Microfluidic paper-based analytical device for measurement of pH using as sensor red cabbage anthocyanins and gum arabic.

The objective of this study was to develop and validate a novel microfluidic paper-based analytical device (µPADpH) for determining the pH levels in foods. Anthocyanins from red cabbage aqueous extract (RCAE) were used as its analytical sensor. Whatman No. 1 filter paper was the most suitable for the device due to its porosity and fiber organization, which allows for maximum color intensity and minimal color heterogeneity of the RCAE in the detection zone of the µPADpH. To ensure the color stability of the RCAE for commercial use of the µPADpH, gum arabic was added. The geometric design of the µPADpH, including the channel length and separation zone diameter, was systematically optimized using colored food. The validation showed that the µPADpH did not differ from the pH meter when analyzing natural foods. However, certain additives in processed foods were found to increase the pH values.

Microfibrous Carbon Paper Decorated with High-Density Manganese Dioxide Nanorods: An Electrochemical Nonenzymatic Platform of Glucose Sensing.

Nanorod structures exhibit a high surface-to-volume ratio, enhancing the accessibility of electrolyte ions to the electrode surface and providing an abundance of active sites for improved electrochemical sensing performance. In this study, tetragonal α-MnO2 with a large K+-embedded tunnel structure, directly grown on microfibrous carbon paper to form densely packed nanorod arrays, is investigated as an electrocatalytic material for non-enzymatic glucose sensing. The MnO2 nanorods electrode demonstrates outstanding catalytic activity for glucose oxidation, showcasing a high sensitivity of 143.82 µA cm-2 mM-1 within the linear range from 0.01 to 15 mM, with a limit of detection (LOD) of 0.282 mM specifically for glucose molecules. Importantly, the MnO2 nanorods electrode exhibits excellent selectivity towards glucose over ascorbic acid and uric acid, which is crucial for accurate glucose detection in complex samples. For comparison, a gold electrode shows a lower sensitivity of 52.48 µA cm-2 mM-1 within a linear range from 1 to 10 mM. These findings underscore the superior performance of the MnO2 nanorods electrode in both sensitivity and selectivity, offering significant potential for advancing electrochemical sensors and bioanalytical techniques for glucose monitoring in physiological and clinical settings.

Chemical Derivatization and Paper Spray Ionization Mass Spectrometry for Fast Screening of Retinoic Acid in Cosmetics.

As a prescription drug, retinoic acid is listed as a banned cosmetic additive in the EU and China regulations. Currently, spectrophotometric methods, including thin-layer chromatography (TLC), high-performance liquid chromatography (HPLC), and HPLC-MS/MS, are commonly used for the determination of retinoic acid. As these conventional methods require complex pretreatment and are time-consuming, chemical derivatization combined with paper spray ionization mass spectrometry was developed for the fast detection of retinoic acid in cosmetics. N,N-dimethylpiperazine iodide (DMPI) was utilized as a derivatization reagent. Carboxylic acid in retinoic acid was derivatized to carry a positive charge and was subjected to mass spectrometry analysis. Results showed that compared with non-derivatized compounds, the detection limit was increased by about 50 times. The linearity in the range of 0.005-1 µg·mL-1 was good. The limit of detection (LOD) was 0.0013 µg·mL-1, and the limit of quantification (LOQ) was 0.0043 µg·mL-1. The recoveries of spiked samples were in the range of 95-105%, and the RSDs were below 5%. Derivatization and paper spray ionization MS render a quick, sensitive, and accurate method for the detection of retinoic acid in a complex matrix.

Paper-Based Microfluidic Device for Extracellular Lactate Detection.

