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Chlorine dioxide is widely used for pulp bleaching because of its high delignification selectivity. However, efficient and clean chlorine dioxide bleaching is limited by the complexity of the lignin structure. Herein, the oxidation reactions of phenolic (vanillyl alcohol) and non-phenolic (veratryl alcohol) lignin model species were modulated using chlorine dioxide. The effects of chlorine dioxide concentration, reaction temperature, and reaction time on the consumption rate of the model species were also investigated. The optimal consumption rate for the phenolic species was obtained at a chlorine dioxide concentration of 30 mmol·L−1, a reaction temperature of 40 °C, and a reaction time of 10 min, resulting in the consumption of 96.3% of vanillyl alcohol. Its consumption remained essentially unchanged compared with that of traditional chlorine dioxide oxidation. However, the consumption rate of veratryl alcohol was significantly reduced from 78.0% to 17.3%. Additionally, the production of chlorobenzene via the chlorine dioxide oxidation of veratryl alcohol was inhibited. The structural changes in lignin before and after different treatments were analyzed. The overall structure of lignin remained stable during the optimization of the chlorine dioxide oxidation treatment. The signal intensities of several phenolic units were reduced. The effects of the selective oxidation of lignin by chlorine dioxide on the pulp properties were analyzed. Pulp viscosity significantly increased owing to the preferential oxidation of phenolic lignin by chlorine dioxide. The pollution load of bleached effluent was considerably reduced at similar pulp brightness levels. This study provides a new approach to chlorine dioxide bleaching. An efficient and clean bleaching process of the pulp was developed.

Herein is presented a novel and efficient portable paper-based sensing platform using paper-incorporated histidine stabilized gold nanoclusters (His-AuNCs), for the sensitive and selective detection of Fe ions from low-volume real water samples based on photoluminescence (PL) quenching. Highly photoluminescent colloidal His-AuNCs are obtained via a novel microwave-assisted method. The His-AuNCs-based sensor reveals a limit of detection (LOD) as low as 0.2 μM and a good selectivity towards Fe ions, in solution. Further, the fabricated portable sensing device based on paper impregnated with His-AuNCs proves to be suitable for the easy detection of hazardous Fe levels from real water samples, under UV light exposure, through evaluating the level of PL quenching on paper. Photographic images are thereafter captured with a smartphone camera and the average blue intensity ratio (I/I0) of the His-AuNCs-paper spots is plotted against [Fe2+] revealing a LOD of 3.2 μM. Moreover, selectivity and competitivity assays performed on paper-based sensor prove that the proposed platform presents high selectivity and accuracy for the detection of Fe ions from water samples. To validate the platform, sensing assays are performed on real water samples from local sources, spiked with 35 μM Fe ions (i.e., Fe2+). The obtained recoveries prove the high sensitivity and accuracy of the proposed His-AuNCs-paper-based sensor pointing towards its applicability as an easy-to-use, fast, quantitative and qualitative sensor suitable for on-site detection of toxic levels of Fe ions in low-volume real water samples.

In this work, we fabricated a novel origami paper-based analytical device (oPAD) assisted by the nanostructuring effect of in situ Pd decoration of Cu/Co-doped CeO2 (CuCo-CeO2-Pd) nanospheres, functionalized with their strongly enhanced electrocatalytic properties to realize an electrochemical and visual signal readout system in oPAD, for highly sensitive detection of amyloid-β (Aβ). The CuCo-CeO2-Pd nanospheres were introduced as an enhanced "signal transducer layer" on account of the electron transfer acceleration caused by catalyzing glucose to produce H2O2 for differential pulse voltammetry signal readout and further 3,3'5,5'-tetramethylbenzidine (TMB) oxidation for colorimetric analysis. Meanwhile, for achieving superior performance of the proposed oPAD, in situ growth of urchin-like gold nanoparticles (Au NPs) onto cellulose fibers was adopted to improve "the recognition layer" in favor of immobilizing antibodies for targeting Aβ through specific antigen-antibody interactions. Combined with the delicate design of oPAD, exhibiting actuation of the conversion procedure between hydrophobicity and hydrophilicity on paper tabs in the assay process, the oPAD successfully enabled sensitive diagnosis of Aβ in a linear range from 1.0 pM to 100 nM with a limit of detection of 0.05 pM (S/N = 3) for electrochemical detection, providing a reliable strategy for quantifying the Aβ protein in clinical applications. Ministry of Education (MOE) This work was financially supported by the Science and Technology Projects of University of Jinan (XKY2002), the Natural Science Foundation of Shandong Province (ZR2020MB057), the Singapore Ministry of Education (MOE AcRF Tier 1 RG176/16), the Taishan Scholars Program, the Case-by-Case Project for Top Outstanding Talents of Jinan, and the project of "20 Items of University" of Jinan (2018GXRC001).

Isothermal amplification strategies capable of rapid, inexpensive, and accurate nucleic acid detection provide new options for large-scale pathogen detection, disease diagnosis, and genotyping. Here we report a highly sensitive multicomponent XNA-based nucleic acid detection platform that combines analyte preamplification with X10-23-mediated catalysis to detect the viral pathogen responsible for COVID-19. The platform, termed RNA-Encoded Viral Nucleic Acid Analyte Reporter (REVEALR), functions with a detection limit of ≤20 aM (∼10 copies/μL) using conventional fluorescence and paper-based lateral flow readout modalities. With a total assay time of 1 h, REVEALR provides a convenient nucleic acid alternative to equivalent CRISPR-based approaches, which have become popular methods for SARS-CoV-2 detection. The assay shows no cross-reactivity for other in vitro transcribed respiratory viral RNAs and functions with perfect accuracy against COVID-19 patient-derived clinical samples.

