Fabrication Of Paper-based Analytical Devices Research Articles

Fabrication of paper-based analytical devices using stencil-printed glass varnish barriers for colorimetric detection of salivary α-amylase

BackgroundDeveloping disposable paper-based devices has positively impacted analytical science, particularly in developing countries. Some benefits of those devices include their versatility, affordability, environmentally friendly, and the possibility of being integrated with portable electrochemical or colorimetric detectors. Paper-based analytical devices (PADs) comprising circular zones and microfluidic networks have been successfully employed in the analytical chemistry reign. However, the combination of the stencil-printing method and alternative binder has not been satisfactorily explored for fabricating colorimetric paper devices. ResultsWe developed PADs exploring the stencil printing approach and glass varnish as the hydrophobic chemical agent. As a proof-of-concept, the colorimetric assay of salivary α-amylase (sAA) was performed in saliva samples. Through the scanning electron microscopy measurements, it was possible to indicate satisfactory definitions between native fibers and barrier, and that the measured values for the channel width revealed suitable fidelity (R2 = 0.99) with the nominal widths (ranging from 400 to 5000 μm). The proposed hydrophobic barrier exhibited excellent chemical resistance. The analytical applicability for detecting sAA revealed linear behavior in the range from 2 to 12 U mL−1 (R2 = 0.99), limit of detection of 0.75 U mL−1, reproducibility (RSD ≤2.4%), recovery experiments ranged from 89 to 108% and AGREE response (0.86). In addition, the colorimetric analysis of sAA in four different saliva samples demonstrated levels ranging from 202 to 2080 U mL−1, which enabled monitoring the absence and presence of periodontitis. SignificanceThis report has presented the first use of a self-adhesive mask and glass varnish for creating circular zones and microfluidic architectures on paper without using thermic or UV curing treatments. Also, the proposed analytical methodology for detecting sAA exhibited suitable ecological impact considering the AGREE tool. We believe the proposed fabrication of paper devices emerges as a novel, simple, high-fidelity microfluidic channel and portable analytical approach for colorimetric sensing.

Smartphone-integrated colorimetric and microfluidic paper-based analytical devices for the trace-level detection of permethrin.

Permethrin is a pyrethroid pesticide and insect repellent that prevents mosquito-borne infections like dengue and malaria in tropical areas. This work describes a new colorimetric sensor based on metronidazole-stabilized silver nanoparticles (MTZ-AgNPs) for the first rapid, sensitive, and selective permethrin detection. The MTZ-AgNPs-based colorimetric sensor has a limit of detection (LOD) of 0.0104µM and a limit of quantification (LOQ) of 0.0348µM, respectively. The sensor is further integrated with smartphone and microfluidic fabrication of paper-based analytical devices (µPADs) for real-time and on-site detection of permethrin. Under optimal settings, no potential environmental contaminants interfere with permethrin detection, confirming its high selectivity. Finally, the practical applicability of sensors is confirmed in real tomato and apple extract samples. The US environmental protection agency's recommended UPLC method validated the detection efficiency of the proposed colorimetric sensor. The % recoveries from UPLC and MTZ-AgNPs suggest that the present sensor can quantitatively analyze permethrin in real samples.

Fabrication of paper-based analytical devices by a laminating method with thermal ink ribbons, sticky notes, and office appliances.

A stencil printing method utilizing sticky notes, a thermal transfer ink ribbon, and office appliances for paper-based analytical device (PAD) fabrication was proposed. A sticky note was attached to a filter paper, and a mask pattern was cut using a cutting machine. A commercially available thermal ink ribbon was then placed over the mask and laminated. We have characterized the fabricated devices. This approach could be used for the fast and mass prototyping of PADs using simple office appliances with no need for a wax printer.

Rapid, Simple and Inexpensive Fabrication of Paper-Based Analytical Devices by Parafilm® Hot Pressing.