Lactate is a critical regulatory factor secreted by tumors, influencing tumor development, metastasis, and clinical prognosis. Precise analysis of tumor-cell-secreted lactate is pivotal for early cancer diagnosis. This study describes a paper-based microfluidic chip to enable the detection of lactate levels secreted externally by living cells. Under optimized conditions, the lactate biosensor can complete the assay in less than 30 min. In addition, the platform can be used to distinguish lactate secretion levels in different cell lines and can be applied to the screening of antitumor drugs. Through enzymatic chemical conversion, this platform generates fluorescent signals, enabling qualitative assessment under a handheld UV lamp and quantitative analysis via grayscale intensity measurements using ImageJ (Ver. 1.50i) software. The paper-based platform presented in this study is rapid and highly sensitive and does not necessitate other costly and intricate instruments, thus making it applicable in resource-constrained areas and serving as a valuable tool for investigating cell lactate secretion and screening various anti-cancer drugs.

Sensitive and reliable lab-on-paper biosensor for label-free detection of exosomes by electrochemical impedance spectroscopy.

A new, sensitive, and cost-effective lab-on-paper-based immunosensor was designed based on electrochemical impedance spectroscopy (EIS) for the detection of exosomes. EIS was selected as the determination method since there was a surface blockage in electron transfer by binding the exosomes to the transducer. Briefly, the carbon working electrode (WE) on the paper electrode (PE) was modified with gold particles (AuPs@PE) and then conjugated with anti-CD9 (Anti-CD9/AuPs@PE) for the detection of exosomes. Variables involved in the biosensor design were optimized with the univariate mode. The developed method presents the limit of detection of  8.7 × 102 exosomes mL-1, which is lower than that of many other available methods under the best conditions. The biosensor was also tested with urine samples from cancer patients with high recoveries. Due to this  a unique, low-cost, biodegradable technology is presented that can directly measure exosomes without labeling them for early cancer or metastasis detection.

Development of a µPAD for the point-of-care testing of serum glutamic oxaloacetic transaminase (SGOT).

A wax-patterned paper analytical device (µPAD) has been developed for point-of-care colourimetric testing of serum glutamic oxaloacetic transaminase (SGOT). The detection method was based on the transamination reaction of aspartate with α-ketoglutarate, leading to the formation of oxaloacetate which reacts with the reagent Fast Blue BB salt and forms a cavern pink colour. The intensity of the cavern pink colour grows as the concentration of SGOT increases. UV-visible spectroscopy was utilized to optimize reaction conditions, and the optimized reagents were dropped onto the wax-patterned paper. The coloured PADs, after the addition of SGOT, have been photographed, and a colour band has been generated to correlate the SGOT concentration visually. The images were used to calculate the intensity values using ImageJ software, which inturn was used to calculate the SGOT concentration. The PADs were also tested with serum samples, and SGOT spiked serum samples. The PAD could detect the SGOT concentration ranging from 5 to 200 U/L. The analysis yielded highly accurate results with less than 6% relative error compared to the clinical sample. This colourimetric test demonstrated exceptional selectivity in the presence of other biomolecules in the blood serum, with a detection limit of 2.77 U/L and a limit of quantification of 9.25 U/L. Additionally, a plasma separation membrane was integrated with the PAD to directly test SGOT from finger-prick blood samples.

Deep Learning-Based Kinetic Analysis in Paper-Based Analytical Cartridges Integrated with Field-Effect Transistors.

This study explores the fusion of a field-effect transistor (FET), a paper-based analytical cartridge, and the computational power of deep learning (DL) for quantitative biosensing via kinetic analyses. The FET sensors address the low sensitivity challenge observed in paper analytical devices, enabling electrical measurements with kinetic data. The paper-based cartridge eliminates the need for surface chemistry required in FET sensors, ensuring economical operation (cost < $0.15/test). The DL analysis mitigates chronic challenges of FET biosensors such as sample matrix interference, by leveraging kinetic data from target-specific bioreactions. In our proof-of-concept demonstration, our DL-based analyses showcased a coefficient of variation of <6.46% and a decent concentration measurement correlation with an r2 value of >0.976 for cholesterol testing when blindly compared to results obtained from a CLIA-certified clinical laboratory. These integrated technologies have the potential to advance FET-based biosensors, potentially transforming point-of-care diagnostics and at-home testing through enhanced accessibility, ease-of-use, and accuracy.