Chronic wounds; Infection biomarker; Myeloperoxidase; Colorimetry Ferides i lesions; Biomarcadors d'infecció; Mieloperoxidasa; Colorimetria Heridas crónicas; Biomarcador de infección; Mieloperoxidasa; Colorimetría Current procedures for the assessment of chronic wound infection are time-consuming and require complex instruments and trained personnel. The incidence of chronic wounds worldwide, and the associated economic burden, urge for simple and cheap point-of-care testing (PoCT) devices for fast on-site diagnosis to enable appropriate early treatment. The enzyme myeloperoxidase (MPO), whose activity in infected wounds is about ten times higher than in non-infected wounds, appears to be a suitable biomarker for wound infection diagnosis. Herein, we develop a single-component foldable paper-based device for the detection of MPO in wound fluids. The analyte detection is achieved in two steps: (i) selective immunocapture of MPO, and (ii) reaction of a specific dye with the captured MPO, yielding a purple color with increasing intensity as a function of the MPO activity in infected wounds in the range of 20-85 U/mL. Ex vivo experiments with wound fluids validated the analytic efficiency of the paper-based device, and the results strongly correlate with a spectrophotometric assay.

The major obstacle to developing nanozymes which are considered as promising alternatives to natural enzymes is their moderate performance, including poor affinity for substrates, low catalytic activity, and severe pH-dependence. To address these issues, herein, we synthesize ultrathin layered double hydroxide (LDH) nanosheets with a thickness of 1.4 nm and an average lateral size of 23 nm using a fast-precipitation method. Through the rational design of their compositions, it is found that NiMn LDHs exhibit the optimum peroxidase mimicking performance with excellent substrate affinity, high catalytic activity (a limit of detection (LOD) of 0.04 μM H2O2) and robustness in a wide pH range (from 2.6 to 9.0), which is superior to that of natural horseradish peroxidase (HRP). The main active centers are identified as Mn sites because of their strong Lewis acidity and low redox potential. Furthermore, a series of disposable paper bioassays based on NiMn LDH nanozymes are designed and used for the highly sensitive detection of H2O2 and ascorbic acid (AA).

We report on a simple, cost-effective, instrument-free, and portable distance-based paper device coupled with NFs for the determination of glucose. The analysis reaction is based upon the oxidative etching reaction of silver nanoparticles (AgNPs) in the presence of H2O2 that is produced from glucose after a glucose oxidase (GOx) catalytic reaction leading to a morphological transformation of AgNPs. A color band length of AgNPs is coated on to a detection channel and then etched by H2O2, and these were changed from a purple color to colorless as a correlate of the glucose concentration. To improve the performance of the enzyme immobilization, NFs, which are biocompatible without compromising their structure and biological activity, were then placed onto the sample zone. The naked-eye detection limit was 0.1 mM for 40 min of analysis time. The recoveries of glucose spiked in the artificial urine samples and control urine samples were then verified by our device and were in the acceptable range of 96 - 100%.

Directed evolution has become an important method to unleash the latent potential of enzymes to make them uniquely suited for human purposes. However, the need for a large reagent volume and sophisticated instrumentation hampers its broad implementation. In an attempt to address this problem, here we report a paper-based high-throughput screening approach that should find broad application in generating desired enzymes. As an example case, the dehalogenation reaction of the halohydrin dehalogenase was adopted for assay development. In addition to visual detection, quantitative measurements were performed by measuring the color intensity of an image that was photographed by a smartphone and processed using ImageJ free software. The proposed method was first validated using a gold standard method and then applied to mutagenesis library screening with reduced consumption of reagents (i.e., ≤ 10 μl per assay) and a shorter assay time. We identified two active mutants (P135A and G137A) with improved activities toward four tested substrates. The assay not only consumes less reagents but also eliminates the need for expensive instrumentation. The proposed method demonstrates the potential of paper-based whole-cell screening coupled with digital image colorimetry as a promising approach for the discovery of industrially important enzymes.Key Points• A frugal method was developed for directed enzyme evolution.• Mutagenesis libraries were successfully screened on a paper platform.• Smartphone imaging was efficiently used to measure enzyme activities.

Protein biomarkers often exist as degradation fragments in biological samples, and affinity agents derived using a purified protein may not recognize them, limiting their value for clinical diagnosis. Herein, we present a method to overcome this issue, by selecting aptamers against a degraded form of the toxin B protein, which is a marker for diagnosing toxigenic Clostridium difficile infections. This approach has led to isolation of a DNA aptamer that recognizes degraded toxin B, fresh toxin B, and toxin B spiked into human stool samples. DNA aptamers selected using intact recombinant toxin B failed to recognize degraded toxin B, which is the form present in stored stool samples. Using this new aptamer, we produced a simple paper-based analytical device for colorimetric detection of toxin B in stool samples, or in the NAP1 strain of Clostridium difficile. The combined aptamer-selection and paper-sensing strategy can expand the practical utility of DNA aptamers in clinical diagnosis.

Cobalt(ii) phthalocyanine (CoPc) was suspended in aqueous medium and the colloidal system was used as catalyst for the electrochemical determination of hydrogen peroxide on paper-based electrodes modified with carbon nanomaterials. H2O2 was oxidised at 0.275 V vs. Ag pseudoreference electrode. This system was adapted to develop a glucose sensor with glucose oxidase immobilized on the cellulose electrode. CoPc suspended nanoparticles acted as nanoenzyme mimicking peroxidase activity and were combined with different carbon nanomaterials to form hybrids with optimised catalytic performance. GO-CoPc paper-based electrodes yielded the best results with a linear range of ∼12 μM to 49 mM for H2O2 and 0.1 mM to 1 mM for glucose. Glucose was determined in physiological serum and juice samples with recoveries of 93.3 and 94.2% respectively. CoPc could replace HRP for the catalytic sensing of H2O2, without the need to be dissolved. This material can be used in situ in a simple protocol with other nanomaterials for electrode modification. The sensor described has the advantage of easy preparation, using the catalyst in colloidal form, long term stability, and versatility to be adapted to other low cost and disposable enzymatic systems.