Paper-based analytical devices have been substantially developed in recent decades. Many fabrication techniques for paper-based analytical devices have been demonstrated and reported. Herein, we report a relatively rapid, simple, and inexpensive method for fabricating paper-based analytical devices using parafilm hot pressing. We studied and optimized the effect of the key fabrication parameters, namely pressure, temperature, and pressing time. We discerned the optimal conditions, including a pressure of 3.8 MPa, temperature of 80 °C, and 3 min of pressing time, with the smallest hydrophobic barrier size (821 µm) being governed by laminate mask and parafilm dispersal from pressure and heat. Physical and biochemical properties were evaluated to substantiate the paper functionality for analytical devices. The wicking speed in the fabricated paper strips was slightly lower than that of non-processed paper, resulting from a reduced paper pore size after hot pressing. A colorimetric immunological assay was performed to demonstrate the protein binding capacity of the paper-based device after exposure to pressure and heat from the fabrication. Moreover, mixing in a two-dimensional paper-based device and flowing in a three-dimensional counterpart were thoroughly investigated, demonstrating that the paper devices from this fabrication process are potentially applicable as analytical devices for biomolecule detection. Fast, easy, and inexpensive parafilm hot press fabrication presents an opportunity for researchers to develop paper-based analytical devices in resource-limited environments.

Fabrication of paper-based analytical devices using a PLA 3D-printed stencil for electrochemical determination of chloroquine and escitalopram.

In recent years, the use of prescribed and non-prescribed drugs has increased. Therefore, advances in new technologies and sensors for detecting molecules in natural environments are required. In this work, a 3D-printed polylactic acid stencil is used to fabricate paper-based analytical devices (ePADs). Herein, we report the use of carbon-based lab-manufactured conductive ink for the fabrication of sensors towards the detection of chloroquine and escitalopram. For each batch, eight ePADs were successfully fabricated. Firstly, the fabricated sensors were evaluated morphologically by scanning electron microscopy and electrochemically by cyclic voltammetry and electrochemical impedance spectroscopy experiments. The sensors displayed a well-defined voltammetric profile in the presence of the redox couple, when compared to a commercial carbon screen-printed electrode. Differential pulse voltammetry conducted the detection of chloroquine and escitalopram with detection limits of 4.0 and 0.5 µmol L−1, respectively. The ePADs fabricated using the 3D stencil are here presented as alternatives for the fabrication of electrochemical analytical devices.Supplementary InformationThe online version contains supplementary material available at 10.1007/s10008-021-05075-w.

Development of a High-Throughput Low-Cost Approach for Fabricating Fully Drawn Paper-Based Analytical Devices Using Commercial Writing Tools

This work reports the development and optimization of a rapid and low-cost pen-on-paper plotting approach for the fabrication of paper-based analytical devices (PADs) using commercial writing stationery. The desired fluidic patterns were drawn on the paper substrate with commercial marker pens using an inexpensive computer-controlled x–y plotter. For the fabrication of electrochemical PADs, electrodes were further deposited on the devices using a second x–y plotting step with commercial writing pencils. The effect of the fabrication parameters (type of paper, type of marker pen, type of pencil, plotting speed, number of passes, single- vs. double-sided plotting), the chemical resistance of the plotted devices to different solvents and the structural rigidity to multiple loading cycles were assessed. The analytical utility of these devices is demonstrated through application in optical sensing of total phenols using reflectance calorimetry and in electrochemical sensing of paracetamol and ascorbic acid. The proposed manufacturing approach is simple, low cost, flexible, rapid and fit-for-purpose and enables the fabrication of sub-“one-dollar” PADs with satisfactory mechanical and chemical resistance and good analytical performance.

3D-PAD: Paper-Based Analytical Devices with Integrated Three-Dimensional Features.