Effect of incubation conditions of cellulase hydrolysis on mechanical pulp fibre morphology.

The mechanical pulp industry is diversifying through the manufacture of high-value paper products, such as microfibrillated cellulose. However, the development of fibre quality is still energy-intensive. Enzymatic hydrolysis is hypothesized to promote fibre cutting, greater fibrillation, and reduce refining energy costs. Despite potential benefits, there is little understanding of the mechanisms behind fibre development during enzymatic hydrolysis of mechanical pulp. This work investigates how incubation pH and temperature during enzymatic hydrolysis impact the refining of mechanical pulp short fibres. Incubation with endoglucanase at pH 5 and 60 °C increased fibre cutting by approximately 20 %. Fibrillation was negatively affected at this condition, resulting in increased slim fines formation with refining. Incubation at pH 8 and 80 °C promoted >15 % reduction in fibre length, despite such conditions being associated with low enzyme activity. The pH variation modified the sedimentation height of the fibres and the conductivity of suspensions, indicating a change in fibre surface charge. Fibre morphology changes were induced by enzyme hydrolysis conducted at conditions representative of the full range of pH and temperature observed in mechanical pulp mills.

Fabrication of highly fluorescent graphene quantum dots for quantification of As3+ ion using modified cellulose paper.

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 As3+ 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 As3+ via aggregation-based fluorescence "turn-off" mechanism. The linear range for quantitating As3+ 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 As3+ ion in water samples. The CA-GQDs-embedded paper strip can be easily extended for assaying of As3+ ion, which meets the demand for monitoring of As3+ ion in real samples.

A portable lateral flow distance-based paper sensor for drinking water hardness test.

Hardness is one of the basic parameters of water, and a high-level hardness of drinking water may be harmful to human health. Thus, it is very important to monitor drinking water hardness. In this work, a portable lateral flow distance-based paper sensor for the semi-quantitative detection of drinking water hardness is demonstrated. In the presence of Ca2+/Mg2+, the hydrogel can be formed via the chelation between sodium alginate and Ca2+/Mg2+, inducing a phase separation process. The viscosity change of the sodium alginate solution is directly related to the Ca2+/Mg2+ concentration and can be determined by the water lateral flow distance on test strips. The sensor successfully realizes the quantification of Ca2+ and Mg2+ in the range of 0-10 mmol L-1 and 4-20 mmol L-1, respectively. The recoveries are found varied from 95% to 108.9%. The water hardness is acceptable for drinking if the Cr values lies in the range of 0.259 to 0.419, and it is high with the Cr value above 0.595. Remarkably, the performance of the sensor is comparable with the commercial kit for real water samples, which avoids the subjective judgment. Overall, this method provides a portable approach for semi-quantitative detection of drinking water hardness with the merits of convenience and low cost, which shows great potential for the potential application.

Wearable electrochemical device based on butterfly-like paper-based microfluidics for pH and Na+ monitoring in sweat.

A wearable potentiometric device is reported based on an innovative butterfly-like paper-based microfluidic system, allowing for continuous monitoring of pH and Na+ levels in sweat during physical activity. Specifically, the use of the butterfly-like configuration avoids evaporation phenomena and memory effects, enabling precise and timely biomarker determination in sweat. Two ad hoc modified screen-printed electrodes were embedded in the butterfly-like paper-based microfluidics, and the sensing device was further integrated with a portable and miniaturized potentiostat, leveraging Bluetooth technology for efficient data transmission. First, the paper-based microfluidic configuration was tested for optimal fluidic management to obtain optimized performance of the device. Subsequently, the two electrodes were individually tested to detect the two biomarkers, namely pH and Na+. The results demonstrated highly promising near-Nernstian (0.056 ± 0.002 V/dec) and super-Nernstian (- 0.080 ± 0.003 V/pH) responses, for Na+ and pH detection, respectively. Additionally, several important parameters such as storage stability, interferents, and memory effect by hysteresis study were also investigated. Finally, the butterfly-like paper-based microfluidic wearable device was tested for Na+ and pH monitoring during the physical activity of three volunteers engaged in different exercises, obtaining a good correlation between Na+ increase and dehydration phenomena. Furthermore, one volunteer was tested through a cardiopulmonary test, demonstrating a correlation between sodium Na+ increase and the energetic effort by the volunteer. Our wearable device highlights the high potential to enable early evaluation of dehydration and open up new opportunities in sports activity monitoring.

