Electron-deficient Fe3O4@AC-NH2@Cu-MOF nanoparticles for enhanced degradation of electron-rich benzene derivatives via synergistic adsorption and catalytic oxidation.

Benzene derivatives in wastewater have negative impacts on ecosystems and human health, making their removal prior to discharge imperative. In this study, Fe3O4@AC-NH2@Cu-opa (AC-NH2 = aminoclay, Cu-opa = [Cu(opa)(bipy)0.5(H2O)]n (H2opa = 3-(4-oxypyridinium-1-yl) phthalic acid)) nanoparticles (NPs) were synthesized as adsorbent and catalyst for phenolic compound removal from wastewater. Fe3O4@AC-NH2@Cu-opa NPs demonstrated outstanding performance in the adsorption of phenol, exhibiting a remarkable adsorption capacity of up to 166.39 mg g-1 according to the Langmuir model. The composite also exhibited higher Fenton activity toward the degradation of electron-rich organic phenolic pollutants, with a rate approximately 3.4 times higher than that of Fe3O4 alone. The high catalytic activity of the composite was attributed to the large surface area and abundant active sites of the 2D charge-separated Cu-MOF. Meanwhile, the superparamagnetism of the Fe3O4 core enabled magnetic recollection and reuse without any significant loss of activity. Therefore, use of Fe3O4@AC-NH2@Cu-opa/H2O2 shows potential in an efficient method for the removal of phenolic compounds from wastewater.

Unveiling the In Situ and Solvent Polymerization Engineering for Highly Efficient and Flexible Thermally Activated Delayed Fluorescence Organic Light-Emitting Diodes.

Thermally activated delayed fluorescence (TADF) polymer has great potential for the construction of flexible solution-processed organic light-emitting diodes (OLEDs). However, the relationship between polymerization engineering and device functions has rarely been reported. Here, two novel TADF polymers, P-Ph4CzCN and P-Ph5CzCN, with a small energy gap between the first excited singlet and triplet states (ΔEST; <0.16 eV) were newly developed by both solvent and in situ polymerization of a styrene component. Detailed device performance testing indicates that both polymerization strategies ensure that the TADF polymer achieves comparable high efficiencies in commonly rigid devices, and the maximum external quantum efficiencies (EQEmax) were 11.9%, 14.1%, and 16.2% for blue, green, and white OLEDs, respectively. Although in situ polymerization provides a simplified device fabrication process, which avoids the complicated synthesis and purification of the polymer, the inevitable high-temperature annealing makes it fail in a plastic substrate device. In contrast, P-Ph5CzCN achieved by solvent polymerization enables the successful fabrication of a flexible device on a poly(ethylene terephthalate) (PET) substrate, which was the first reported flexible OLED based on a TADF polymer. This work provides a strong guideline for the simple fabrication of TADF polymer devices and the application of TADF polymer materials in OLED flexible panels and flexible lighting.

Online Accurate Detection of Breath Acetone Using Metal Oxide Semiconductor Gas Sensor and Diffusive Gas Separation.

Breath acetone (BrAce) level is an indicator of lipid oxidation rate, which is crucial for evaluating the status of ketoacidosis, ketogenic diet, and fat burning during exercise. Despite its usefulness, detecting BrAce accurately is challenging because exhaled breath contains an enormous variety of compounds. Although many sensors and devices have been developed for BrAce measurement, most of them were tested with only synthetic or spiked breath samples, and few can detect low concentration BrAce in an online manner, which is critical for extending application areas and the wide acceptance of the technology. Here, we show that online detection of BrAce can be achieved using a metal oxide semiconductor acetone sensor. The high accuracy measurement of low concentration BrAce was enabled by separating major interference gases utilizing their large diffusion coefficients, and the accuracy is further improved by the correction of humidity effect. We anticipate that the approach can push BrAce measurement closer to being useful for various applications.