A bio-inspired cellulose paper–poly(amidoxime) composite hydrogel is explored via UV-polymerization. This hydrogel has a highly efficient uranium capture capacity of up to 6.21 mg g−1 for WU/Wdry gel and 12.9 mg g−1 for WU/Wpoly(amidoxime) in seawater for 6 weeks, due to its enhanced hydrophilicity, good hydraulic/ionic conductivity and broad-spectrum antibacterial performance.

The first discrete bimetallic europium(iii)/copper(ii) complex for the fast, sensitive and selective luminescent detection of both aqueous and gaseous hydrogen sulfide has been developed. The chemosensor displayed an impressive response time of 30 seconds and a low theoretical limit of detection (100 ppb) for gaseous hydrogen sulfide.

Accurate quantification of disease-signature microRNAs (miRNAs) in biomedical samples is in high demand for clinical diagnosis but still challenging because of the low abundance of miRNAs and complicating interferences in the milieus. Here, we report a multi-amplification strategy based on paper-spray mass spectrometry (PS MS) for the analysis of miRNAs in blood. A toehold-mediated DNA-strand-displacement reaction (TSD) is employed to amplify the signal chain and to ensure the specificity. The signal chain is then cleaved by UV light to release signal molecules for detection. Moreover, the paper spray method can efficiently filter out interfering substances in the blood and further enhance the sensitivity of detection. This concept is successfully demonstrated in the prototypical detection of the cancer biomarker miRNA-141 in blood and serum. The proposed TSD-PS MS approach provides an efficient method for the sensitive detection of oligonucleotides at low concentration in complicated milieus.

Detection and characterization of DNA damage plays a critical role in genotoxicity testing, drug screening, and environmental health. We developed a fully integrated origami paper-based analytical device (oPAD) for measuring DNA damage. This simple device allows on-paper cell lysis, DNA extraction, terminal deoxynucleotidyl transferase dUTP nick end labeling (TUNEL) reaction and signal readout with simple operation steps, enabling rapid (within 30 min) and high throughput assessment of multiple DNA damages induced by exogenous chemical agents.

Xylanases can boost pulp bleachability in Elemental Chlorine Free (ECF) processes, but their industrial implementation for producing bleached kraft pulps is not straightforward. It requires enzymes to be active and stable at the extreme conditions of alkalinity and high temperature typical of this industrial process; most commercial enzymes are unable to withstand these conditions. In this work, a novel highly thermo and alkaline-tolerant xylanase from Pseudothermotoga thermarum was overproduced in E. coli and tested as a bleaching booster of hardwood kraft pulps to save chlorine dioxide (ClO2) during ECF bleaching. The extremozyme-stage (EXZ) was carried out at 90 °C and pH 10.5 and optimised at lab scale on an industrial oxygen-delignified eucalyptus pulp, enabling us to save 15% ClO2 to reach the mill brightness, and with no detrimental effect on paper properties. Then, the EXZ-assisted bleaching sequence was validated at pilot scale under industrial conditions, achieving 25% ClO2 savings and reducing the generation of organochlorinated compounds (AOX) by 18%, while maintaining pulp quality and papermaking properties. Technology reproducibility was confirmed with another industrial kraft pulp from a mix of hardwoods. The new enzymatic technology constitutes a realistic step towards environmentally friendly production of kraft pulps through industrial integration of biotechnology., This work was supported by WoodZymes project funded by the Bio-based Industries Joint Undertaking (BBI JU) under GA 792070. The BBI JU received support from the EU’s H2020 research and innovation programme and the Bio Based Industries Consortium.

Negative ion mode paper spray mass spectrometry (PS-MS) suffers from intense background noise and unstable MS signal. For the first time, we reported fluorinated boron nitride nanosheet (h-FBN) assisted negative ion PS-MS for the detection of a series of molecules. We demonstrated that the introduction of h-FBN can greatly improve the detection sensitivity and signal stability in the negative ion mode.

The development of low cost, portable, and disposable biosensors for equipment-free and naked-eye biosensing is in eager demand for their widespread application in biomedical field, but it is still a challenge. Herein, we propose a novel paper analytical device (PAD) for truly equipment-free and naked-eye biosensing using dopamine as the chromogenic agent based on target-initiated catalyzed oxidation reaction. The dopamine-functionalized PAD (DPAD) possesses a significant three-dimensional net structure, excellent hydrophilicity, and unique response toward G-quadruplex DNAs against other DNAs, benefiting the bio/chemo reaction occurrence to assay target biomolecules. In light of the exceptional properties, the fabricated DPAD was applied in the analysis of Dam MTase through target-triggered exponential isothermal amplification. The recognition and methylation of H1 by Dam MTase contribute to formation of abundant hemin/G-quadruplexes, which catalyze oxidation of dopamine into dopachrome and reduce the dopamine amount on the DPAD surface. In comparison with the case in which Dam MTase is absent, an evident deep pink signal originating from dopachrome is observed directly by the naked eye and relied on Dam MTase concentrations. Therefore, truly equipment-free and naked-eye detection of Dam MTase is achieved with a detection limit of 1.46 U/mL. The fabricated DPAD not only achieves Dam MTase-visualized detection but also permits the accurate determination of other analytes by varying recognizable DNA's sequences, thus offering a universal biosensor and depicting significant potential for widespread applications in biomedical field.

Recently, resistance random access memories (RRAMs) have been studied extensively, because the demand for information storage is increasing. However, it remains challenging to obtain a flexible device because the active materials involved need to be nontoxic, nonpolluting, distortion-tolerable, and biodegradable as well adhesive to diverse flexible substrates. In this paper, tannic acid (TA) and an iron ion (FeIII ) coordination complex were employed as the active layer in a sandwich-like (Al/active layer/substrate) device to achieve memory performance. A nontoxic, biocompatible TA-FeIII coordination complex was synthesized by a one-step self-assembly solution method. The retention time of the TA-FeIII memory performance was up to 15 000 s, the yield up to 53 %. Furthermore, the TA-FeIII coordination complex can form a high-quality film and shows stable ternary memory behavior on various flexible substrates, such as polyethylene terephthalate (PET), polyimide (PI), printer paper, and leaf. The device can be degraded by immersing it in vinegar solution. Our work will broaden the application of organic coordination complexes in flexible memory devices with diverse substrates.

