for printing hydrophobic barrier on paper substrate for microfluidic paper-based analytical devices (µPADs). Low-cost, screen-printing apparatus (e.g., screen mesh, squeegee, and printing table) and materials (e.g. PVC ink and solvent) were employed to print the PVC ink solution onto Whatman filter paper No. 4. This provides a one-step strategy to print flow barriers without the need of further processing except evaporation for 3-5 min in a fume hood to remove the solvent. The production of the single layer µPADs is reasonably high with up to 77 devices per screening with 100% success rate. This method produces very narrow fluidic channel 486 ±â€¯14 µm in width and hydrophobic barrier of 642 ±â€¯25 µm thickness. Reproducibility of the production of fluidic channels and zones is satisfactory with RSDs of 2.9% (for 486-µm channel, n = 10), 3.7% (for 2-mm channel, n = 50) and 1.5% (for 6-mm diameter circular zone, n = 80). A design of a 2D-µPAD produced by this method was employed for the colorimetric dual-measurements of thiocyanate and nitrite in saliva. A 3D-µPADs with multiple layers of ink-screened paper was designed and constructed to demonstrate the method's versatility. These 3D-µPADs were designed for gas-liquid separation with in-situ colorimetric detection of ethanol vapor on the µPADs. The 3D-µPADs were applied for direct quantification of ethanol in beverages and highly colored pharmaceutical products. The printed barrier was resistant up to 8% (v/v) ethanol without liquid creeping out of the barrier.

Highly sensitive and selective electrochemical paper-based device using a graphite screen-printed electrode modified with molecularly imprinted polymers coated Fe3O4@Au@SiO2 for serotonin determination.

Herein, we propose a highly sensitive and selective three-dimensional electrochemical paper-based analytical device (3D-ePAD) to determine serotonin (Ser). It uses a graphite-paste electrode modified with nanoparticles coated with molecularly imprinted polymer (MIP). Fe3O4@Au nanoparticles were encapsulated with silica to create novel nano-sized MIP. Morphology and structural characterization reveal that silica imprinted sites (Fe3O4@Au@SiO2) synthesized via sol-gel methods provide excellent features for Ser detection, including high porosity, and greatly improve analyte diffusion and adsorption to provide a faster response by the MIP sensor. The template molecule was effectively removed by solvent extraction to provide a greater number of specific cavities that enhance analyte capacity and sensitivity. The 3D-ePAD was fabricated by alkyl ketene dimer (AKD)-inkjet printing of a circular hydrophobic detection zone on filter paper for application of aqueous samples, coupled with screen-printed electrodes on the paper, which was folded underneath the hydrophobic zone. The sensor was constructed by drop coating of Fe3O4@Au@SiO2-MIP nanocomposites on the graphite electrode (GPE) surface. The MIP sensor (Fe3O4@Au@SiO2-MIP/GPE) was used in the detection of Ser by linear-sweep voltammetry (LSV) in 0.1 M phosphate buffer at pH 8.0. The device exhibits high sensitivity toward Ser, which we attribute to synergistic effects between catalytic properties, electrical conductivity of Fe3O4@Au@SiO2, and significantly increased numbers of imprinted sites. Ser oxidation was observed at +0.39 V. Anodic peak currents for Ser show linearity from 0.01 to 1000 µM (y = 0.0075 ± 0.0049 x + 0.4071 ± 0.0052, r2 = 0.993), with a detection limit of 0.002 µM (3S/N). The device provides good repeatability (%relative standard deviations; RSD) = 4.23%, calculated from the current responses of ten different MIP sensors). The device also exhibits high selectivity and reproducibility (%RSD = 8.35%, obtained from five calibration plots). The analytical performance of the device is suitable for the determination of Ser in pharmaceutical capsules and urine samples.

Simple and green method for direct quantification of hypochlorite in household bleach with membraneless gas-separation microfluidic paper-based analytical device.