A PCR-free screen-printed magnetic electrode for the detection of circular RNA from hepatocellular cancer based on a back-splice junction.

Circular RNA (circRNA) has the potential to be applied to disease diagnosis and therapy. However, the currently available circRNA detection techniques are limited. This work proposes a sensitive and selective approach for circRNA detection based on gold nanoparticle-modified screen-printed magnetic electrodes (AuNPs-SPME). Magnetic beads (MBs) with capture probes based on specific back-splice junction (BSJ) sites were employed to identify and selectively isolate the target circRNA, which could be directly adsorbed onto the AuNPs-SPME. Then, the circRNA attached to the surface was detected by changes in the methylene blue redox signal. The simple and time-saving AuNPs-SPME is highly sensitive (LOD = 1.0 pM) to circCDYL, one of the biomarkers of hepatocellular cancer (HCC). The analytical performance of the method presented has also been verified in human serum samples, holding great promise for clinical diagnosis.

Differential coulometry based on dual screen-printed strips for high accuracy levodopa determination towards Parkinson's disease management.

As a vital therapeutic agent for Parkinson's disease, dosage control of levodopa has always been a major obstacle in ensuring efficacy and curbing side effects. Simple and fast electrochemical detection methods are the main force in this field. Here, we presented a differential dual-strip method based on the coulometry for high accuracy determination of levodopa. The difference between the two strip signals with or without the tyrosinase extracted the levodopa signal from the samples. The Prussian Blue modified carbon screen-printed electrode was used to convert and amplify the electrochemical signal upon the presence of levodopa. The system exhibited a linear behavior in the 0-10 µM concentration range and a detection limit of 0.25 µM. Furthermore, it was proved to be stable in effectively distinguishing levodopa from complex samples through anti-interference experiments and serum tests. We demonstrated the superiority of dual-strip differential coulometry for the determination of levodopa towards Parkinson's disease clinical management.

One-step modification of nano-polyaniline/glucose oxidase on double-side printed flexible electrode for continuous glucose monitoring: Characterization, cytotoxicity evaluation and in vivo experiment.

The single-step modification of the nanostructured polyaniline (PANI)/glucose oxidase (GOD) enzyme on double-sided, screen-printed, flexible electrodes doped with Prussian blue (PB), has been achieved and successfully applied in continuous glucose monitoring in vivo, and its biocompatibility has been evaluated systematically. The proposed fabrication procedure is simple, low cost, and suitable for large-scale production. PB doped with carbon ink catalyzes the reduction of hydrogen peroxide (H2O2) in low-voltage conditions, which could help eliminate interferences. And the PANI/GOD nanostructure makes the GOD enzyme more stable for long-term, in vivo monitoring. More importantly, a polyurethane (PU) layer is deposited on the electrode's surface as a diffusion limiting membrane that enhanced the linear range and biocompatibility. In tests in vitro, the proposed biosensor achieved a linear range of 0-12 mM and a good sensitivity of 16.66 µA·mM-1·cm-2(correlation coefficient R2 = 0.9962) with an excellent specificity to glucose. The biosensor exhibits long-term stability, with a maximum lifespan of 14 days when stored in phosphate buffer solution at 4 °C, and achieves a sensitivity of 120%. The biocompatibilities of the electrode materials have also been systematically evaluated in cytotoxicity and cell adhesion tests to ensure the safety of implantation. In experiments in vivo, the biosensor can successfully monitor the glucose level fluctuation of rats after 24 h following implantation. Overall, the biosensor fabricated with the double-side, screen-printing process, satisfies the glucose monitoring range in vivo and eliminates various types of interference, thus establishing a new, large-scale production procedure for flexible in vivo biosensors.

Fully transient electrochemical testing strips for eco-friendly point of care testing.

