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Abstract In this study, we introduce a uricase-immobilized paper (UOx­-paper) integrated electrochemical sensor for detection of uric acid (UA) in saliva. The UOx was immobilized on the detection zone in the wax-patterned paper substrate. This UOx-paper was integrated with a Prussian blue­-modified, screen-printed carbon electrode after electropolymerization of o-phenylenediamine to construct an electrochemical cell for small-volume (20 μL) of samples. First, we optimized the fabrication conditions of UOx-paper. Next, the amperometric response of the UOx-paper-based electrochemical UA sensor was analyzed using a known concentration of UA standard solution in artificial saliva at an applied potential of − 0.1 V (versus Ag pseudo-reference electrode). The UOx-­paper based electrochemical UA sensor showed a sensitivity of 4.9 μA·mM−1 in a linear range of 50 to 1000 μM (R2 = 0.998), high selectivity and good reproducibility, as well as a limit of detection of 18.7 μM (0.31 mg/dL) UA. Finally, we quantified the UA levels in undiluted saliva samples of healthy controls (n = 20) and gout patients (n = 8). The levels were correlated with those measured with conventional salivary UA enzymatic assays as well as serum UA levels. The UOx-paper-based electrochemical UA sensor is a user-friendly and convenient tool to assess salivary UA levels.

Abstract Various agents, including ethylenediaminetetraacetic acid, oxalic acid, citric acid, and HCl, were applied to remove heavy metals from raw paper incineration ash and render the ash recyclable. Among these prepared agent solutions, ethylenediaminetetraacetic acid showed the highest efficiency for Pb removal, while oxalic acid showed the highest efficiencies for Cu, Cd, and As removal. Additionally, three modes of an advanced removal method, which involved the use of both ethylenediaminetetraacetic acid and oxalic acid, were considered for use at the end of the rendering process. Among these three modes of the advanced removal method, that which involved the simultaneous use of ethylenediaminetetraacetic acid and oxalic acid, i.e., a mixture of both solutions, showed the best heavy metal removal efficiencies. In detail, 11.9% of Cd, 10% of Hg, 28.42% of As, 31.29% of Cu, and 49.19% of Pb were removed when this method was used. Furthermore, the application of these three modes of the advanced removal method resulted in a decrease in the amounts of heavy metals eluted and brought about an increase in the CaO content of the treated incineration ash, while decreasing its Cl content. These combined results enhanced the solidification effect of the treated incineration ash. Thus, it was confirmed that the advanced removal method is a promising strategy by which recyclable paper incineration ash can be obtained.

Abstract Oxazolidine is a new category of stimuli-chromic organic compounds with unique characteristics in response to polarity, pH changes, water, light, and metal ions that were well-known as solvatochromism, acidochromism, hydrochromism, photochromism, and ionochromism, respectively. Therefore, oxazolidine derivatives have been developed for their potential applications in chemosensors, anticounterfeiting, and rewritable hydrochromic papers. In this study, various oxazolidine derivatives containing hydroxyl and naphthalene substituted groups were synthesized by using two different indolenine compounds. The synthesized oxazolidine derivatives were used for investigation of solvatochromism in different solvents, and also acidochromism in various pHs by using UV–Vis and fluorescence spectroscopies. In addition, the oxazolidine derivatives were coated on cellulosic papers using a layer-by-layer strategy to develop rewritable acidochromic papers for printing of security tags on cellulosic papers by using acidic and alkaline solutions as water-based inks. Therefore, the developed rewritable acidochromic papers could be used as security papers.

Abstract Up-converting nanoparticles can be a demand for requirements in many areas, including bioimaging and conversion of energy, but also in the battle against counterfeiting. The properties of lanthanide ions make falsification difficult or even impossible using appropriately designed systems. The proposition of such an approach is the NaErF4:Tm3+@NaYF4 core@shell up-converting nanoparticles combined with transparent varnishes. Given the spectroscopic properties of Er3+ ions present in the fluoride matrix, the obtained up-converting nanoparticles absorb light by 808 and 975 nm wavelengths. The intentionally co-doped Tm3+ ions enable tuning characteristic green Er3+ emission to red luminescence, particularly desirable in anti-counterfeiting applications. The article includes a thorough analysis of structural and morphological properties. Moreover, this work shows that exclusive luminescent properties of NaErF4:Tm3+@NaYF4 NPs can be given to the transparent varnish, providing an excellent anti-counterfeiting system, revealing red emission under two different excitation wavelengths.

Abstract Paper-based biosensors featuring immunoconjugated gold nanoparticles have gained extraordinary momentum in recent times as the platform of choice in key cases of field applications, including the so-called rapid antigen tests for SARS-CoV-2. Here, we propose a revision of this format, one that may leverage on the most recent advances in materials science and data processing. In particular, we target an amplifiable DNA rather than a protein analyte, and we replace gold nanospheres with anisotropic nanorods, which are intrinsically brighter by a factor of ~ 10, and multiplexable. By comparison with a gold-standard method for dot-blot readout with digoxigenin, we show that gold nanorods entail much faster and easier processing, at the cost of a higher limit of detection (from below 1 to 10 ppm in the case of plasmid DNA containing a target transgene, in our current setup). In addition, we test a complete workflow to acquire and process photographs of dot-blot membranes with custom-made hardware and regression tools, as a strategy to gain more analytical sensitivity and potential for quantification. A leave-one-out approach for training and validation with as few as 36 sample instances already improves the limit of detection reached by the naked eye by a factor around 2. Taken together, we conjecture that the synergistic combination of new materials and innovative tools for data processing may bring the analytical sensitivity of paper-based biosensors to approach the level of lab-grade molecular tests.

Abstract The homeostatic control of Sodium (Na+) ion in the human body assumes paramount relevance owing to its physiological importance. Any deviation from the normal level causes serious health problems like hypernatremia, hyponatremia, stroke, kidney problems etc. Therefore, quantification of Na+ levels in body fluids has significant diagnostic and prognostic importance. However, interfering ions like Potassium ion (K+) is the major hurdle in sodium detection. In this work, we synthesized the clusters of 3–9 nm-sized highly stable and pure Copper nanoparticles surface functionalised with curcumin, through chemical reduction method. Each cluster of particles is encapsulated in a curcumin layer which is clearly visible in TEM images. The results show that these curcumin functionalized Cu NPs (CuC) are highly selective to the colorimetric detection of Na+. The ions like K+, Mg2+ and Zn2+ did not interfere with the Na+ in this sensing technique. Low-cost paper-based sensor strips are fabricated and calibrated for the sensing of sodium in the physiological range and shade cards were developed as a calorimetric guide for estimation of Na+ which makes them ideal point of care diagnostic platform. We demonstrate that the proposed CuC paper strip can be used for detecting Na+ concentration within the whole physiological range in both blood serum and urine.

