Green, pH-Sensitive, Highly Stretchable, and Hydrogen Bond-Dominated Ionogel for Wound Healing Activity.

Traditional hydrogel dressings generally have poor mechanical properties and stability when subjected to external stress due to the undesirable chain entanglement structure of their single valence bond compositions. Therefore, it is particularly important to develop a type of gel dressing with good mechanical strength, stability, and environment-friendly monitoring. In this work, a transparent, pH-sensitive, highly stretchable, and biocompatible anthocyanidin ionogel dressing was prepared, realizing green and accurate detection. Attributed to the antibacterial activity of the ionic liquid, the biocompatibility of the pectin, and the ability to scavenge free radicals of the anthocyanidin, the ionogel dressing exhibited excellent re-epithelialization in the 14 day wound healing process. Besides, changes in pH values monitoring of the ionogel over 3 days coincided with normal wound exudate. The obtained ionogel also showed good water retention, swelling properties, mechanical stretchability, and 5 week stability, illustrating great potential in wound dressings.

A label-free colorimetric 3D paper-based device for ochratoxin A detection using G-quadruplex/hemin DNAzyme with a smartphone readout.

The colorimetric sensor usually depends on enzyme-mediated signal amplification to achieve trace analysis of ochratoxin A (OTA) residues in food samples. However, the enzyme labeling and manual addition of reagents steps increased assay time and operation complexity, restricting their application in point-of-care testing (POCT). Herein, we report a label-free colorimetric device integrating a 3D paper-based analytical device and a smartphone as handheld readout for rapid and sensitive detection of OTA. Using vertical-flow design, the paper-based analytical device enables the specific recognition of target and self-assembly of G-quadruplex (G4)/hemin DNAzyme to be performed, then employs DNAzyme for transducing the OTA binding event signal into a colorimetric signal. The design of independent functional units, including biorecognition unit, self-assembly unit and colorimetric units, which can address crowding and disorder of biosensing interfaces and improve the recognition efficiency of aptamer (apta). In addition, we eliminated signal losses and nonuniform coloring by introducing carboxymethyl chitosan (CMCS) to obtain perfectly focused signals on colorimetric unit. On the basis of parameter optimization, the device exhibited a detection range of 0.1-500 ng/mL and a detection limit of 41.9 pg/mL for OTA. Importantly, good results were obtained in spiked real samples, indicating applicability and reliability of developed device.

Prussian blue analogues based polymer monolith with amphiphilic interface to construct highly selective and sensitive imidacloprid chemosensor.

The most widely used assays for pesticides currently rely on the inhibition of natural enzymes, which are particularly sensitive to the surrounding environment, leading to some unreliable results. Up till now, there are few studies explored chemical detection methods for these stable pesticides. Here, we reported a novel chemosensor system and polymer materials for highly sensitive detection of imidacloprid pesticide. The polymer monolith with tunable surface hydrophilicity allows solvent-dependent adsorption of low-abundance target pesticide molecule. Prussian blue particles with Fenton catalytic activity were introduced into the polymeric monolith through Pickering emulsion, which capable of degrading the pesticide adsorbed on the column surface into easily detectable ions (NO3-, Cl-). This all-in-one functional material can minimize the interference of other non-target molecules through dual-channel detection, enabling sensitive detection of imidacloprid pesticide (30 ppb). We believe that the material described in this paper demonstrates for the first time the combination of an active polymer monolith for the enrichment and catalytic degradation with sensitive detection of pesticides, and this protocol can be used to develop a range of pesticides chemical sensing methods in the future.

Novel Paraquat Detection Strategy Enabled by Carboxylatopillar[5]arene Confined in Nanochannels on a Paper-Based Sensor.

Paper-based optical sensors have emerged as a promising technology for pesticide detection and attracted extensive attention. However, in practical analytical applications, it may suffer from limited sensitivity with traditional signal amplification strategies. Here, we developed a novel mesoporous silica-modified paper-based sensor for a sensitive capture and analysis of the pesticide paraquat. Carboxylatopillar[5]arene was covalently introduced into the nanochannels for the rapid capture of target paraquat molecules due to the mass transfer confinement effect within nanopores. In addition, the large specific surface area of mesoporous silica enabled high-abundance immobilization of the capture agent and promoted its binding efficiency, which, in turn, contributed to improving the sensitivity. This work highlights the great potential of nanochannels as a development platform for sensitive paper-based sensors that can be used to develop new systems for the detection of paraquat and even other pesticides.