Treatment of pulp and paper mill effluent through combined aerobic and anaerobic suspended fixed-bed bioreactor.

This study explored using ultrafiltration (UF) membranes to treat pulp and paper mill wastewater, implementing a novel Taguchi experimental design to optimize operating conditions for pollutant removal and minimal membrane fouling. Researchers examined four factors: pH, temperature, transmembrane pressure, and volume reduction factor (VRF), each at three levels. Optimal conditions (pH 10, 25°C, 6 bar, VRF 3) led to a 35% reduction in flux due to fouling and high pollutant rejections: total hardness (83%), sulfate (97%), spectral absorption coefficient (SAC254) (95%), and chemical oxygen demand (COD) (89%). Conductivity had a lower rejection rate of 50%. Advanced imaging techniques like atomic force microscopy (AFM) and scanning electron microscopy (SEM) revealed reduced membrane fouling under these conditions. The Taguchi method effectively identified optimal conditions, significantly improving wastewater treatment efficiency and promoting environmental sustainability in the pulp and paper industry. PRACTITIONER POINTS: This study optimized UF membrane conditions for pulp and paper mill wastewater, reducing fouling and enhancing pollutant removal, offering practical strategies for industrial treatment. AFM and SEM provided key insights into membrane fouling and mitigation, promoting real-time diagnosis and optimization for enhanced treatment efficiency. Prioritizing anaerobic fixed-bed systems in wastewater treatment is beneficial for achieving high COD removal efficiency. Optimizing hydraulic retention time (HRT) in these systems can further improve their overall effectiveness and sustainability.

Chemical and toxicological characterization of food contact recycled paperboard extracts.

Food contact paperboard poses a potential risk of food contamination due to the possible release of chemicals (intentionally added or not), particularly in recycled paperboard. Water extractions were performed, according to wet food procedures, of paperboard samples collected from a manufacturer at the beginning and the end of a recycling production chain. Chemical analysis and hormonal activities in vitro of water extracts were studied. ICP-MS analysis confirmed the presence of 15 trace elements with lower concentrations after the recycling process, with the exception of chlorine. The chromatographic analyses demonstrated that the identified substances in the starting paperboard, before the recycling process, were approximately twice as high as in the end paperboard, after the recycling process. These substances included also natural wood products, chemical additives, and undesirable substances such as phthalates. Two major products (3,5-di-tert-butylphenol and methyl-2-pyrrolidone) were found in the starting and the end paperboard extracts, respectively. Two common substances were identified in both extracts: 2,4-di-tert-buthylphenol and dehydroabietic acid. Evaluation of potential endocrine disruption showed that the starting paperboard extract exhibited oestrogenic and antiandrogenic effects, while these effects nearly disappeared in the end paperboard extract. These results confirmed that the recycling process was effective in removing most of the contaminant substances.

Functionalized N95 Face Mask with a Chemical-Free Paper-Based Collector for Exhaled Breath Analysis: SARS-CoV-2 Detection with a Printed Immunosensor as a Case Study.