Abstract A one-step analysis method was developed for four types of amino acids using a microfluidic paper-based analytical device fabricated from chromatography filtration paper and laminate films. Aminoacyl-tRNA synthetase was used to detect each amino acid. The obtained laminated paper-based analytical device (LPAD) contained four enzymatic reaction areas. Colorimetric detection was performed based on the molybdenum blue reaction. A model method for the simple, easy, and simultaneous detection of several amino acid concentrations was suggested, in contrast to the conventional methods such as HPLC or LC–MS. The method provided a selective quantification at the ranges of 3.6–100 μM for tryptophan, 10.1–100 μM for glycine, 5.9–100 μM for histidine and 5.6–100 μM for lysine with a detection limit of 1.1 μM, 3.3 μM, 1.9 μM and 1.8 μM, respectively. LPAD fabrication was considerably simple, and the subsequent detection process was easy and required a short period of time (within 15 min).

Abstract Bloodstream infection (BSI) is a major complication in patients with cancers due to therapy-induced neutropenia and underlying conditions, which increases hospitalization time and mortality rate. Targeted and timely antimicrobial management is crucial to save the patients’ lives and reduce the social and economic burdens. Blood culture is a routine clinical diagnostic method of BSI with a long turnaround time, and generally identifies monomicrobial BSI. Thus, polymicrobial BSI often goes undetected although it occurs more frequently in these patients and results in more severe outcomes compared to monomicrobial BSI. In this work, we apply glutaric anhydride, N-hydroxysuccinimide and N,N′-dicyclohexylcarbodiimide to fabricate a functional surface on cellulose filter paper. Targeting three pathogens (Escherichia coli, Saccharomyces cerevisiae, and human cytomegalovirus) commonly occurring in BSI in neutropenic patients, we demonstrate rapid and accurate triplex pathogen DNA detection using the functionalized paper. All three pathogen DNA was identified in 1–5 min with a detection limit of 0.1–0.5 ng/µL. The developed test tool has the potential to provide rapid polymicrobial BSI diagnosis in support of timely, accurate antimicrobial treatment, and could be integrated into an automatic sample-to-result portable equipment.

Abstract Milk adulteration is a common problem in developing countries, and it can lead to fatal diseases in humans. Despite several studies to identify different adulterants in milk samples, the effects of multiple adulterants remain unexplored. In this work, a three-dimensional (3D) paper-based microfluidic device is designed and fabricated to simultaneously detect multiple chemical adulterants in milk. This device comprises a top cover, a bottom cover, and a middle layer composed of transportation and a detection zone. By making cuts on the middle layer’s support, the device’s flow path is characterised by optimum and uniform velocity. For the first time, seven adulterants (urea, detergents, soap, starch, hydrogen peroxide, sodium-hydrogen-carbonate, and salt) are detected in the milk sample simultaneously with specificity evaluation and detailed color interference analysis. Only 1–2 mL of sample volume is required to detect 7 adulterants at one time. We have used only 10 $$\upmu$$ μ L of the reagent’s volume for the colorimetric reaction and found the results within a few seconds. Observation reveals that the limit of detection (LOD) of the adulterants lies in the range between $$0.05\%$$ 0.05 % (vol./vol.) to $$0.2\%$$ 0.2 % (vol./vol.) using the colorimetric detection technique. The unknown quantity of the added adulterants is measured using the calibration curves obtained from the experiments results. The repeatability and reproducibility of the process, sensitivity, and the linear range of detection of the calibration curves and the statistical study of the color intensity data are thoroughly analysed herein. In any resource-limited setting, this simple, portable, and user-friendly 3D microfluidic device is expected to be used for testing liquid foods before consumption.

Abstract Asymptomatic visceral leishmaniasis cases increase continuously, particularly among patients with HIV who are at risk to develop further symptoms of leishmaniasis. A simple, sensitive and reliable diagnosis is crucially needed due to risk populations mostly residing in rural communities with limited resources of laboratory equipment. In this study, a highly sensitive and selective determination of Leishmania among asymptomatic patients with Leishmania/HIV co-infection was achieved to simultaneously interpret and semi-quantify using colorimetric precipitates (gold-nanoparticle probe; AuNP-probe) and fluorescence (SYBR safe dye and distance-based paper device; dPAD) in one-step loop-mediated isothermal amplification (LAMP) assay. The sensitivities and specificities of 3 detection methods were equivalent and had reliable performances achieving as high as 95.5%. Detection limits were 102 parasites/mL (0.0147 ng/µL) which were 10 times more sensitive than other related studies. To empower leishmaniasis surveillance as well as prevention and control, this dPAD combined with SYBR safe and gold nanoparticle probe LAMP assay is reliably fast, simple, inexpensive and practical for field diagnostics to point-of-care settings in resource-limited areas which can be set up in all levels of healthcare facilities, especially in low to middle income countries.

Abstract In this study, the performance of a paper-based, screen-printed biofuel cell with mesoporous MgO-templated carbon (MgOC) electrodes was improved in two steps. First, a small amount of carboxymethyl cellulose (CMC) was added to the MgOC ink. Next, the cathode was modified with bilirubin prior to immobilizing the bilirubin oxidase (BOD). The CMC increased the accessibility of the mesopores of the MgOC, and subsequently, the performance of both the bioanode and biocathode. CMC also likely increased the stability of the electrodes. The pre-modification with bilirubin improved the orientation of the BOD, which facilitated direct electron transfer. With these two steps, an open circuit potential of 0.65 V, a maximal current density of 1.94 mA cm−2, and a maximal power density of 465 μW cm−2 was achieved with lactate oxidase as bioanode enzyme and lactate as fuel. This is one of the highest reported performances for a biofuel cell.