A pH-Sensitive, Stretchable, Antibacterial Artificial Tongue Based on MXene Cross-Linked Ionogel.

Dehydration has always been a confusing problem for a hydrogel exposed to air, which restricts its application in practical detection. While an ionogel with unique properties can lock water molecules efficiently due to its low vapor pressure, the design and development of an ionogel with excellent water-locking properties and stability to achieve satisfactory detection are thus highly desirable. In this work, a pH-sensitive, stretchable, antibacterial, and stable ionogel artificial tongue was fabricated through dual cross-linking. The artificial tongue consisted of MXene as a cross-linking agent, phenol red as an indicator, gelatin, N-(2-hydroxyethyl) acrylamide, and 1-butyl-3-methylimidazolium chloride as the three-dimensional polymer network. A small quantity of MXene was used as a cross-linker the first time to promote the initiator in the system to generate free radicals, accelerating the reaction process and the multilevel linkage among the polymers. Meanwhile, the indicator phenol red was introduced into the ionogel successfully for the first time, showing great stability in 5 weeks. After evaluation by the Brand-Altman analysis, it was found that the method of pH measurement using ionogels had good consistency with the pH meter measurement method. Additionally, the prepared ionogel presented excellent water retention, mechanical stretchability, antibacterial property, and stability, as well as good test results in the test of artificial simulated saliva, demonstrating great potential in clinical applications.

A Novel Virus Detection Strategy Enabled by TR512-Peptide-Based Bioorthogonal Capture and Enrichment of Preamplified Nucleic Acid.

High-cost viral nucleic acid detection devices (e.g., qPCR system) are limited resources for developing counties and rural areas, leading to underdiagnosis or even pandemics of viral infectious diseases. Herein, a novel virus detection strategy is reported. Such detection method is enabled by TR512-peptide-based biorthogonal capture and enrichment of commercially available Texas red fluorophore labeled nucleic acid on the functionalized paper. The GST-TR512 fusion protein electrostatically immobilized on the paper is constructed to retain the binding affinity of TR512-peptide toward Texas red fluorophore labeled nucleic acid released in the preamplification process, then the enrichment of analytes enhances fluorescence signal for rapid detection as volume of sample filters through the paper. The method is generally applicable to different nucleic acid preamplification strategies (PCR, RAA, CRISPR) and different virus types (Hepatitis B virus (HBV), African swine fever virus (ASFV), human papillomavirus (HPV), and severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2 or 2019 nCoV)). Finally, a full-set virus detection device is developed in house to detect the presence of Hepatitis B virus (HBV) viral gene in patients' blood samples. Taken together, we first apply TR512-peptide in the signal enrichment and the novel detection strategy may offer an inexpensive, rapid, and portable solution for areas with limited access to a standard diagnosis laboratory.

Target-Responsive Smart Nanomaterials via a Au-S Binding Encapsulation Strategy for Electrochemical/Colorimetric Dual-Mode Paper-Based Analytical Devices.

Target-responsive nanomaterials attract growing interest in the application of drug delivery, bioimaging, and sensing due to the responsive releasing of guest molecules by the smart molecule gate. However, it remains a challenge to develop smart nanomaterials with simple assembly and low nonspecific leakage starting from encapsulation strategies, especially in the sensing field. Herein, Au nanoclusters (Au NCs) were first grown on porous carbon derived from ZIF-8 (PCZIF) to be employed as nanocarriers. By employing the Au NCs as linkers and aptamer (Apta) double-strand hybrids (target Apta and SH-complementary DNA) as capping units, we reported the novel target-responsive nanomaterials of Apta/Au NCs-PCZIF/hemin through Au-S binding encapsulation for sensing assays. The Au-S binding encapsulation strategy simplified the packaging procedure and reduced non-target responsive leakage. As a proof, ochratoxin A (OTA) as a model target participates in the double-strand hybrid competitive displacement reaction and triggered Apta conformation switches from a coil to a G-quadruplex structure accompanied by the dissociation of the gatekeeper. Simultaneously, the released hemin can initiate a self-assembly to form G-quadruplex/hemin DNAzyme. Interestingly, owing to DNAzyme providing electron transfer mediators and peroxidase-like activity, we proposed an electrochemical/colorimetric dual-mode paper-based analytical device (PAD) that provided self-verification to enhance reliability and accuracy, benefiting from independent signal conversion and transmission mechanism. As a consequence, the proposed dual-mode PAD could achieve sensitive electrochemical detection and visual prediction of OTA in the range of 1 pg/mL to 500 ng/mL and 50 pg/mL to 500 ng/mL, respectively. The electrochemical detection limit for OTA was as low as 0.347 pg/mL (S/N = 3). We believe that this work provides point-of-care testing (POCT) tools for a broad spectrum of applications.