This paper describes the use of fused deposition modeling (FDM) printing to fabricate paper-based analytical devices (PAD) with three-dimensional (3D) features, which is termed as 3D-PAD. Material depositions followed by heat reflow is a standard approach for the fabrication of PAD. Such devices are primarily two-dimensional (2D) and can hold only a limited amount of liquid samples in the device. This constraint can pose problems when the sample consists of organic solvents that have low interfacial energies with the hydrophobic barriers. To overcome this limitation, we developed a method to fabricate PAD integrated with 3D features (vertical walls as an example) by FDM 3D printing. 3D-PADs were fabricated using two types of thermoplastics. One thermoplastic had a low melting point that formed hydrophobic barriers upon penetration, and another thermoplastic had a high melting point that maintained 3D features on the filter paper without reflowing. We used polycaprolactone (PCL) for the former, and polylactic acid (PLA) for the latter. Both PCL and PLA were printed with FDM without gaps at the interface, and the resulting paper-based devices possessed hydrophobic barriers consisting of PCL seamlessly integrated with vertical features consisting of PLA. We validated the capability of 3D-PAD to hold 30 μL of solvents (ethanol, isopropyl alcohol, and acetone), all of which would not be retained on conventional PADs fabricated with solid wax printers. To highlight the importance of containing an increased amount of liquid samples, a colorimetric assay for the formation of dimethylglyoxime (DMG)-Ni (II) was demonstrated using two volumes (10 μL and 30 μL) of solvent-based dimethylglyoxime (DMG). FDM printing of 3D-PAD enabled the facile construction of 3D structures integrated with PAD, which would find applications in paper-based chemical and biological assays requiring organic solvents.

Alternative Patterning Methods for Paper-based Analytical Devices Using Nail Polish as a Hydrophobic Reagent

A rapid, easy, and cost effective fabrication method for paper-based analytical devices (PADs) is described. This newly developed method is based on the use of nail polish as an alternative hydrophobic reagent, and the nail polish was resistant to basic and organic solvents. Three approaches for fabrication of paper-based analytical devices (PADs) were investigated, namely writing, stamping, and spraying. The writing approach was carried out by drawing the hydrophobic area of a pre-designed pattern on filter paper with a simple lab-made pen filled with nail polish as the hydrophobic agent. The stamping and spraying approaches required the use of a designed mask, which was made by laser cutting of the magnet rubber sheet. With laser cutting, two types of templates were made, i.e., positive and negative counterparts. The positive counterpart was the inside pattern and the negative counterpart was the outside pattern of the magnet sheets. For the stamping approach, the negative counterpart of the magnet rubber mask was attached onto a simple rubber stamper that was then stamped onto filter paper after loading with nail polish solution. With the spraying method, the positive counterpart was used to cover the hydrophilic area on the paper. Then, the nail polish solution was used with an air brush and sprayed on the paper covered with the magnet rubber mask. All approaches were cost effective and required neither extra equipment nor any pretreatment step. Among all three methods, however, the spraying method was found most suitable for mass production and provided the best resolution when compared with the other two approaches. With this approach, the actual channel widths obtained were similar to the designed widths, with the narrowest possible channel width of 650 μm. Furthermore, a nail polish-treated PAD was prepared by soaking the paper in the nail polish solution. The ability of the nail polish-treated PAD was examined for its resistance to a strong basic solution and an organic solvent (up to 30% ethanol and dichloromethane). The nail polish-treated paper also showed the potential to be used as an organic-aqueous separator.

Superhydrophobic titania nanoparticles for fabrication of paper-based analytical devices: An example of heavy metals assays

A new strategy has been introduced to successfully fabricate the hydrophobic barriers of PADs by using organofluorine-modified superhydrophobic TiO2 NPs. Superhydrophobic TiO2-140 NPs with high-photoactivity can be converted to hydrophilicity by self-degradation of surface organic moieties under full spectrum light irradiation. Superhydrophobic TiO2-RT NPs with low-photoactivity exhibits good hydrophobic stability under light irradiation. Thus, combining these features, the PADs have been designed and constructed by photo-induced fabrication of hydrophobic barriers on the surface of the paper. To demonstrate the effectiveness of the constructed PADs, colorimetric detections have been displayed for Fe3+ and Ni2+ ions. The synchronous multi-component detections based on the “multi-channel” PADs and the intuitive detections based on the “chemical-symbol-style” PADs are rapid and feasible. A detection range of Fe3+ and Ni2+ ions based on the “circle-array” PAD is applicable and reliable in 0.2–6.0 mM and 0.4–4.0 mM, respectively. Thus, these results make it to be believed that this new strategy provides an alternative way to effectively construct the PADs.