Exhaled breath electrochemical sensing is a promising biomedical technology owing to its portability, painlessness, cost-effectiveness, and user-friendliness. Here, we present a novel approach for target analysis in exhaled breath by integrating a comfortable paper-based collector into an N95 face mask, providing a universal solution for analyzing several biomarkers. As a model analyte, we detected SARS-CoV-2 spike protein from the exhaled breath by sampling the target analyte into the collector, followed by its detection out of the N95 face mask using a magnetic bead-based electrochemical immunosensor. This approach was designed to avoid any contact between humans and the chemicals. To simulate human exhaled breath, untreated saliva samples were nebulized on the paper collector, revealing a detection limit of 1 ng/mL and a wide linear range of 3.7-10,000 ng/mL. Additionally, the developed immunosensor exhibited high selectivity toward the SARS-CoV-2 spike protein, compared to other airborne microorganisms, and the SARS-CoV-2 nucleocapsid protein. Accuracy assessments were conducted by analyzing the simulated breath samples spiked with varying concentrations of SARS-CoV-2 spike protein, resulting in satisfactory recovery values (ranging from 97 ± 4 to 118 ± 1%). Finally, the paper-based hybrid immunosensor was successfully applied for the detection of SARS-CoV-2 in real human exhaled breath samples. The position of the collector in the N95 mask was evaluated as well as the ability of this paper-based analytical tool to identify the positive patient.

Streamlined integrated protein isoelectric focusing using microfluidic paper-based device.

An innovative integrated paper-based microdevice was developed for protein separation by isoelectric focusing (IEF), allowing for robust design thanks to a 3D-printed holder integrating separation channel, reservoirs, and electrodes. To reach robustness and precision, the optimization focused on the holder geometry, the paper nature, the reservoir design, the IEF medium, and various focusing parameters. A well-established and stable pH gradient was obtained on a glass-fiber paper substrate with simple sponge reservoirs, and the integration of the electrodes in the holder led to a straightforward system. The separation medium composed of water/glycerol (85/15, v/v) allowed for reducing medium evaporation while being an efficient medium for most hydrophobic and hydrophilic proteins, compatible with mass spectrometry detection for further proteomics developments. To our knowledge, this is the first report of the use of glycerol solutions as a separation medium in a paper-based microdevice. Analytical performances regarding pH gradient generation, pI determination, separation efficiency, and resolution were estimated while varying the IEF experimental parameters. The overall process led to an efficient separation within 25 min. Then, this methodology was applied to a sample composed of saliva doped with proteins. A minimal matrix effect was evidenced, underscoring the practical viability of our platform. This low-cost, versatile and robust paper-based IEF microdevice opens the way to various applications, ranging from sample pre-treatment to integration in an overall proteomic-on-a-chip device.

Distance-based paper device coupled with uracil-rich DNA hydrogel for visual quantification of Uracil-DNA glycosylase.

Uracil-DNA glycosylase (UDG), an enzyme for repairing uracil-containing DNA damage, is crucial for maintaining genomic stability. Simple and fast quantification of UDG activity is essential for biological assay and clinical diagnosis, since its aberrant level is associated with DNA damage and various diseases. Herein, we developed a fully integrated "sample in-signal out" distance-based paper analytical device (dPAD) for visual quantification of UDG using a flow-controlled uracil-rich DNA hydrogel (URDH). The uracil base sites contained in the DNA hydrogel are mis-incorporated with dUTP by rolling circle amplification (RCA), which simplifies the preparation process of the functionalized hydrogel. In the presence of UDG, the uracil in URDH can be recognized and removed to induce the permeability change of URDH, resulting in the visible distance signal along the paper channel. Using dPAD, as low as 6.4 × 10-4 U/mL of UDG (within 80 min) is visually identified without any instruments and complicated operations. This integrated dPAD is advantageous for its simplicity, cost effectiveness, and ease of use. We envision that it has the great potential for point-of-care testing (POCT) in DNA damage testing, personalized healthcare assessment, and biomedical applications.

Multi-Functional Repair and Long-Term Preservation of Paper Relics by Nano-MgO with Aminosilaned Bacterial Cellulose.