The BODIPY-based chemosensor for the fluorometric determination of organochlorine pesticide dicofol.

Dicofol is an organochlorine pesticide, which is widely used in fruits, tea and other crops, and is moderately toxic to humans. Therefore, the monitoring of organochlorine pesticide-dicofol is critical for food safety. In this work, a fluorometric chemosensor based on mercaptoethanol and boron dipyrromethene (BODIPY) was first constructed to detect the dicofol. The chemosensor displayed turn-off fluorescence behavior upon dicofol with a detection limit of 200 ppb. The nucleophilicity of the glutathione and other biological thiols was studied to evaluate the reactivity of thiols with dicofol. In practical applications, an obvious color difference was observed on a paper based microfluidic device modified by phenyltriethoxysilane (PTES). We designed an integrated device for pretreatment and paper-based detection, and successfully used for the detection of dicofol in tea. The applicability was demonstrated by detection of dicofol in real tea samples with good recovery ranging from 86% to 109%. The apparatus was convenient and could be used for on-site evaluation of dicofol.

[Preparation of Fe3O4@BA-MOF magnetic solid-phase extraction material and its application to the detection of pesticide residues in tea].

Tea is one of the most popular beverages worldwide, and its quality is often affected by the excessive pesticide residues during production. During the detection of pesticide residues in tea by chromatography-mass spectrometry and other methods, a strong matrix effect attributed to tea polyphenols and pigments is observed, which seriously impacts the analysis results. In this study, Fe3O4 magnetic nanoparticles and boric acid-functionalized metal organic framework (BA-MOF) materials were combined to prepare a highly efficient adsorbent Fe3O4@BA-MOF for capturing tea polyphenols and pigments. An effective analysis method for pesticide residues in tea samples in combination with gas chromatography-mass spectrometry was established. The introduction of boronic acid ligands into the metal organic framework, as the recognition site of cis-diols, enhanced the polyphenol capture ability. Adsorption of the pigment in the matrix was achieved through π-π interactions between the MOF ligand and the pigment. This new material has significant advantages such as rapid magnetic separation, large surface area, and abundant functional sites. Fe3O4@BA-MOF was prepared by employing simple conditions and characterized by Fouriertransform infrared spectroscopy, scanning electron microscopy, and X-ray diffractometry to identify its functional groups and morphology. After investigating the adsorption effect of different doses of Fe3O4@BA-MOF adsorbents (5, 10, 30, 50, and 80 mg) on tea polyphenols, 50 mg of the adsorbent was added to the tea matrix and shaken thoroughly. The tea polyphenol content in the matrix solution was determined using an ultraviolet spectrophotometer. The polyphenols were reduced by 74.58% within 5 min. The effect of solution pH (2.0, 4.0, 6.0, and 7.0) on the adsorption efficiency was investigated, and pH 7.0 was chosen as the optimal condition. By adjusting the pH of the solution, Fe3O4@BA-MOF could be recycled, and it maintained the excellent adsorption performance after four cycles of use. The introduction of Fe3O4 magnetic nanoparticles led to rapid magnetic response characteristics during sample pretreatment and improved the pretreatment efficiency. In the actual application of tea pesticide detection, after Fe3O4@BA-MOF pretreatment, the average recovery rates of the ten pesticides were in the range of 75.8%-138.6%, and the RSD was in the range of 0.5%-18.7% (n=3). The Fe3O4@BA-MOF nanocomposite prepared by introducing the boric acid ligand into the MOF structure and incorporating Fe3O4 magnetic nanoparticles could specifically adsorb the tea polyphenol matrix. When applied to the detection of pesticide residues in tea, it purifies the matrix and improves the detection efficiency, thus being suitable for the detection and analysis of pesticides in tea.

Flexible Ti3C2Tx MXene/PANI/Bacterial Cellulose Aerogel for e-Skins and Gas Sensing.

