Fabrication of an Antifouling Surface Plasmon Resonance Sensor with Stratified Zwitterionic Peptides for Highly Efficient Detection of Peanut Allergens in Biscuits.

Peanut allergen monitoring is currently an effective strategy to avoid allergic diseases, while food matrix interference is a critical challenge during detection. Here, we developed an antifouling surface plasmon resonance sensor (SPR) with stratified zwitterionic peptides, which provides both excellent antifouling and sensing properties. The antifouling performance was measured by the SPR, which showed that stratified peptide coatings showed much better protein resistance, reaching ultralow adsorption levels (<5 ng/cm2). Atomic force microscopy was used to further analyze the antifouling mechanism from a mechanical perspective, which demonstrated lower adsorption forces on hybrid peptide coatings, confirming the better antifouling performance of stratified surfaces. Moreover, the recognition of peanut allergens in biscuits was performed using an SPR with high efficiency and appropriate recovery results (98.2-112%), which verified the feasibility of this assay. Therefore, the fabrication of antifouling sensors with stratified zwitterionic peptides provides an efficient strategy for food safety inspection.

Regenerated SERS substrate based on Ag/AuNPs-TiO2-oxidized carbon cloth for detection of imidacloprid.

Imidacloprid (IMI) are widely used in modern tea industry for pest control, but IMI residues pose a great threat to human health. Herein, we propose a regeneration metal-semiconductor SERS substrate for IMI detection. We fabricated the SERS sensor through the in-situ growth of a nano-heterostructure incorporating a semiconductor (TiO2) and plasmonic metals (Au, Ag) on oxidized carbon cloth (OCC). Leveraging the high-density hot spots, the formed Ag/AuNPs-TiO2-OCC substrate exhibits higher enhancement factors (1.92 × 108) and uniformity (RSD = 7.68%). As for the detection of IMI on the substrate, the limit of detection was lowered to 4.1 × 10-6 µg/mL. With a hydrophobic structure, the Ag/AuNPs-TiO2-OCC possessed excellent self-cleaning performance addressing the limitation of single-use associated with traditional SERS substrates, as well as the degradation capability of the substrate under ultraviolet (UV) light. Accordingly, Ag/AuNPs-TiO2-OCC showcases outstanding SERS sensing and regenerating properties, making it poised for extensive application in the field of food safety assurance.

Design of a Facile Antifouling Sensor Based on the Synergy between an Antibody and Phase-Transited BSA.

Nonspecific adsorption has always been a critical challenge for sensor detection; thus, an efficient and facile approach for fabricating antifouling sensors is highly desirable. Here, we developed an antifouling coating on sensor surfaces, conveniently made with a simple drip of phase-transited BSA (PTB) followed by a modification with a peanut allergen antibody, which unexpectedly provides synergistic antifouling properties in sensors. Atomic force microscopy and scanning electron microscopy were used to evaluate the surface evenness. Optimizations in terms of PTB modification time and concentrations were performed using surface plasmon resonance by measuring protein resistance capabilities. Compared to bare Au surfaces, the PTB-modified surfaces exhibited low adsorption against BSA (<10 ng/cm2) and good resistance against lysozyme (Lyz). After immobilizing antibodies, the antifouling performance of the sensor coatings had an obvious enhancement, with almost no BSA adsorption and low lysozyme adsorption. The target recognition was also analyzed to verify the good sensing performance of the antifouling sensor. This understanding of antibody synergy provides suggestions for the development of antifouling sensors.

Rethreading Design of Ratiometric roGFP2 Mimetic Peptide for Hydrogen Peroxide Sensing.

Reconstruction of the miniaturized peptide to mimic the tailored functions of protein has been attractive but challenging. Herein, initialized from the crystal structure of redox-sensitive green fluorescent protein-2 (roGFP2), we propose a practical approach to construct the roGFP2 mimetic peptide by rethreading the aromatic residues adjacent to the chromophore fragment. By fine-tuning the residues of peptides, a mini tetrapeptide (Cys-Phe-Phe-His) was designed, which can act as a hydrogen peroxide sensor using its ratiometric fluorescence. The roGFP2 mimetic tetrapeptide is biocompatible and photostable and has competitive fluorescent properties with roGFP2 by the virtue of its assembly induced emissions. We expand the ratiometric tetrapeptide for sensing hydrogen peroxide in acidic chambers. The results provide a promising approach for the artificial design of miniaturized peptides with the desired function.