Efficient and reliable methods for the generation of bioactive papers are of growing interest in relation to point-of-care testing devices that do not require extensive analytical equipment. Herein, we report the immobilization of functional proteins on paper fibers using a modular chemoenzymatic approach. The synthetic strategy relies on a combination of highly efficient spatially controllable photo-triggered cycloaddition followed by site-specific sortase A-catalyzed transamidation. This site-directed and regiospecific method has allowed unidirectional and covalent immobilization of several proteins displaying different functional properties, with ramifications for application in paper-based diagnostics.

An anthracene carboxyimide derivative was synthesized as a colorimetric and fluorogenic sensor to determine NO2- with a rapid response (

A green and facile method is presented for in situ synthesis of a novel photoluminescence-quenching nanopaper with a highly-efficient quenching ability, rapid reaction time and long-term storage. The as-prepared nanopaper is further used to construct an aptasensor platform with high performance, rapidness and robustness.

Novel high-performance biosensing devices, based on a microporous cellulose matrix, have been of great interest due to their high sensitivity, low cost, and simple operation. Herein, we report on the design and testing of portable paper-based immunostrips (IMS) for in-field blood typing in emergencies requiring blood transfusion. Cellulose fibrils of a paper membrane were functionalized with antibodies via supramolecular interactions. The formation of hydrogen bonds between IgM pentamer and cellulose fibers was corroborated using quantum mechanical calculations with a model cellulose chain and a representative amino acid sequence. In the proposed immunostrips, paper with a pore size of 3 µm dia. was used to enable functionalization of its channels with antibody molecules while blocking the red blood cells (RBC) from channel entering. Under the optimized test conditions, all blood types of AB0 and Rh system could be determined by naked eye examination, requiring only a small blood sample (3.5 µL). The durability of IgM immunostrips against storing has been tested. A new method of statistical evaluation of digitized blood agglutination images, compatible with a clinical five-level system, has been proposed. Critical parameters of the agglutination process have been established to enable future development of automatic blood typing with machine vision and digital data processing.

A two-dimensional (2D) Co-MOF nanosheet-based nanozyme was developed for colorimetric detection of disease-related biomolecules. The prepared 2D Co-MOFs exhibited ultrahigh peroxidase catalytic activity. 2D Co-MOFs can catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to the blue product oxTMB, accompanying an obvious change of absorption value at 652 nm. However, alkaline phosphatase can catalyze the hydrolysis of L-ascorbic acid-2-phosphate to produce ascorbic acid which can reduce the oxTMB to TMB, resulting in an obvious color fading. Therefore, by recording the change of absorption value at 652 nm, the 2D Co-MOF nanosheets were used to detect ascorbic acid (AA) and alkaline phosphatase (ALP). The limit of detection for AA and ALP was 0.47 μM and 0.33 U L−1, respectively. The limit of quantification for AA and ALP was 1.56 μM and 1.1 U L−1, respectively. The developed nanozyme was successfully used to determine alkaline phosphatase in clinical human serum samples and the results were consistent with those provided by the hospital. Furthermore, by integrating 2D Co-MOF nanosheets with image recognition and data processing function fixed on a smartphone, a portable test of ascorbic acid was reached.

A novel miniaturized and sustainable platform exploiting two merged paper-based substrates has been applied for the programmable pre-concentration of analytes of interest and electrochemical detection of mercury traces in drinking water using printable sensor strips. This strategy represents a novel versatile possibility in merging humble materials maximizing their impacts on analytical and remediation challenges.

Electrochemical aptamer-based (E-AB) sensors offer a powerful and general means for analyte detection in complex samples for various applications. Paper-based E-AB sensors could enable portable, low-cost, and rapid detection of a broad range of targets, but it has proven challenging to fabricate suitable three-electrode systems on paper. Here, we demonstrate a simple, economic, and environmentally-friendly strategy for fabricating aptamer-modified paper electrochemical devices (PEDs) via ambient vacuum filtration. The electrode material, shape, size, and thickness of the three-electrode PED system can be fully customized. We developed aptamer-modified PEDs that enable sensitive and specific detection of small molecules in minimally processed biosamples. The sensitivity and stability of the PEDs is comparable to E-AB sensors based on commercial gold electrodes. We believe our fabrication strategy can lead to the development of high performance PEDs that enable on-site detection of a variety of analytes, simplifying the development of portable sensors for real-world applications.

Hybrid nanomaterials fabricated by the heterogeneous integration of 1D (carbon nanotubes) and 2D (graphene oxide) nanomaterials showed synergy in electrical and mechanical properties. Here, we reported the infiltration of carboxylic functionalized single-walled carbon nanotubes (C-SWNT) into free-standing graphene oxide (GO) paper for better electrical and mechanical properties than native GO. The stacking arrangement of GO sheets and its alteration in the presence of C-SWNT were comprehensively explored through scanning electron microscopy, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction. The C-SWNTs bridges between different GO sheets produce a pathway for the flow of electrical charges and provide a tougher hybrid system. The nanoscopic surface potential map reveals a higher work function of the individual functionalised SWNTs than surrounded GO sheets showing efficient charge exchange. We observed the enhanced conductivity up to 50 times and capacitance up to 3.5 times of the hybrid structure than the GO-paper. The laminate of polystyrene composites provided higher elastic modulus and mechanical strength when hybrid paper is used, thus paving the way for the exploitation of hybrid filler formulation in designing polymer composites.