Abstract As members of a social species, we spend most of our time interacting with others. In interactions, we tend to mutually align our behavior and brain responses to communicate more effectively. In a semi-computerized version of the Rock-Paper-Scissors game, we investigated whether people show enhanced interpersonal neural synchronization when making explicit predictions about others’ actions. Across four experimental conditions, we measured the dynamic brain activity using the functional near-infrared spectroscopy (fNIRS) hyperscanning method. Results showed that interpersonal neural synchrony was enhanced when participants played the game together as they would do in real life in comparison to when they played the game on their own. We found no evidence of increased neural synchrony when participants made explicit predictions about others’ actions. Hence, neural synchrony may depend on mutual natural interaction rather than an explicit prediction strategy. This study is important, as it examines one of the presumed functions of neural synchronization namely facilitating predictions.

Abstract Social insects are highly diverse in their social structures, aside from the consistent presence of reproductive castes. Among social insects, the Australian paper wasp Ropalidia plebeiana constructs extremely dense colony aggregations consisting of hundreds of colonies within a few square meters; however, little is known about the aggregation structures. We genetically analyzed the colony and population structure of R. plebeiana, and concomitant variations in colony sex ratios. In spring, the foundress (candidate queen) group started their colonies on a single old comb from the previous season, subsequently dividing these old combs via relatedness-based comb-cutting. Female philopatry, a prerequisite condition of Local Resource Competition (LRC), was confirmed. The colony sex ratio of reproductive individuals (male and female offspring for the next generation) became slightly male-biased in larger colonies, as predicted under LRC. However, the number of foundresses was positively associated with the number of reproductive individuals, suggesting that Local Resource Enhancement (LRE) also operates. Although the population structure appears to meet the prerequisites of LRC, the sex ratio appears to be modulated by factors other than LRC. Rather, through LRE, the availability of female helpers at the founding stage is likely to mitigate the sex ratios predicted under LRC.

Abstract Many studies have been conducted on measuring avian influenza viruses and their hemagglutinin (HA) antigens via electrochemical principles; most of these studies have used gold electrodes on ceramic, glass, or silicon substrates, and/or labeling for signal enhancement. Herein, we present a paper-based immunosensor for label-free measurement of multiple avian influenza virus (H5N1, H7N9, and H9N2) antigens using flexible screen-printed carbon nanotube-polydimethylsiloxane electrodes. These flexible electrodes on a paper substrate can complement the physical weakness of the paper-based sensors when wetted, without affecting flexibility. The relative standard deviation of the peak currents was 1.88% when the electrodes were repeatedly bent and unfolded twenty times with deionized water provided each cycle, showing the stability of the electrodes. For the detection of HA antigens, approximately 10-μl samples (concentration: 100 pg/ml–100 ng/ml) were needed to form the antigen–antibody complexes during 20–30 min incubation, and the immune responses were measured via differential pulse voltammetry. The limits of detections were 55.7 pg/ml (0.95 pM) for H5N1 HA, 99.6 pg/ml (1.69 pM) for H7N9 HA, and 54.0 pg/ml (0.72 pM) for H9N2 HA antigens in phosphate buffered saline, and the sensors showed good selectivity and reproducibility. Such paper-based sensors are economical, flexible, robust, and easy-to-manufacture, with the ability to detect several avian influenza viruses.

Abstract The wettability of the paper surface is greatly affected by the wettability of the pulp fibers. We conducted this study in order to understand the relationship between the wettability of a single fiber of recycled pulp and the strength of recycled paper, as well as the inter-fiber bonding strength. The contact angle was determined from a series of photographs of the pulp fiber and the water silhouettes at the point of contact. The contact line and profile history were continuously photographed in every 1 s after the initial contact. The recycled softwood kraft pulp fibers were clearly much less hydrophilic than the original fibers, regardless of whether the fibers had been bleached or not. The contact angle of the original chemi-thermomechanical pulp fiber was much higher than that of the original softwood bleached kraft pulp fiber. Furthermore, increased number of recycling decreased the contact angle of the chemi-thermomechanical pulp fiber. The Page equation was used to evaluate the strength contributions of single fiber and fiber–fiber bonding to tensile strength of paper. As a result, an increase in weakness factor of fiber–fiber bonding strength was obtained for the recycled softwood kraft pulp handsheet. On the other hand, the weakness factor of the original chemi-thermomechanical pulp handsheet decreased with recycling. In addition, the weakness factor of fiber–fiber bonding strength and the contact angles of the provided softwood bleached kraft pulp fibers bore a proportional relationship to each other.

Abstract Non-Hermitian topology is a recent hot topic in condensed matters. In this paper, we propose a novel platform drawing interdisciplinary attention: rock–paper–scissors (RPS) cycles described by the evolutionary game theory. Specifically, we demonstrate the emergence of an exceptional point and a skin effect by analyzing topological properties of their payoff matrix. Furthermore, we discover striking dynamical properties in an RPS chain: the directive propagation of the population density in the bulk and the enhancement of the population density only around the right edge. Our results open new avenues of the non-Hermitian topology and the evolutionary game theory.

Abstract Zinc–air batteries proffer high energy density and cyclic stability at low costs but lack disadvantages like sluggish reactions at the cathode and the formation of by-products at the cathode. To resolve these issues, a new perovskite material, CaCu3Ti4O12 (CCTO), is proposed as an efficacious electrocatalyst for oxygen evolution/reduction reactions to develop zinc–air batteries (ZAB). Synthesis of this material adopted an effective oxalate route, which led to the purity in the electrocatalyst composition. The CCTO material is a proven potential candidate for energy applications because of its high dielectric permittivity (ε) and occupies an improved ORR-OER activity with better onset potential, current density, and stability. The Tafel value for CCTO was obtained out to be 80 mV dec−1. The CCTO perovskite was also evaluated for the zinc–air battery as an air electrode, corresponding to the high specific capacitance of 801 mAh g−1 with the greater cyclic efficiency and minimum variations in both charge/discharge processes. The highest power density (Pmax) measured was 127 mW cm−2. Also, the CCTO based paper battery shows an excellent performance achieving a specific capacity of 614 mAh g−1. The obtained results promise CCTO as a potential and cheap electrocatalyst for energy applications.