Flexible pressure sensors made of carbon materials have been used in electronic skins (e-skins), whose performance can be enhanced if composite sensing materials are used. Herein, an MXene/polyaniline/bacterial cellulose (MXene/PANI/BC) aerogel sensor has been fabricated through the self-assembly process between the MXene and one-dimensional active material. Combined with fewer-layer or single-layer MXenes, the as-fabricated aerogel could be used as the active layer of the pressure sensor, monitoring tiny motion signals of finger bending, wrist bending, and pulse beating. Bluetooth wireless transmission could also be realized to monitor the real-time spatial pressure distributions on the mobile phone, making the aerogel-based sensor an ideal candidate in e-skins. Meanwhile, the aerogel-based sensor is sensitive toward NH3 due to the unique three-dimensional (3D) structure of the aerogel and the abundant terminal groups (such as -O, -OH, and -F) of the MXene in the system that ensure efficient electronic transfer for the sensing process and create active sites for the absorption with the target gas. This work offers a versatile platform to develop MXenes to fabricate 3D composite aerogels for high-performance flexible multiple sensors.

Electrochemical/visual dual-readout aptasensor for Ochratoxin A detection integrated into a miniaturized paper-based analytical device.

Development of portable, sensitive and reliable devices for Ochratoxin A (OTA) detection is highly demanded, especially for resource-limited regions. Herein, a novel paper-based analytical device (PAD) is designed through wax printing and screen-printed technologies, which integrates sample flowing, electrode modification, cleaning and electrochemical (EC)/colorimetric signal output. To greatly enhance the detection sensitivity, we synthesized a chitosan functionalized MoS2-Au@Pt (Ch-MoS2-Au@Pt) via electrostatic self-assembly, and used it to immobilize the label aptamer (apta2) for signal regulation and amplification. Concretely, with the addition of analytes, the Ch-MoS2-Au@Pt-apta2 could be combined on the sensing interface by specific biorecognition and catalyzed reduction of H2O2, resulting in a remarkable EC response. Meanwhile, the released hydroxyl radicals (·OH) flowed to the visualization zone and promoted the oxidation of 3,3',5,5'-tetramethylbenzidine for colorimetric detection. Consequently, the dual-mode PAD achieved acceptable prediction and accurate analysis in the range of 0.1-200 ng mL-1 and 1 × 10-4-200 ng mL-1 by matching the visual and EC signal intensity, respectively. Compared with traditional single-mode sensor for OTA, the proposed dual-mode aptasensor featuring independent signal conversion and readout, not only avoided the false-positive signal associated with detection condition and operation, but also enlarged the detection ranges and improved the sensitivity. Furthermore, the consistency of EC/colorimetric assay was validated in real OTA samples. Overall, this work provided a portable, cost-effective, sensitive and visualized aptasensor platform, which could be extended to various other mycotoxins in the field of food safety.

Comparison of Lipids Extracted by Different Methods from Chinese Mitten Crab (Eriocheir sinensis) Hepatopancreas.

The effects of four different extraction methods (Folch, Soxhlet, two-step, and enzyme-assisted aqueous extraction) on the yields, lipid class, fatty acids (FAs) composition, minor components (including carotenoid, cholesterol), and thiobarbituric acid reactive substances values of lipids in the hepatopancreas of Chinese mitten crab (Eriocheir sinensis) were investigated. The C16:0, C18:1, and C18:2 were identified to be the dominant FAs in crab lipids, and the FAs were present in the form of triglycerides. The Soxhlet and enzyme-assisted extraction were more suitable for crab lipids extraction, showing higher extraction rates and oxidative stability. Especially, the lipid extracted by enzyme-assisted extraction has high carotenoids content. The components of crab lipids extracted by enzyme-assisted aqueous extraction were further identified using untargeted metabolomics methods. The polyunsaturated fatty acid, sterols, amino acids, products of lipid ß-oxidation and ATP degradation, phosphatidyl ethanolamine, and astaxanthin were founded in crab oil. PRACTICAL APPLICATION: The Chinese mitten crab (Eriocheir sinensis) is a popular aquatic food in China. The hepatopancreas is the major lipid storage organ of crab, and the distinctive flavor of crab is mainly from it. To compare the different extraction methods on yield, composition and properties of crab lipids can be helpful for lipids production from crab hepatopancreas. Meanwhile, the crab hepatopancreas lipids are rich in polyunsaturated fatty acids and astaxanthin, and have potential to be as a functional component and a crab flavor additive in food industry.