Fabricating Simple Wax Screen-Printing Paper-Based Analytical Devices To Demonstrate the Concept of Limiting Reagent in Acid–Base Reactions

In this article, a low-cost, simple, and rapid fabrication of paper-based analytical devices (PADs) using a wax screen-printing method is reported here. The acid–base reaction is implemented in the simple PADs to demonstrate to students the chemistry concept of a limiting reagent. When a fixed concentration of base reacts with a gradually increasing concentration of acid, a dramatic demonstration allows students to discover the limiting reagent by naked eyes observing the color change from phenolphthalein as an indicator. This demonstration is not only a new approach to enhancing students’ learning of the chemistry concept of the limiting reagent, but also presents potential applications of PADs into all levels of chemistry from middle school through college classes.

Fabrication of paper-based analytical devices optimized by central composite design.

In this work, an application of a design of experiments approach for the optimization of an isoniazid assay on a single-area inkjet-printed paper-based analytical device (PAD) is described. For this purpose, a central composite design was used for evaluation of the effect of device geometry and amount of assay reagents on the efficiency of the proposed device. The factors of interest were printed length, width, and sampling volume as factors related to device geometry, and amounts of the assay reagents polyvinyl alcohol (PVA), NH4OH, and AgNO3. Deposition of the assay reagents was performed by a thermal inkjet printer. The colorimetric assay mechanism of this device is based on the chemical interaction of isoniazid, ammonium hydroxide, and PVA with silver ions to induce the formation of yellow silver nanoparticles (AgNPs). The in situ-formed AgNPs can be easily detected by the naked eye or with a simple flat-bed scanner. Under optimal conditions, the calibration curve was linear in the isoniazid concentration range 0.03-10 mmol L-1 with a relative standard deviation of 3.4% (n = 5 for determination of 1.0 mmol L-1). Finally, the application of the proposed device for isoniazid determination in pharmaceutical preparations produced satisfactory results.

Facile fabrication of paper-based analytical devices for rapid and highly selective colorimetric detection of cesium in environmental samples

Cesium (Cs), a radioactive contaminant of the ecosystem, causes a major risk to human health and environments. This chemo-indicator is designed to exhibit a powerful detection capability featuring high selectivity and sensitivity to inactive Cs.

Fabrication of paper-based analytical device by silanisation of filter cellulose using alkyltrimethoxysilane coupled with UV radiation

AbstractA method was developed for the fabrication of microfluidic paper-based analytical devices (μPAD). This method was based on the silanisation of cellulose in filter paper using alkyltrimethoxysilane coupled with UV radiation. The filter paper sheet was hydrophobised by immersion in an octadecyltrimethoxysilane/heptane (OTMS/heptane) solution (0.25 vol. %) containing 5 vol. % of ethyl acetate (EtOAc). The hydrophobic-hydrophilic contrast was generated on the filter paper after the hydrophobised paper sheet was exposed to UV light with a metal mask creating the desired pattern on the sheet. The exposed area was oxidised to create a hydrophilic area, while the hydrophobic area was protected by the metal mask. The optimal conditions for the fabrication of μPAD were studied; these included ethyl acetate concentration (CEtOAc), immersion time, octadecyltrimethoxysilane concentration (COTMS) and exposure time. This method is costeffective and simple. In addition, different functional groups could be further grafted for various assay purposes. To demonstrate the feasibility of the μPAD in analytical applications, a flowershaped μPAD with eight channels and eight detection units was fabricated and used to determine the nitrite content in pickled vegetables. The nitrite content (124 μg g