Abstract Polistes paper wasps are a widespread taxon inhabiting various climates. They build nests in the open without a protective outer layer, which makes them vulnerable to changing temperatures. To better understand the options they have to react to environmental variation and climate change, we here compare the thermoregulatory behavior of Polistes biglumis from cool Alpine climate with Polistes gallicus from warm Mediterranean climate. Behavioral plasticity helps both of them to withstand environmental variation. P. biglumis builds the nests oriented toward east-south-east to gain solar heat of the morning sun. This increases the brood temperature considerably above the ambience, which speeds up brood development. P. gallicus, by contrast, mostly avoids nesting sites with direct insolation, which protects their brood from heat stress on hot days. To keep the brood temperature below 40–42 °C on warm days, the adults of the two species show differential use of their common cooling behaviors. While P. biglumis prefers fanning of cool ambient air onto the nest heated by the sun and additionally cools with water drops, P. gallicus prefers cooling with water drops because fanning of warm ambient air onto a warm nest would not cool it, and restricts fanning to nests heated by the sun.

Abstract Infectious diseases are among the leading causes of mortality worldwide. A new coronavirus named severe acute respiratory syndrome corona virus 2 (SARS-CoV-2) was identified in Wuhan, China in 2019, and the World Health Organization (WHO) declared its outbreak, coronavirus disease 2019 (COVID-19), as a global pandemic in 2020. COVID-19 can spread quickly from person to person. One of the most challenging issues is to identify the infected individuals and prevent potential spread of SARS-CoV-2. Recently, anti-SARS-CoV-2 immunoglobulin M (IgM) and immunoglobulin G (IgG) antibody tests using immunochromatographic methods have been used as a complement to current detection methods and have provided information of the approximate course of COVID-19 infection. However, blood sampling causes pain and poses risks of infection at the needle puncture site. In this study, a novel patch sensor integrating porous microneedles and an immunochromatographic assay (PMNIA) was developed for the rapid detection of anti-SARS-CoV-2 IgM/IgG in dermal interstitial fluid (ISF), which is a rich source of protein biomarkers, such as antibodies. Biodegradable porous microneedles (MNs) made of polylactic acid were fabricated to extract ISF from human skin by capillary effect. The extracted ISF was vertically transported and flowed into the affixed immunoassay biosensor, where specific antibodies could be detected colorimetrically on-site. Anti-SARS-CoV-2 IgM/IgG antibodies were simultaneously detected within 3 min in vitro. Moreover, the limit of detection of anti-SARS-CoV-2 IgM and IgG concentrations was as low as 3 and 7 ng/mL, respectively. The developed device integrating porous MNs and immunochromatographic biosensors is expected to enable minimally invasive, simple, and rapid anti-SARS-CoV-2 IgM/IgG antibody testing. Furthermore, the compact size of the MN and biosensor-integrated device is advantageous for its widespread use. The proposed device has great potential for rapid screening of various infectious diseases in addition to COVID-19 as an effective complementary method with other diagnostic tests.

Abstract While traditional techniques have long allowed forensic investigators to positively identify fingermarks on documents of interest, understanding the chronological sequence of events that led to their deposition is still seen as a ‘holy grail’ for forensic examinations. By way of example, the question of whether a mark is above or below printed text is crucial. The work herein reveals that a novel application of a recently established fingermark development technique readily allows such differentiation. The process in question allies forensic gelatin lifters with RECOVER, a development system that hinges on the polymerisation of disulfur dinitride. While the latter was specifically developed in its current form for the retrieval of prints from metal surfaces exposed to extreme conditions or washing, its ability to target surface effects allows for visualisation of surface interactions on forensic gelatin lifts. Crucially, in doing so the order in which the lifted material was originally deposited is also revealed. This, therefore, permits clear elucidation of the order of deposition of printed text and fingermarks—and does so both rapidly and in a non-invasive way. This long sought-after capability has the potential to revolutionise forensic document examinations.

Abstract Three-dimensional visualization of cellular and subcellular-structures in histological-tissues is essential for understanding the complexities of biological-phenomena, especially with regards structural and spatial relationships and pathologlical-diagnosis. Recent advancements in tissue-clearing technology, such as Magnified Analysis of Proteome (MAP), have significantly improved our ability to study biological-structures in three-dimensional space; however, their wide applicability to a variety of tissues is limited by long incubation-times and a need for advanced imaging-systems that are not readily available in most-laboratories. Here, we present optimized MAP-based method for paper-thin samples, Paper-MAP, which allow for rapid clearing and subsequent imaging of three-dimensional sections derived from various tissues using conventional confocal-microscopy. Paper-MAP successfully clear tissues within 1-day, compared to the original-MAP, without significant differences in achieved optical-transparency. As a proof-of-concept, we investigated the vasculature and neuronal-networks of a variety of human and rodent tissues processed via Paper-MAP, in both healthy and diseased contexts, including Alzheimer’s disease and glioma.

Abstract One of the main objectives of microfluidic paper-based analytical devices is to present solutions particularly, for applications in low-resource settings. Therefore, screen-printing appears to be an attractive fabrication technique in the field, due to its overall simplicity, affordability, and high-scalability potential. Conversely, the minimum feature size attained using screen-printing is still rather low, especially compared to other fabrication methods, mainly attributed to the over-penetration of hydrophobic agents, underneath defined patterns on masks, into the fiber matrix of paper substrates. In this work, we propose the use of the over-penetration to our advantage, whereby an appropriate combination of hydrophobic agent temperature and substrate thickness, allows for the proper control of channel patterning, rendering considerably higher resolutions than prior arts. The implementation of Xuan paper and nail oil as novel substrate and hydrophobic agent, respectively, is proposed in this work. Under optimum conditions of temperature and substrate thickness, the resolution of the screen-printing method was pushed up to 97.83 ± 16.34 μm of channel width with acceptable repeatability. It was also found that a trade-off exists between achieving considerably high channel resolutions and maintaining high levels of repeatability of the process. Lastly, miniaturized microfluidic channels were successfully patterned on pH strips for colorimetric pH measurement, demonstrating its advantage on negligible sample-volume consumption in nano-liter range during chemical measurement and minimal interference on manipulation of precious samples, which for the first time, is realized on screen-printed microfluidic paper-based analytical devices.