This work presents development of a microfluidic paper-based analytical device (µPAD) for direct determination of hypochlorite in household bleach. The recent design of a membraneless gas-separation microfluidic paper-based analytical device (MBL-GS µPAD) was employed to fabricate the hypochlorite-µPAD. Chlorine gas is generated in the µPAD via acidification of an aliquot of sample loaded on to the donor reservoir located at the bottom layer of the µPAD. The liberated chlorine gas diffuses through the air space to oxidize iodide ion previously impregnated in the acceptor reservoir at the top layer of the µPAD, leading to formation of the brown color of the tri-iodide ions. Digital image of the brown zone was captured at exactly 5 min after loading the acid. Image J program is used for analysis of the image for quantification of the hypochlorite in unit of g Cl2 L-1. It was found that employing a relatively large volume of the air space (ca. 270 µL) direct analysis of the high concentration of hypochlorite in the bleach was achieved without prior dilution. The method thus provides a linear working range of 25-100 g Cl2 L-1, which is suitable for most commercial household products. The calibration line has a coefficient of determination of 0.999. The precision of measurements is 0.96% RSD and 0.30% RSD at 30 g Cl2 L-1 and 80 g Cl2 L-1 (n = 10), respectively. Using the paired t-test (P = 0.05, n = 8), the method agreed well with the iodometric titration method. Our µPAD for hypochlorite is portable and cost-effective. The method is also "green" since there is a significant reduction in use of reagents compared to other conventional methods.

Membraneless Gas-Separation Microfluidic Paper-Based Analytical Devices for Direct Quantitation of Volatile and Nonvolatile Compounds.

This work presents new chemical sensing devices called "membraneless gas-separation microfluidic paper-based analytical devices" (MBL-GS µPADs). MBL-GS µPADs were designed to make fabrication of the devices simple and user-friendly. MBL-GS µPADs offer direct quantitative analysis of volatile and nonvolatile compounds. Porous hydrophobic membrane is not needed for gas-separation, which makes fabrication of the device simple, rapid and low-cost. A MBL-GS µPAD consists of three layers: "donor layer", "spacer layer", and "acceptor layer". The donor and acceptor layers are made of filter paper with a printed pattern. The donor and acceptor layers are mounted together with a spacer layer in between. This spacer is a two-sided mounting tape, 0.8 mm thick, with a small disc cut out for the gas from the donor zone to diffuse to the acceptor zone. Photographic image of the color that is formed by the reagent in the acceptor layer is analyzed using the ImageJ program for quantitation. Proof of concept of the MBL-GS µPADs was demonstrated by analyzing standard solutions of ethanol, sulfide, and ammonium. Optimization of the MBL-GS µPADs was carried out for direct determination of ammonium in wastewaters and fertilizers to demonstrate the applicability of the system to real samples.

Simultaneous determination of iodide and creatinine in human urine by flow analysis with an on-line sample treatment column.

This work presents the first flow system for direct analysis of iodide and creatinine suitable for screening of human urine samples. The system had a mini-column packed with strong anion exchange resin for on-line extraction of iodide. After injection of a sample on the column the unretained urine sample was analyzed for creatinine in one section of the flow system using the Jaffe's reaction with spectrometric detection at 520 nm. Iodide was eluted off with 1.42 mL 5 M NaNO3. A 150 µL fraction of the eluate was analyzed in another section of the same flow system for iodide using the kinetic-spectrometric Sandell-Kolthoff reaction. At the optimum condition, the sample throughput was 12 samples per h. The linear working range covered the normal levels of iodide and creatinine in human urine: 0-200 µg I L(-1) and 50-1200 mg creatinine L(-1), respectively. Recoveries tested in 10 samples were 87-104% for iodide and 89-104% for creatinine. Bland-Altman plots (n = 50) showed that the scatter of the differences between values obtained by this method and those of reference methods, for both iodide and creatinine, was within mean ± 2SD.