With the growing number of patients suffering from noninfectious chronic diseases, the consumption of point of care testing strips increases exponentially, particularly blood glucose testing strips, causing an increasingly severe conflict between strip recycling and the environment. In this paper, fully transient electrochemical strips are developed as a substitute for non-degradable strips. Proper explorations were made, including finding out suitable degradable substrates for strip-making among different degradable materials and optimization of degradable conducting paste. Taking advantage of dissolvable polymer-based materials and nontoxic carbon materials, the transient strips have validated electrochemical functionality to determine physiological levels of glucose with a sensitivity of 14.33 µA mM-1 cm-2 (correlation coefficient R 2 is 0.99498) and reached full-degradation within a week after disposal. The interference experiment (negligible interference current response under 7%) and recovery tests (recovery ratio ranging from 92.46% to 102.47%) have illustrated its practical application in real sample detection. Such degradable-characterized testing strips can be widely used in chronic disease management with daily eco-friendly point of care testing, without potential pollution to the environment.

High-Resolution Rapid Prototyping of Liquid Metal Electronics by Direct Writing on Highly Prestretched Substrates.

A rapid and inexpensive method to produce high-resolution liquid metal patterns and electronics on stretchable substrates was introduced. Two liquid-phase gallium-indium (GaIn) alloy patterns, conductive lines, and interdigitated electrodes, were directly written or shadow mask-printed on a prestretched elastomeric substrate surface. Then, the prestretched substrate was released to recover its original length, and thus, electronic patterns simultaneously shrank on it. After these patterns were transferred to another prestretched substrate by the stamp printing method, the patterning resolution was demonstrated to increase by totally 50 times for the two successive stretch-release-shrink operations. Additionally, the resistance of the handwritten liquid metal conductive line traces remained nearly unchanged during the stretching process, which is believed to be feasible for electrical connections in stretchable electronics. The rapid prototyping of a serpentine strain sensor was successfully demonstrated to be highly sensitive and repeatable with a stretching ratio ranging from 0 to 200%. The proposed method paves a new way to fabricate stretchable electronic devices with high patterning resolution.

A simple and low-cost screen printed electrode for hepatocellular carcinoma methylation detection.

There is a great demand for robust diagnostic and prognostic approaches for Hepatocellular Carcinoma (HCC). DNA methylation, a common epigenetic modification, has been found in many promoter regions of tumor suppressor genes. Hypermethylation of these gene promoters will repress the gene transcription and lead to the occurrence of cancers. The abnormal methyation level of the p16 gene promoter could be a promising marker for the detection of HCC. The adsorption affinities between different DNA bases and AuNPs are not the same. After bisulfite treatment and asymmetric PCR, methylation and unmethylation sequences can be changed into guanine-enriched and adenine-enriched sequences, respectively. A home-made gold nanoparticle modified screen printed carbon electrode (AuNP-SPCE) was employed to distinguish the adsorption affinities between guanine-enriched and adenine-enriched sequences, which could be used to analyze the level of DNA methylation. Several key experimental factors were investigated and optimized. The results had shown that the optimal AuNP electrodeposition time was 100 s and 15 min of adsorption could distinguish guanine-enriched and adenine-enriched sequences with a concentration of 100 nM at 25 °C. The detection limit of our AuNP-SPCE was 1.1 ng, and the assay had a good sensitivity of 10% methylation change and was able to distinguish only one methylated CpG site. What's more, the RSD over three assays with a disposable AuNP-SPCE was ≤7.2%. The assay was applied to real samples including cell lines and clinical tissues. Compared with normal hepatic cell lines and normal tissues, lower signals of HCC cell lines and cancer tissues were observed, respectively. It had shown a good discrimination of the abnormal methylation level of the p16 gene promoter.

Three-dimensional paper-based microfluidic electrochemical integrated devices (3D-PMED) for wearable electrochemical glucose detection.