Abstract This study introduces a novel geotechnical composite material comprising two types of fill material sourced from the paper industry—deinking paper sludge ash (DPSA) and deinking paper sludge (DPS). Five composites with different DPSA and DPS contents were investigated. Two composites were selected for further analyses. The technology and procedure for composite installation were implemented in field tests. The composites with 80% and 70% DPSA exhibited the elasticity required to withstand minor landslide slip deformations, in addition to achieving sufficiently high values of uniaxial compressive strength. The composites had a low maximum dry density value, which led to fewer settlements in the entire support structure. The enhanced shear characteristics can enable the construction of a thinner retaining wall. The delay between preparation and installation of the composites was further investigated. The field tests confirmed that the composites with 80% and 70% DPSA can be installed on the construction site 4 h and even 24 h after mixing. In 2018, a retaining wall structure with 70% DPSA and 30% DPS was successfully implemented near a railway line using conventional technology as followed-up research to the herein presented study. Results have been derived from work performed in the scope of the H2020 Paperchain project in which novel circular economy models centered on the valorization of the waste streams generated by the pulp and paper industry as secondary raw material for several resource-intensive sectors, including the construction sector, have been developed. Environmental benefits are savings in natural raw materials, reduction of landfill disposal as well as CO2 emission reduction.

Abstract The study was aimed to validate paper strip sensors for the detection of pesticide residues in milk, cereal-based food, and fruit juices in comparison with GC–MS/MS under field conditions. The detection limit of pesticide using rapid paper strip sensor for organophosphate, carbamate, organochlorine, fungicide, and herbicide group ranges from 1 to 10, 1–50, 250–500, 1–50, and 1 ppb, respectively in milk and milk product, cereal-based food and fruit juices. Among 125 samples of milk samples collected from the market 33 milk samples comprising 31 raw milk and 2 pasteurized milk found positive for pesticide using the strip-based sensor. In cereal based food and fruit juice samples, 6 cereal flours and 4 fruit juices were found positive for pesticide residues. The pesticide positive samples were further evaluated quantitatively using GC–MS/MS wherein 7 samples comprised of raw milk, pasteurized milk, rice flour, wheat flour, maize flour, apple juice, and pomegranate juice have shown the presence of chlorpyrifos, chlorpyrifos-methyl, α-endosulfan, β-endosulfan DDD and DDT at trace level as well as at above MRL level. It is envisaged that the developed paper strip sensor can be a potential tool in the rapid and cost-effective screening of a large number of food samples for pesticide residues.

Abstract Oily water contamination has been sighted as one of the most global environmental pollution. Herein, copper hydroxide nanorods layer was constructed onto cellulosic filter paper surface cured with polydopamine, Ag nanoparticles, and Cu NPs through immersion method. This work has been aimed to produce a superhydrophobic and superoleophilic cellulosic filter paper. The structure, crystalline, and morphological properties of these modified cellulosic filter paper were investigated. Scanning electron microscope images confirmed that the modified surface was rougher compared with the pristine surface. The contact angle measurement confirmed the hydrophobic nature of these modified surfaces with a water contact angle of 169.7°. The absorption capacity was 8.2 g/g for diesel oil and the separation efficiency was higher than 99%. It was noted that the flux in the case of low viscosity solvent as n-hexane was 9663.5 Lm−2 h−1, while for the viscous oil as diesel was 1452.7 Lm−2 h−1.

Abstract The electrochemical activity of catalysts strongly depends on the uniform distribution of monodisperse Pt nanoparticles without aggregates. Here, we propose a new hydrolysis-assisted smearing method for Pt loading on a free-standing paper-type electrode. Polyacrylonitrile (PAN)-based nanofiber paper was used as the electrode, and it acted as a Pt support. Hydrolysis of the electrode tripled the number of active nucleation sites for Pt adsorption on the PAN nanofibers, thereby significantly enhancing the wettability of the nanofibers. This facilitated the uniform distribution of Pt nanoparticles without aggregate formation up to 40 wt% (about 0.8 mg/cm2) with a particle size of about 3 nm. The catalytic current of the hydrolyzed Pt electrode in CH3OH/H2SO4 solution exceeded 213 mA/cm2 Pt mg, which was considerably greater than the current was 148 mA/cm2 Pt mg for an unhydrolyzed electrode.

Abstract Recycled paper and some hardwood paper often display poorer mechanical properties, which hinder its practical applications and need to be addressed. In this work, cellulose nanofibrils (CNFs) obtained by a combined process of enzymatic hydrolysis and grinding (EG-CNFs), grinding and microfluidization (GH-CNFs) or TEMPO-mediated oxidation and grinding (TE-CNFs) were characterized by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Moreover, CNFs were made into films on which some characterizations including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and UV–Vis transmittance spectroscopy were implemented. Results showed that CNF fibrillation was promoted as times of passes increased in microfluidization, and CNFs pretreated by enzyme possessed shorter length. Crystallinity of CNFs was related to CNF manufacturing methods, while CNF films’ transparency was correlated to CNF diameter distributions. Moreover, CNFs were applied with different dosages on recycled and hardwood paper. Lengths of CNFs, strength of CNF network, and pulp properties were critical factors affecting the mechanical strength of CNFs-enhanced paper. GH-CNFs showed better strengthened effect on tensile strength of paper than TE-CNFs and EG-CNFs. The best overall improvement was achieved at GH-CNF10 dosage of 5.0 wt% on hardwood paper. The increment of tensile index, burst index, and folding endurance were 108.32%, 104.65%, and 600%, respectively. This work aims to find out the relationship between production methods and morphologies of CNFs and how the morphological characteristics of CNFs affecting the mechanical performance of paper when they are added as strength additives.

Abstract Ovarian cancer has a poor cure rate and rates of relapse are high. Current recurrence detection is limited by non-specific methods such as blood testing and ultrasound. Based on reports that human epididymis four (HE4) / creatinine (CRE) ratios found in urine are elevated in ovarian cancers, we have developed a paper-based device that combines lateral flow technology and cell phone analysis to quantitatively measure HE4/CRE. Surrogate samples were used to test the performance over clinically expected HE4/CRE ratios. For HE4/CRE ratios of 2 to 47, the percent error was found to be 16.0% on average whether measured by a flatbed scanner or cell phone. There was not a significant difference between the results from the cell phone or scanner. Based on published studies, error in this method was less than the difference required to detect recurrence. This promising new tool, with further development, could be used at home or in low-resource settings to provide timely detection of ovarian cancer recurrence.