Paper relics, as carrieres of historical civilization's records and inheritance, could be severely acidic and brittle over time. In this study, the multi-functional dispersion of nanometer magnesium oxide (MgO) carried by 3-aminopropyl triethoxysilane-modified bacterial cellulose (KH550-BC) was applied in the impregnation process to repair aged paper, aiming at solving the key problems of anti-acid and strength recovery in the protection of ancient books. The KH550-BC/MgO treatment demonstrated enhanced functional efficacy in repairing aged paper, attributed to the homogeneous and stable distribution of MgO within the nanofibers of BC networks, with minimal impact on the paper's wettability and color. Furthermore, the treatment facilitated the formation of adequate alkali reserves and hydrogen bonding, resulting in superior anti-aging properties in the treated paper during prolonged preservation. Even after 30 days of hygrothermal aging tests, the paper repaired by KH550-BC/MgO was still in a gently alkaline environment (pH was about 7.56), alongside a 32.18% elevation compared to the untreated paper regarding the tear index. The results of this work indicate that KH550-BC/MgO is an effective reinforcement material for improving the long-term restoration of ancient books.

Improving the performance of kraft paper by cinnamon essential oil/soybean protein isolate microcapsules and konjac glucomannan for citrus preservation.

In order to reduce the quality loss of citrus and extend its storage time after harvest, it is essential to develop coated kraft papers with antibacterial and fresh-keeping properties. In this study, cinnamon essential oil (CEO)/soybean protein isolate (SPI) microcapsules were prepared by the coagulation method, and their properties were optimized. Then, the microcapsules were added to konjac glucomannan (KGM) as a coating solution to enhance the physical, and chemical properties of kraft paper by a coating method. The release behavior of CEO, tensile properties, antibacterial properties and preservation effects of the paper were investigated. The results show that when the ratio of wall to core was 7:3, the highest encapsulation rate was 92.20 ± 0.43 %. The coating treatment significantly reduced the oxygen and water vapor transmission rates of kraft paper. The shelf life of citrus treated with coated Kraft was extended by >10 days. Thus, the CEO/SPI microencapsulation and KGM coating could improve the properties of kraft paper and have the potential for citrus preservation.

Competitive coordination assisted scalable fabrication of FITC­nickel frameworks anchored nanofiber paper for colorimetric/fluorescent monitoring of shrimp freshness.

A novel type of colorimetric/fluorescent nanopaper indicator has been developed from the melt-extruded poly (vinyl alcohol-co-ethylene) nanofibers with surface anchored metal-organic frameworks (MOFs) by an interfacial coordination strategy. Specifically, the fluorescein isothiocyanate molecules could be anchored to the nanofiber surface by nickel ions and co-assembled into a hydrophilic nanocoating via a dynamic water/alcohol solvent evaporation method. Interestingly, this hydrophilic surface enables fast adsorption of moistures and interaction with biological amine vapors, resulting a saffron cake-layer of MOF nanocrystals with ultra-sensitive colorimetric/fluorescent responses based on an alkaline pH/ammonia induced competitive coordination mechanism. Finally, these porous nanofibrous matrix and active nanocoating make the nano-paper an ultra-sensitive optical platform for in-situ monitoring of the shrimp freshness from mins to weeks. Therefore, this composite film shows great potential into advanced paper-based indicators for food quality control and safety in processing industry.

Waste newspaper as cellulose resource of activated carbon by sodium salts for methylene blue and congo red removal.

The work was aimed at evaluating the adsorptive properties of waste newspaper (WN) activated carbons chemically produced using sodium salts for methylene blue (MB) and congo red (CR) removal. The activated carbons, designated as AC1, AC2, AC3 and AC4 were prepared through impregnation with NaH2PO4, Na2CO3, NaCl and NaOH, respectively and activation at 500 °C for 1 h. The activated carbons were characterized for surface chemistry, thermal stability, specific area, morphology and composition. The AC1 with a surface area of 917 m2/g exhibits a greater MB capacity of 651 mg/g. Meanwhile, a greater CR capacity was recorded by AC2 at 299 mg/g. The pseudo-second order model fitted well with the kinetic data, while the equilibrium data could be described by Langmuir model. The thermodynamic parameters, i.e.., positive ΔH°, negative ΔG° and positive ΔS° suggest that the adsorption of dyes is endothermic, spontaneous and feasible at high solution temperature. To conclude, WN is a potential cellulose source for producing activated carbon, while NaH2PO4 activation could be employed to convert WN into activated carbon for effective dye wastewater treatment.