Wearable electrochemical sensors have attracted tremendous attention in recent years. Here, a three-dimensional paper-based microfluidic electrochemical integrated device (3D-PMED) was demonstrated for real-time monitoring of sweat metabolites. The 3D-PMED was fabricated by wax screen-printing patterns on cellulose paper and then folding the pre-patterned paper four times to form five stacked layers: the sweat collector, vertical channel, transverse channel, electrode layer and sweat evaporator. A sweat monitoring device was realized by integrating a screen-printed glucose sensor on polyethylene terephthalate (PET) substrate with the fabricated 3D-PMED. The sweat flow process in 3D-PMED was modelled with red ink to demonstrate the capability of collecting, analyzing and evaporating sweat, due to the capillary action of filter paper and hydrophobicity of wax. The glucose sensor was designed with a high sensitivity (35.7 µA mM-1 cm-2) and low detection limit (5 µM), considering the low concentration of glucose in sweat. An on-body experiment was carried out to validate the practicability of the three-dimensional sweat monitoring device. Such a 3D-PMED can be readily expanded for the simultaneous monitoring of alternative sweat electrolytes and metabolites.

Layer-by-layer chitosan-decorated pristine graphene on screen-printed electrodes by one-step electrodeposition for non-enzymatic hydrogen peroxide sensor.

Layer-by-layer chitosan-decorated pristine graphene on screen-printed electrodes was achieved by one-step electrodeposition method and an enzyme-free hydrogen peroxide electrochemical biosensor was fabricated for its application. Negatively charged pristine graphene absorbed with positively charged chitosan by electrostatic interactions was electrodeposited on the electrodes. The successful immobilization of pristine graphene was confirmed by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and electrochemical characterizations. The graphene-chitosan volume ratio and cyclic voltammetry scan cycles during the electrodeposition process were optimized. The resulting hydrogen peroxide biosensors showed a 178 times improved sensitivity and exhibited two wide linear detection ranges from 20 µM to 20 mM and from 20 mM to 60 mM. The biosensors also showed a good reproducibility, stability, selectivity and could be used in real samples detection. The superior electrochemical performance of graphene-chitosan was attributed to the preservation of excellent properties of pristine graphene, and the formation of layer-by-layer structure with high surface area. The proposed strategy of direct immobilization of pristine graphene can be extended for the immobilization of other nanomaterials and biomolecules.

Characterization of polysaccharides with antioxidant and hepatoprotective activities from the wild edible mushroom Russula vinosa Lindblad.

The aim of the present study was to investigate the antioxidant and hepatoprotective effects of water-soluble polysaccharides (RVLWP) and alkali-soluble polysaccharides (RVLAP) from Russula vinosa on carbon tetrachloride (CCl4)-induced acute liver damage in mice. For the in vitro antioxidant activities, RVLWP and RVLAP exhibited potent 1,1-diphenyl-2-picrylhydrazyl (DPPH) radical scavenging activity (IC50 = 1.55 ± 0.04 and 3.37 ± 0.21 mg/mL, respectively), hydrogen peroxide scavenging activity (IC50 = 6.07 ± 0.24 and 9.23 ± 0.54 mg/mL, respectively), lipid peroxidation inhibitory effect (IC50 = 0.52 ± 0.095 and 0.86 ± 0.043 mg/mL, respectively), and moderate reducing power and Fe(2+) chelating activity (IC50 = 1.86 ± 0.0036 and 0.22 ± 0.0057 mg/mL, respectively). Ascorbic acid was employed as the standard antioxidant in the present study. For the in vivo hepatoprotective activity, administration of RVLWP and RVLAP (200 mg/kg) significantly prevented the elevation in serum alanine aminotransferase (ALT) and aspartate aminotransferase (AST) activities in acute liver damage induced by CCl4 and suppressed hepatic malondialdehyde (MDA) formation. Mice treated with RVLWP and RVLAP demonstrated a better profile of antioxidants with augmented activities of superoxide dismutase (SOD) and glutathione peroxidase (GSH-Px) in the liver. The results suggest that RVLWP and RVLAP protect the liver from CCl4-induced hepatic damage via antioxidant mechanisms.