Abstract Cellulose fibers are a major industrial input, but due to their irregular shape and anisotropic material response, accurate material characterization is difficult. Single fiber tensile testing is the most popular way to estimate the material properties of individual fibers. However, such tests can only be performed along the axis of the fiber and are associated with problems of enforcing restraints. Alternative indirect approaches, such as micro-mechanical modeling, can help but yield results that are not fully decoupled from the model assumptions. Here, we compare these methods with nanoindentation as a method to extract elastic material constants of the individual fibers. We show that both the longitudinal and the transverse elastic modulus can be determined, additionally enabling the measurement of fiber properties in-situ inside a sheet of paper such that the entire industrial process history is captured. The obtained longitudinal modulus is comparable to traditional methods for larger indents but with a strongly increased scatter as the size of the indentation is decreased further.

Abstract Low energy surface coatings have found wide range of applications for generating hydrophobic and superhydrophobic surfaces. Most of the studies have been related to use of a single coating material over a single substrate or using a single technique. The degree of hydrophobicity is highly dependent on fabrication processes as well as materials being coated and as such warrants a high-level study using experimental optimization leading to the evaluation of the parametric behavior of coatings and their application techniques. Also, a single platform or system which can predict the required set of parameters for generating hydrophobic surface of required nature for given substrate is of requirement. This work applies the powerful machine learning algorithms (Levenberg Marquardt using Gauss Newton and Gradient methods) to evaluate the various processes affecting the anti-wetting behavior of coated printable paper substrates with the capability to predict the most optimized method of coating and materials that may lead to a desirable surface contact angle. The major application techniques used for this study pertain to dip coating, spray coating, spin coating and inkjet printing and silane and sol–gel base coating materials.

Abstract Achieving an efficient catalyst in the ATRP system with a simple design, preparation from available materials, and high recyclability is a significant challenging issue. To attain the goal, herein, we used chitosan (CS)-modified cellulose filter paper (FP) as a green support for the synthesis of dip catalyst. The preparation of this catalyst involved surface treatment of the FP strips by CS coating through a dipping method, which increased the affinity of the substrate for adsorbing copper ions in the next step. The Cu@CS-FP catalyst was prepared without the requirement of any ligands. The synthesized dip-catalyst, in the form of the strips, was employed for the first time in the ATRP reaction of methyl methacrylate to assay catalytic activity. Catalytic insertion/ removal (ON/OFF) experiments were carried out during the polymerization. A reasonable control over the molecular weight with high conversion (68%) and polydispersity index of 1.32 under mild reaction conditions were obtained. Significantly, because of the facile separation of the catalyst, the amount of copper that remained in the polymer was very low (2.7 ppm). Also, the recyclability of the catalyst was investigated for five runs. The conversion in the final run was 64% without a loss of catalyst efficiency.

Abstract Paper spray ionization (PSI) mass spectrometry (MS) is an emerging tool for ambient reaction monitoring via microdroplet reaction acceleration. PSI-MS was used to accelerate and monitor the time course of the reaction of dansyl chloride with aniline, in acetonitrile, to produce dansyl aniline. Three distinct PSI arrangements were explored in this study representing alternative approaches for sample loading and interaction; conventional single tip as well as two novel setups, a dual-tip and a co-axial arrangement were designed so as to limit any on-paper interaction between reagents. The effect on product abundance was investigated using these different paper configurations as it relates to the time course and distance of microdroplet travel. It was observed that product yield increases at a given distance and then decreases thereafter for all PSI configurations. The fluorescent property of the product (dansyl aniline) was used to visually inspect the reaction progress on the paper substrate during the spraying process. Amongst the variety of sample loading methods the novel dual-tip arrangement showed an increased product yield and microdroplet density, whilst avoiding any on-paper interaction between the reagents.

Abstract This study introduces an applicable colorimetric sensor array for the detection of pesticides in the vapor phase. The array consisted of six metal nanoparticles spotted on the piece of filter paper. 3D-origami pattern was used for the fabrication of a paper-based sensor to decrease the effect of the nanoparticles leaching after exposure to analytes. Exposure to pesticide aerosols caused changes in the color of the array due to the aggregation of nanoparticles. These changes provided selective responses to thion pesticides such as malathion, parathion, chlorpyrifos, and diazinon. The sensing assay could also differentiate between aliphatic and aromatic thions and discriminate amine-containing compounds from the other studied analytes. These finding results are clearly confirmed by both visual detection and multivariate statistical methods. The proposed sensor was successfully developed for the quantitative measurement of pesticide aerosols at a very low concentration. The limit of detection of this method determined for malathion, parathion, chlorpyrifos and diazinon were 58.0, 103.0, 81.0 and 117.0, respectively. Moreover, the array could be employed to simultaneously analyze four studied pesticides. The statistcal results confirmed that the method has high performance for concurrent detection of thions as a major air pollutant without the interference of other species.

Abstract Graphite pencil stroked electrodes for paper-based Microfluidic devices are gaining immense attention due to their electrochemical properties, cost efficiency, and ease-of-use. However, their widespread use has been hindered by the challenges associated with their manual fabrication such as non-uniformity in graphite deposition, applied pressure, etc. This work presents the design and development of an automated graphite pencil stroking device for graphite electrode fabrication with high efficiency through a compact, inexpensive and automatic process, with reduced fabrication time and human intervention leading to more uniformity. The motion platform of Graphtec plotter was used to create multiple strokes with the help of the proposed device. Such inexpensive graphite electrodes (less than the US $1) have been observed to be porous in nature, acting as diffusion agents. The automated graphite electrodes were used to study the performance of microfluidic paper fuel cells (MPFCs) with formic acid, oxygen, and sulphuric acid acting as fuel, oxidising agent and electrolyte respectively. From this configuration, the maximum current density and power density were measured to be 1,305.5 µA cm−2 and 135.5 µW cm−2, respectively at 0.3 V stable OCP at 100 strokes. Overall, the study enumerates the development of an automated pencil stroke device for fabricating graphite electrodes, which can potentially be harnessed in numerous miniaturized paper based applications.

Abstract Development of paper-based microfluidic devices that perform colorimetric measurements requires quantitative image analysis. Because the design geometries of paper-based microfluidic devices are not standardized, conventional methods for performing batch measurements of regularly spaced areas of signal intensity, such as those for well plates, cannot be used to quantify signal from most of these devices. To streamline the device development process, we have developed an open-source program called ColorScan that can automatically recognize and measure signal-containing zones from images of devices, regardless of output zone geometry or spatial arrangement. This program, which measures color intensity with the same accuracy as standard manual approaches, can rapidly process scanned device images, simultaneously measure identified output zones, and effectively manage measurement results to eliminate requirements for time-consuming and user-dependent image processing procedures.