A new colorimetric aptasensor equipped with a novel composite of graphitic carbon nitride (g-C

In this work, a new chemiluminescence (CL) system of Co-Fe prussian blue analogs nanocubes (Co-Fe PBA NCs) that can catalyze luminol to produce strong CL in the absence of H2O2 was established. Co-Fe PBA NCs have the property of oxidase-like activity, and it can catalyze the generation of active oxygen radicals in a dissolved oxygen system. Since caffeic acid (CA) can remove reactive oxygen species in the system, a sensitive detection method for CA on a paper-based chip was developed. Under the optimal conditions, this method showed a good linear response to CA in the range of 10 - 800 ng mL-1 with a limit of 3 ng mL-1. The proposed method had been used for the determination of CA in tea samples. The results may open a new avenue for the catalytic property on luminol CL system without extra oxidants.

A novel fluorescence strategy based on the outstanding catalytic capability of CuS nanoparticles (CuSNPs) has been developed for highly sensitive and specific determination of o,o-dimethyl-o-2,2-dichlorovinyl phosphate (DDVP) under enzyme-free and hydrogen peroxide (H2O2)-free conditions. In the presence of DDVP, CuSNPs can catalyze non-fluorescence substratum of Amplex red (AR) into resorufin, which exhibits fluorescence emission at 584 nm under excitation at 540 nm. The sensing system exhibits outstanding specificity and only responds to DDVP and no other organophosphorus pesticides (OPs). A wide linear range is obtained from 0.0001 to 0.1 μg/mL, and the limit of detection (LOD) is 0.1 ng/mL. Furthermore, paper-based test strips have been constructed for visual detection of DDVP under ultraviolet light irradiation. By integrating a smartphone installed with Color Picker APP, point-of-care detection with quantitative determination is realized, demonstrating substantial potential applications of the as-developed assay for in situ detection.

In this study, hexagonal boron nitride nanosheets enriched with hydroxyl groups (h-BN-OH) were successfully grafted on the surface of cellulose fibers after the simple and effective exfoliation and oxidation of bulk h-BN. OH groups of h-BN-OH and the ones presented on the surface of cellulose fibers interacted via hydrogen bonding. Both spectroscopic (FT-IR, XRD) and microscopic (TEM, SEM, and atomic force microscopy (AFM)) methods results proved the successful functionalization of the cellulose fibers with the nanomaterial. Modified cellulose fibers were used to prepare paper sheets samples with different concentrations of the nanomaterial (1 wt %, 2 wt %, and 3 wt %). All the samples were tested for the antibacterial properties via the colony forming unit method and exhibited good performance against both Gram-negative (E. coli) and Gram-positive (S. epidermidis) model bacteria. Additionally, the influence of the volume of working bacterial suspension on the antibacterial efficiency of the obtained materials was examined. The results showed significantly better antibacterial performance when the volume of bacterial suspension was reduced. Mechanical properties of the paper samples with and without nanofiller were also characterized. Tensile strength, tearing strength, and bursting strength of the paper samples containing only 2 wt % of the nanofiller were improved by 60%, 61%, and 118% in comparison to the control paper samples, respectively. Furthermore, the nanofiller improved the thermal properties of the composite paper&mdash, the heat release rate decreased by up to 11.6%. Therefore, the composite paper can be further explored in a wide range of antibacterial materials, such as packaging or paper coatings

A paper-based electrochemiluminescence (ECL) biosensor characterized by the signal amplification of reticular DNA-functionalized PtCu nanoframes (DNA-PtCuTNFs) and analyte-triggered DNA walker was developed for sensitive streptavidin assay. Silver microflower functionalized paper-based sensing platform was prepared to fix the hairpin strand (S1). With addition of the streptavidin, plenty of DNA walkers consisting of the walking strands (S2) labeled with biotin and streptavidin were established, which protected S2 from digestion via the terminal protection mechanism. The sequential introduction of the DNA walker and capture probe initiated the hairpin structure opening of S1 and strand displacement reaction (SDR) happening, causing the S2 release. Subsequently, S1 hybridized with S3. The free S2 further hybridized with adjacent S1 to trigger the next cycle. After multiple cycles, the DNA-PtCuTNFs, the fire-new signal enhancer, with remarkable peroxidase activity, were successfully attached onto the paper electrode via metal-catalyst-free click chemistry. Based on the SDR of the DNA walker and the catalysis of DNA-PtCuTNFs, a significantly boosted ECL signal of luminol was obtained. Under the optimal conditions, the developed sensor for streptavidin assay exhibited a low detection limit of 33.4 fM with a linear range from 0.1 pM to 0.1 μM. Graphical abstract.

β-cyclodextrin-functionalized porous Pd@Au nanostructures (β-CD-Pd@Au) with intrinsic and enhanced peroxidase-like activity were successfully synthesized by a two-step method. The synthesized β-CD-Pd@Au can efficiently catalyze the oxidation of various substrates, such as 3,3′,5,5′-tetramethylbenzidine (TMB), mixture of 4-amino antipyrine (4-AAP) and 3,5-dichloro-2-hydroxy acid sodium (DHBS) (4-AAP/DHBS), and mixture of 4-AAP and N-Ethyl-N-(3-sulfopropyl)-3-methyl-aniline sodium salt (TOPS) (4-AAP/TOPS), by H2O2 to generate visual blue, purple, and pink color, respectively. The UV-vis absorbance peak of the threeβ-CD-Pd@Au catalyzed the chromogenic reaction system located at 650 nm, 510 nm, and 550 nm, respectively. The β-CD-Pd@Au-catalyzed TMB-H2O2 chromogenic reaction exhibited higher absorbance intensity, catalytic efficiency, and color stability in comparison to 4-AAP/DHBS-H2O2 and 4-AAP/TOPS-H2O2 chromogenic reactions. The catalytic activity of β-CD-Pd@Au was enhanced about 4-fold compared to that of Pd@Au in terms of Kcat for H2O2. Using TMB as chromogenic substrate, a colorimetric assay was fabricated for the determination of H2O2 with a detection limit of 2.78 μM (absorbance at 650 nm). The colorimetric determination of glucose with a detection limit of 9.28 μM was further achieved by coupling with glucose oxidase enzymatic reaction, indicating the versatility of the β-CD-Pd@Au-based detection strategy. A paper-based detection method coupled with smartphone for fast visual and instrument-free detection of glucose was further developed. Finally, the developed colorimetric assay and paper-based detection method were successfully applied to the determination of glucose in human serum sample.