Abstract Cyanide-based blood poisoning can seriously damage fire victims and cause death if not detected quickly. Previous conventional methods require laboratory equipment, which are expensive and increase the duration of the analysis. Here, a simple origami based microfluidic device was introduced for point of need detection of blood cyanide concentration in people involved in fire. The device is made of four layers of paper. Each layer was in the size of 1 × 1 cm folded on each other. In this work, the blood sample was acidified by trichloroacetic acid to separate cyanide from methaemoglobin in the form of HCN gas. The produced gas released into borate buffer to recover free cyanide ions which interacted with the Pt complex ([Pt(p-MeC6H4)2(phen)]) used as a receptor in this study. Optimized conditions were applied to have a suitable interaction causing the color of the receptor to change from yellow to colorless. The color changes were recorded by a smartphone, and the sensor response was calculated by the routine image analysis software. The assay was capable of determining cyanide ions at different concentrations in the range of 1.0 to 100.0 µmol L−1. The detection limit of these determination was equal to 0.4 µmol L−1. The assay responses were not affected by the interfering species. As a practical analysis, the proposed sensor was applied to determine cyanide ions in the blood sample of 20 studied fire survivors and 10 controls with high accuracy.

Abstract Analyzing electrolytes in urine, such as sodium, potassium, calcium, chloride, and nitrite, has significant diagnostic value in detecting various conditions, such as kidney disorder, urinary stone disease, urinary tract infection, and cystic fibrosis. Ideally, by regularly monitoring these ions with the convenience of dipsticks and portable tools, such as cellphones, informed decision making is possible to control the consumption of these ions. Here, we report a paper-based sensor for measuring the concentration of sodium, potassium, calcium, chloride, and nitrite in urine, accurately quantified using a smartphone-enabled platform. By testing the device with both Tris buffer and artificial urine containing a wide range of electrolyte concentrations, we demonstrate that the proposed device can be used for detecting potassium, calcium, chloride, and nitrite within the whole physiological range of concentrations, and for binary quantification of sodium concentration.

Abstract We present a prototype for conducting rapid, inexpensive and point-of-care-compatible nucleic acid amplification tests (NAATs) for tuberculosis (TB). The fluorescent isothermal paper-and-plastic NAAT (FLIPP-NAAT) uses paper-based loop mediated isothermal amplification (LAMP) for DNA detection. The cost of materials required to build a 12-test-zone device is $0.88 and the cost of reagents per reaction is $0.43. An inexpensive imaging platform enables filter-free fluorescence detection of amplified DNA using a cell-phone camera. FLIPP-NAAT can be operated by an untrained user and only requires a regular laboratory incubator as ancillary equipment. All reagents can be dry-stored in the device, facilitating storage and transportation without cold chains. The device design is modular and the assay demonstrated high specificity to Mycobacterium tuberculosis (Mtb), analytical sensitivity of the order of 10 copies of Mtb gDNA, and tolerance to complex samples. The clinical sensitivity and specificity of sputum-based FLIPP NAAT tests were 100% (zero false negatives) and 68.75% (five false positives), respectively (N = 30), using Xpert MTB/RIF assay as the reference standard. FLIPP-NAAT has the potential to provide affordable and accessible molecular diagnostics for TB in low- and middle-income countries, when used in conjunction with an appropriate sample preparation technique. Although demonstrated for the detection of TB, FLIPP-NAAT is a platform technology for amplification of any nucleic acid sequence.

Abstract Understanding mechanisms of biodiversity has been a central question in ecology. The coexistence of three species in rock-paper-scissors (RPS) systems are discussed by many authors; however, the relation between coexistence and network structure is rarely discussed. Here we present a metapopulation model for RPS game. The total population is assumed to consist of three subpopulations (nodes). Each individual migrates by random walk; the destination of migration is randomly determined. From reaction-migration equations, we obtain the population dynamics. It is found that the dynamic highly depends on network structures. When a network is homogeneous, the dynamics are neutrally stable: each node has a periodic solution, and the oscillations synchronize in all nodes. However, when a network is heterogeneous, the dynamics approach stable focus and all nodes reach equilibriums with different densities. Hence, the heterogeneity of the network promotes biodiversity.

Abstract Here we report the vertical paper analytical devices (vPADs) fabricated using the principles of quilling and kirigami. What differentiates the vPADs from conventional paper microfluidic devices is that the paper substrate used to fabricate the device is placed vertically to the device plane. The fabrication of vPADs with high precision is instrument-free, requiring no photolithography, printing or heating. Two- and three-dimensional vPADs are fabricated for multiplex colorimetric assays of four biochemical indicators and automated enzyme-linked immunosorbent assay of human myoglobin, respectively.

Abstract In this paper, a novel nitrogen-doped carbon paper (NCP) with both highly dense three-dimensional cellular structure and excellent bending flexibility is fabricated by pyrolyzing a melamine foam under compression. When serving as a free-standing anode for lithium-ion batteries, the NCP electrode delivers a reversible capacity up to 329.8 mA h g−1 after 200 cycles at 0.5 A g−1 (1.34 C) and 126.5 mA h g−1 after 500 cycles at 8.0 A g−1 (21.5 C). Such electrochemical performance is much higher than those of the counterparts prepared by pyrolysis without compression and can be mainly attributed to (a) the 3D highly dense interconnected carbon network with numerous junctions which can facilitate the efficient electron transfer and provide short transportation paths for lithium ions; and (b) the excellent mechanical flexibility and self-standing capability which exempt the use of binder, conductive additive and current collector. The NCP electrode implies a great promise of application in the high-performance Li-ion batteries for the flexible and wearable electronics.

Abstract During microbial electrosynthesis (MES) driven CO2 reduction, cathode plays a vital role by donating electrons to microbe. Here, we exploited the advantage of reduced graphene oxide (RGO) paper as novel cathode material to enhance electron transfer between the cathode and microbe, which in turn facilitated CO2 reduction. The acetate production rate of Sporomusa ovata-driven MES reactors was 168.5 ± 22.4 mmol m−2 d−1 with RGO paper cathodes poised at −690 mV versus standard hydrogen electrode. This rate was approximately 8 fold faster than for carbon paper electrodes of the same dimension. The current density with RGO paper cathodes of 2580 ± 540 mA m−2 was increased 7 fold compared to carbon paper cathodes. This also corresponded to a better cathodic current response on their cyclic voltammetric curves. The coulombic efficiency for the electrons conversion into acetate was 90.7 ± 9.3% with RGO paper cathodes and 83.8 ± 4.2% with carbon paper cathodes, respectively. Furthermore, more intensive cell attachment was observed on RGO paper electrodes than on carbon paper electrodes with confocal laser scanning microscopy and scanning electron microscopy. These results highlight the potential of RGO paper as a promising cathode for MES from CO2.

Abstract Constructing methods for cleaning stains on paper artworks that meet the requirements of preservation of cultural relics are still challenging. In response to this problem, a novel electrochemical cleaning method and the preparation of corresponding electrodes were proposed. For this purpose, the conductive graphene (rGO)/polyacryamide (PAM)/montmorillonite (MMT) composite hydrogel as cathode and PbO2-based material as anode were prepared and characterized. The electrochemical cleaning efficiencies of real sample and mimicking paper artifacts were evaluated, and the effects of the electrochemical cleaning on paper itself were detected. Based on the above experiments, the following results were obtained. The composite hydrogel with attractive mechanical properties is mainly based on the hydrogen bond interactions between PAM chains and MMT. The results of cleaning efficiency revealed that the black mildew stains together with the yellowish foxing stains were almost completely eliminated within 6 min at 8 mA/cm2, and various stains formed by tideline, foxing, organic dyes and drinks could be thoroughly removed at 4 mA/cm2 within 5 min. In addition, the proposed cleaning method has advantages in local selectivity, easy control of cleaning course, and reusability, which represents a potential utility of this approach.

Abstract Biodegradable highly nanostructured paper has received great interest in past years due to its excellent optical properties which facilitate its wide applications in green flexible electronics and devices. However, energy and/or time-consuming procedure during the process of fabricating most nanostructured transparent paper are presently the main obstacle to their scalable production. In this work, we demonstrated a novel nanostructured paper with dually high transparency (∼91%) and high haze (∼89%) that was directly fabricated from original paper with rapid ILs-polishing processes. The whole fabricating time only requires 10 min. Compared to the previously reported nanopaper made of the isolated cellulose nanofibers by pure mechanical and/or chemical approaches, this work presented herein is devoted to use green ILs to polish directly the micrometer-sized fibrous paper into the nanostructured paper. This new method brings a rapid fabrication of transparent nanostructured paper while also retaining dual intriguing properties both in optical transmittance and haze. This work is capable of fabricating next-generation flexible and highly transparent and haze paper by a high-speed roll-to-roll manufacturing process with a much lower cost.

Abstract The unusually broad physical and chemical property window of ionic liquids allows for a wide range of applications, which gives rise to the recent spring-up of ionic liquid-based functional materials. Via solvothermal copolymerization of a monomeric ionic liquid and divinylbenzene in the presence of a tissue paper in autoclave, we fabricated a flexible porous polymer/paper hybrid membrane. The surface areas of the hybrid membranes depend on the weight fraction of the copolymer impregnated inside the tissue paper. The as-prepared hybrid membrane shows controlled surface wettability in terms of ethanol wetting and ethanol removal by harsh drying condition. This unique property provides the hybrid membrane with switchable oil/water separation function, thus of practical values for real life application.

Abstract In this study, we investigated the antibacterial activity of silver-coated gold nanoparticles (Au-Ag NPs) immobilized on cellulose paper. Ag NPs are known to have strong antibacterial properties, while Au NPs are biocompatible and relatively simple to prepare. We made the Au-Ag NPs using a facile process called Ag enhancement, in which Au NPs serve as the nuclei for precipitation of a Ag coating, the thickness of which can be easily controlled by varying the ratio of the reactants. After synthesis, electron microscopy showed that the Au-Ag NPs displayed a core-shell structure, and that they could be successfully immobilized onto a cellulose membrane by heat treatment. We then investigated the antibacterial properties of this NP-coated cellulose paper against E. coli JM109. The inhibition rate, growth curve, and AATCC 100 activity test showed that cellulose paper coated with 15 nm Au-Ag NPs possessed excellent antibacterial activity against E. coli JM109. These results suggest that Au-Ag NPs immobilized on cellulose paper could be a valuable antibacterial technology for applications such as food packaging, clothing, wound dressings, and other personal care products.

Abstract Paper-based micro analytical devices offer significant advantages compared to the conventional microfluidic chips including cost-effectiveness, ease of fabrication, and ease of use while preserving critical features including strong capillary action and biological compatibility. In this work, we demonstrate an inexpensive, rapid method for high-throughput fabrication of paper-based microfluidics by patterning hydrophobic barriers using a desktop pen plotter integrated with a custom-made, low-cost paper feeder. We tested various types of commercial permanent markers and compared their water-resistant capabilities for creating hydrophobic barriers. Additionally, we studied the performance of markers with different types of paper, plotting speeds, and pattern dimensions. To verify the effectiveness of the presented fabrication method, colorimetric analysis was performed on the results of a glucose assay.

Abstract The most performing techniques enabling early diagnosis of infectious diseases rely on nucleic acid detection. Today, because of their high technicality and cost, nucleic acid amplification tests (NAAT) are of benefit only to a small fraction of developing countries population. By reducing costs, simplifying procedures and enabling multiplexing, paper microfluidics has the potential to considerably facilitate their accessibility. However, most of the studies performed in this area have not quit the lab. This letter brings NAAT on paper closer to the field, by using clinical samples and operating in a resource-limited setting. We first performed isothermal reverse transcription and Recombinase Polymerase Amplification (RT-RPA) of synthetic Ribonucleic Acid (RNA) of Ebola virus using paper microfluidics devices. We further applied this method in Guinea to detect the presence of Ebola virus in human sample RNA extracts, with minimal facilities (carry-on detection device and freeze-dried reagents on paper). RT-RPA results were available in few minutes and demonstrate a sensitivity of 90.0% compared to the gold-standard RT-PCR on a set of 43 patient samples. Furthermore, the realization of a nine-spot multilayered device achieving the parallel detection of three distinct RNA sequences opens a route toward the detection of multiple viral strains or pathogens.