This work reports on fully integrated “sample‐in‐signal‐out” microfluidic paper‐based analytical devices (μPADs) relying on bioluminescence resonance energy transfer (BRET) switches for analyte recognition and colorimetric signal generation. The devices use BRET‐based antibody sensing proteins integrated into vertically assembled layers of functionalized paper, and their design enables sample volume‐independent and fully reagent‐free operation, including on‐device blood plasma separation. User operation is limited to the application of a single drop (20–30 μL) of sample (serum, whole blood) and the acquisition of a photograph 20 min after sample introduction, with no requirement for precise pipetting, liquid handling, or analytical equipment except for a camera. Simultaneous detection of three different antibodies (anti‐HIV1, anti‐HA, and anti‐DEN1) in whole blood was achieved. Given its simplicity, this type of device is ideally suited for user‐friendly point‐of‐care testing in low‐resource environments.

In this work, an eco-friendly solution for the remediation of wastewater generated in the lignin recovery process from eco-industrial paper mill has been proposed in their way towards a more circular economy strategy. Thus, the application of the electro-Fenton process for the degradation of the non-recovered lignin and other organic compounds form a scarcely studied acid black liquor waste (ABLW) was successfully performed. This treatment was able to operate in a range of COD loads (0.5–19.5 mg O2·L–1) showing high degradation values of the ABLW determined by the abatement of color, total phenolic content and COD. Then, the optimization of the working conditions for the design of a sustainable treatment system with optimum efficiency was carried out using a response surface methodology. The experiment carried out in the calculated optimal conditions for the electro-Fenton degradation process (current intensity 132.5 mA, catalyst dosage of 0.10 mM, and temperature 40 °C) showed a COD removal of 74.82% and current efficiency 77.79%, close to the theoretical value predicted by the model 73.12% and 77.06%, respectively. In addition, the identification of the final products permitted to confirm the mineralization efficiency.

We developed a paper-based analytical device based on the electropolymerization of poly (3,4-ethylenedioxythipohene) (PEDOT) and graphene oxide (GO) composites on the ITO substrate for the detection of uric acid (UA) in authentic human saliva. Scanning electron microscopy, UV-vis spectrum and X-ray diffraction confirmed the formation of porous PEDOT combined with GO film during the electropolymerization process. The nanocomposite based sensor showed an enhanced electrocatalytic activity toward UA with high sensitivity and stability. We demonstrate that UA can be directly detected in undiluted saliva using the paper-based electroanalytical device with no interference from ascorbic acid and dopamine that are normally present in biological fluids. The results indicated that the developed device is promising for non-invasive monitoring of salivary UA in human body.

Micrometer-sized functional nucleic acid (FNA) superstructures (denoted as 3D DNA) were examined as a unique class of biorecognition elements to produce highly functional bioactive paper surfaces. 3D DNA containing repeating sequences of either a DNA aptamer or DNAzyme was created from long-chain products of rolling circle amplification followed by salt aging. The resulting 3D DNA retained its original spherical shape upon inkjet printing and adhered strongly to the paper surface via physisorption. 3D DNA paper sensors showed resistance to degradation by nucleases, suppressed nonspecific protein adsorption, and provided a much higher surface density of functional DNA relative to monomeric FNAs, making such species ideally suited for development of paper-based biosensors.

A potentially universal approach is presented for enzyme attachment to cellulose that significantly enhances enzyme stability while retaining high activity, and involves no chemical functionalization of cellulose. Bovine serum albumin (BSA) was interlocked in cellulose to form a protein-friendly surface (named BSA-Paper), while also providing COOH and NH2 groups for subsequent attachment of enzymes. The desired enzyme is then mixed with additional BSA and interlocked on BSA-Paper. The second BSA layer dilutes and crosslinks the enzyme for improved stability. Laccase was tested as a model enzyme for interlocking on BSA-Paper, and was found to retain over 100 % activity and was 240 times more stable at 25 °C (half life=180 d) than laccase. This new approach was also tested with a few other enzymes with encouraging results, thus providing a potentially universal method for stabilization of enzymes on cellulose with retention of high activities.

The selectivity of the substitution reaction of phosphoryl chloride with organometallic reagents was investigated using NMR spectroscopy. This led to the discovery that the selectivity of the substitution reaction can be tuned by choosing a proper organometallic reagent. A phosphinate could be obtained by using a Grignard reagent whereas an organozinc reagent provided a phosphonate. Based on these results, one-pot synthetic methods for the preparation of phosphinates and phosphonates using commercially available starting materials were developed. Both methods allow the synthesis of a broad range of either phosphinate or phosphonate derivatives in a straightforward and general procedure. Moreover, using these one-pot procedures, mixed systems substituted with different alkyl/aryl groups can be prepared. ispartof: Synthesis (Germany) vol:50 issue:10 pages:2019-2026 status: published

Gold nanoparticles (AuNPs) were directly synthesized and anchored on lignocellulose fiber without an external immobilizing agent via a facile green approach using unbleached kraft (UBK) softwood pulp. The obtained AuNPs were confirmed by UV–vis diffuse reflectance spectroscopy, field-emission scanning electron microscopy, energy dispersive spectroscopy, X-ray diffraction, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The antioxidant behavior of the as-prepared AuNP-UBK fiber nanocomposite was evaluated by free radical scavenging of 2,2-diphenyl-1-picrylhydrazyl hydrate (DPPH). The nanocomposite fiber exhibited greatly enhanced radical scavenging activity compared to that of the pure fiber. As a consequence, AuNP-UBK nanocomposite paper showed exceptional antioxidant performance with a radical scavenging rate of over 98%, which is attributed to the synergistic effects of adsorption by the fiber–fiber network and subsequent catalytic activity of the AuNPs. This research indicated that AuNP-UBK fiber nanocomposites could be a new candidate for antioxidant active packaging for use in food preservation.

We report a general anion sensing platform based on a portable and cost-effective ion-selective optode and a smartphone detector equipped with a color analysis app. In contrast to traditional anion-selective optodes using a hydrophobic polymer and/or plasticizer to dissolve hydrophobic sensing elements, the new optode relies on hydrophilic cellulose paper. The anion ionophore and a lipophilic pH indicator are inkjet-printed and adsorbed on paper and form a “dry” hydrophobic sensing layer. Porous cellulose sheets also allow the sensing site to be modified with dried buffer that prevents any sample pH dependence of the observed color change. A highly selective fluoride optode using an Al(III)-porphyrin ionophore is examined as an initial example of this new anion sensing platform for measurements of fluoride levels in drinking water samples. In addition to Lewis acid-base recognition, hydrogen bonding recognition is also shown to be compatible with this sensing platform.

H. Koga, N. Namba, T. Takahashi, M. Nogi, Y. Nishina. Renewable Wood Pulp Paper Reactor with Hierarchical Micro/Nanopores for Continuous‐Flow Nanocatalysis. ChemSusChem 2017, 10, 2560. https://doi.org/10.1002/cssc.201700576., Continuous-flow nanocatalysis based on metal nanoparticle catalyst-anchored flow reactors has recently provided an excellent platform for effective chemical manufacturing. However, there has been limited progress in porous structure design and recycling systems for metal nanoparticle-anchored flow reactors to create more efficient and sustainable catalytic processes. In this study, traditional paper is used for a highly efficient, recyclable, and even renewable flow reactor by tailoring the ultrastructures of wood pulp. The “paper reactor” offers hierarchically interconnected micro- and nanoscale pores, which can act as convective-flow and rapid-diffusion channels, respectively, for efficient access of reactants to metal nanoparticle catalysts. In continuous-flow, aqueous, room-temperature catalytic reduction of 4-nitrophenol to 4-aminophenol, a gold nanoparticle (AuNP)-anchored paper reactor with hierarchical micro/nanopores provided higher reaction efficiency than state-of-the-art AuNP-anchored flow reactors. Inspired by traditional paper materials, successful recycling and renewal of AuNP-anchored paper reactors were also demonstrated while high reaction efficiency was maintained.

The reactivity of N-cyanomethyl quaternary salts of 4-, 5- and 7-azaindoles towards salicylic aldehydes has been studied. The interaction of azaindolium salts with salicylic aldehydes proceeds as a base-promoted domino reaction, giving the corresponding chromenoimidazopyrrolopyridines. In the case of the 7-(cyanomethyl)-7-azaindolium salt, the reaction was found to be more sensitive, but the use of the 1-methyl-substituted salt allowed the synthesis of the desired compounds, incorporating the heterocyclic core of isogranulatimide C, a marine natural product.

An efficient synthetic approach to access (indol-3-yl)ethane-1,2-diamines with a protecting group at the indole N atom from readily available 3-(2-nitrovinyl)indoles is reported. This approach includes solvent-free conjugate addition of O-pivaloylhydroxylamines to 1-Boc-3-(2-nitrovinyl)indoles followed by mild reduction of the adducts. The obtained (indol-3-yl)ethane-1,2-diamines are convenient synthetic precursors for several classes of marine alkaloids. The first total synthesis of racemic topsentin C, a secondary metabolite from Hexadella sp., based on this approach is reported. The initially proposed structure for topsentin C has been revised.

A chemosensor containing an o-hydroxyaniline unit as the reaction site was developed for colorimetric and fluorimetric detection of phosgene, which showed fast response (15 s), high specificity, and an extremely low detection limit. The chemosensor was incorporated into paper strips for visual detection of phosgene vapor.

Herein we demonstrate the first example of oligonucleotide-templated reaction (OTR) performed on paper, using lateral flow to capture and concentrate specific nucleic acid biomarkers on a test line. Quantitative analysis, using a low-cost benchtop fluorescence reader showed very high specificity down to the single nucleotide level and proved sensitive enough for amplification-free, on-chip, detection of endogenous concentrations of miR-150-5p, a recently identified predictive blood biomarker for preterm birth.

International audience; We developed a chemical method to covalently functionalize cellulose nanofibers and cellulose paper with mannoside ligands displaying a strong affinity for the FimH adhesin from pathogenic E. coli strains. Mannose-grafted cellulose proved efficient to selectively bind FimH lectin and discriminate pathogenic E. coli strains from non-pathogenic ones. These modified papers are valuable tools for diagnosing infections promoted by E.coli, such as cystitis or inflammatory bowel diseases, and the concept may be applicable to other life-threatening pathogens. The worldwide spread of antibiotic resistances raises serious health problems, and has driven the identification of new virulence factors and development of alternative antibacterial therapeutics. Mannose-binding FimH adhesin, expressed by Escherichia coli strains has been extensively studied as a target for disrupting bacterial attachment to the host cells. 1 Impressive results were obtained in the context of urinary tract infections (UTI), a prevalent infection type generally mediated by the attachment of uropathogenic E. coli strains (UPEC) to the highly mannosylated uroplakin transmembrane protein of urothelial lining cells. FimH antagonists orally administered to in vivo UTI mouse models, were shown to decrease the E.coli load in the bladder by several orders of magnitude, 2-4 making them competitive with conventional antibiotic treatment. 5,6 This concept was more recently extended to Crohn's disease (CD), an inflammatory disorder of the intestine where an altered gut microbiota, particularly the presence of adherent-invasive E. coli strains (AIEC), is suspected to play a key role in the pathogenesis. 7 Synthetic derivatives of heptylmannoside (HMan), a nanomolar FimH antagonist, 8 were shown to lower the AIEC bacterial level, signs of colitis and gut inflammation when administered per os (10 mg/kg) in CD mouse models. 9,10 Sensitive and rapid diagnostic systems are essential to evaluate the presence of E. coli expressing FimH adhesin in gut microenvironments in order to properly stratify patients before treatment. While the high prevalence of UPEC in the normally sterile urinary tract environment facilitates diagnosis, the AIEC niche is more complex, located at the ileal mucosa in 21 to 63% of CD patients, 11,12 within an ecological community of hundreds of symbiotic microorganisms. Furthermore, no specific biomarkers are currently effective at distinguishing AIEC from other commensal E. coli of the gut microbiota. Previously, it has been shown that AIEC pathobiont possesses specific allelic variants in the fimH gene, conferring them a high ability to adhere in vitro and to colonize the gut of CEABAC10 mice. 13 Establishing an approach to discriminate the strong mannose-binders from other bacteria would therefore be of tremendous importance for efficient diagnosis. In this work, we developed a heterogeneous support to specifically trap and accumulate pathogenic E.coli from biological fluids. Heptyl-α-D-mannoside (HMan) was grafted by click chemistry techniques onto cellulose nanofibers (CN) and cellulose paper (CP). HMan was previously identified as a potent binder of the isolated FimH lectin domain. 8 It should be noted that the lectin domain represents the high-affinity state of FimH under mechanical force and that full-length FimH display a lower affinity for mannosides. 14,15 Covalently functionalized CN or CP were characterized by Fourier transform spectroscopy (FTIR), elemental analysis, X-ray photo-electron spectrometry (XPS), and scanning electron microscopy (SEM). HMan-CN was first compared in vitro against CN grafted with lower FimH affinity ligands i.e. Man-CN lacking the hydrophobic heptyl chain, and HGlc-CN an analog with a glucose sugar that is not recognized by FimH lectin (Scheme 1). In addition, we switched the anomeric oxygen atom to a sulfur and synthesized HSMan-CN to prevent potential sugar hydrolysis from the surface by mannosidases. The modified CN were first assessed for their faculty to bind FimH and to prevent AIEC adhesion to intestinal cells. HMan-CN was then orally administered to the CEABAC10 mouse model of CD to assess its capacity to decrease AIEC in the feces of AIEC-infected mice and to act as a potential CD therapeutic. HM was next coated on CP and the capacity of the HMan-CP to selectively catch AIEC in solution was analyzed. Scheme 1. Chemical synthesis of the sugar-coated cellulose fibers.

Made available in DSpace on 2020-12-12T02:30:20Z (GMT). No. of bitstreams: 0 Previous issue date: 2020-02-15 Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) This paper describes the development and application of a paper-based analytical device (μPAD) for the determination of hydrogen peroxide, an important adulterant in milk. The method employs the reaction between hydrogen peroxide and guaiacol, catalyzed by peroxidase, producing a red product, which is then quantified by digital imaging. Experimental design methodology was used to optimize the experimental conditions. The linear concentration range was from 12.5 × 10− 4 to 150 × 10− 4 mol L− 1, resulting in the regression equation AB = 0.02466 (±0.00192) + 17.053 (±0.750) C, with an excellent correlation coefficient (r = 0.986). The relative standard deviations obtained were 1.1 and 1.3% (intra-day), and 4.8 and 2.9% (inter-day), for 25.0 × 10−4 and 100 × 10−4 mol L−1 of hydrogen peroxide, respectively. The limits of detection and quantification were 3.54 × 10− 4 and 11.8 × 10− 4 mol L− 1, respectively, with standard deviation of the blank of 0.002012. The proposed method was successfully applied for the determination of peroxide in milk samples, with recoveries between 92.2 and 109%. The proposed device constitutes a valuable analytical tool for the identification of hydrogen peroxide adulteration and offers advantages including low cost, simplicity, portability, and no (or minimal) requirement for sample pretreatment. Instituto de Química UNESP – São Paulo State University, R. Prof. Francisco Degni 55, P.O.Box 355 Instituto de Química UNESP – São Paulo State University, R. Prof. Francisco Degni 55, P.O.Box 355 FAPESP: #2015/21733-1 CAPES: 001

A nanostructured catalyst is introduced that demonstrates peroxidase mimicking activity. It consists of nickel- and nitrogen-doped graphene nanotubes loaded with platinum nanoparticles. Pt-decorated Ni-doped nitrogen-rich graphitic nanotube (Pt/Ni@NGT) was synthesized using a two-step procedure in which the precursors were first refluxed to form a supramolecular assembly followed by a pyrolysis and leaching step to form nanotubes. Afterwards, Pt was decorated on the outer surface of nanotube by an ultrasound assisted method. Pt/Ni@NGT was characterized by XPS, TEM, SEM, and HAADF–STEM. The as-prepared Pt/Ni@NGT nanostructure was used for the detection of glucose via catalyzing the oxidation of a substrate, 3,3′,5,5′-tetramethylbenzidine (TMB), to form a blue product (ox-TMB), thereby enabling colorimetric assay for enzymatically generated H2O2. The nanostructure exhibited excellent biocompatibility and led to highly efficient immobilization and retention of GOx. The method has a linear response in the 43 pM to 220 μM glucose concentration range, a detection limit as low as 1 pM and a limit of quantification of 3.4pM, along with good reproducibility(< 3%). A paper based visual microfluidic assay was also worked out that has an analytical range that extends from 0.1–50 mM. It is simple and rapid enough to be useful as a glucose home test.. The method was successfully applied to the determination of glucose in tear and saliva samples.

Enteromorpha prolifera-derived Fe