Quantitative Ratiometric Biosensors Based on Fluorescent Ferrocene-Modified Histidine Dipeptide Nanoassemblies.

Fluorescent proteins (FPs) provide a ratiometric readout for quantitative assessment of the destination of internalized biomolecules. FP-inspired peptide nanostructures that can compete with FPs in their capacity are the most preferred building blocks for the synthesis of fluorescent soft matter. However, realizing a ratiometric emission from a single peptide fluorophore remains exclusive since multicolor emission is a rare property in peptide nanostructures. Here, we describe a bioinspired peptidyl platform for ratiometric intracellular quantitation by employing a single ferrocene-modified histidine dipeptide. The intensiometric ratio of green to blue fluorescence correlates linearly with the concentration of the peptide by three orders of magnitude. The ratiometric fluorescence of the peptide is an assembly-induced emission originating from hydrogen bonds and aromatic interactions. Additionally, modular design enables ferrocene-modified histidine dipeptides to use as a general platform for the construction of intricate peptides that retain the ratiometric fluorescent properties. The ratiometric peptide technique promises flexibility in the design of a wide spectrum of stoichiometric biosensors for quantitatively understanding the trafficking and subcellular fate of biomolecules.

The Safety of Cold-Chain Food in Post-COVID-19 Pandemic: Precaution and Quarantine.

Since the outbreak of coronavirus disease-19 (COVID-19), cold-chain food contamination caused by the pathogenic severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) has attracted huge concern. Cold-chain foods provide a congenial environment for SARS-CoV-2 survival, which presents a potential risk for public health. Strengthening the SARS-CoV-2 supervision of cold-chain foods has become the top priority in many countries. Methodologically, the potential safety risks and precaution measures of SARS-CoV-2 contamination on cold-chain food are analyzed. To ensure the safety of cold-chain foods, the advances in SARS-CoV-2 detection strategies are summarized based on technical principles and target biomarkers. In particular, the techniques suitable for SARS-CoV-2 detection in a cold-chain environment are discussed. Although many quarantine techniques are available, the field-based quarantine technique on cold-chain food with characteristics of real-time, sensitive, specific, portable, and large-scale application is urgently needed.

Color-Tunable Fluorescent Hierarchical Nanoassemblies with Concentration-Encoded Emission.

Cephalopods possess a dynamic coloration behavior to change their iridescence due to the concentration-induced optical properties of chromatophores and hierarchical assembly of reflectin. However, cephalopods rarely have iridescence in the darkfield. It would be interesting to develop color-tunable fluorescent hierarchical nanoassemblies with concentration-encoded emission. Herein, to construct the bioavailable fluorophore with dynamic coloration properties, a histidine-rich peptide is designed, which can self-assemble into hierarchical nanoassemblies stabilized by hydrogen bonds and π-π stacking interactions. The peptidyl nanoassemblies emit fluorescent iridescence, encompassing the blue to orange region due to the assembly-induced emission. The fluorescence of histidine-rich peptides is color-tunable and reversible, which can be dynamically controlled in a concentration-encoded mode. Due to the coloration ability of histidine-rich peptides, fluorescent polychromatic human cells are developed, highlighting its potential role as a fluorescent candidate for future applications such as bioimaging, implantable light-emitting diodes, and photochromic camouflage.

Lubricin-Inspired Loop Zwitterionic Peptide for Fabrication of Superior Antifouling Surfaces.

Biofouling represents great challenges in many applications, and zwitterionic peptides have been a promising candidate due to their biocompatibility and excellent antifouling performance. Inspired by lubricin, we designed a loop-like zwitterionic peptide and investigated the effect of conformation (linear or loop) on the antifouling properties using a combination of surface plasma resonance (SPR), surface force apparatus (SFA), and all atomistic molecular dynamics (MD) simulation techniques. Our results demonstrate that the loop-like zwitterionic peptides perform better in resisting the adsorption of proteins and bacteria. SFA measurements show that the loop-like peptides reduce the adhesion between the modified surface and the modeling foulant lysozyme. All atomistic MD simulations reveal that the loop-like zwitterionic peptides are more rigid than the linear-like zwitterionic peptides and avoid the penetration of the terminus into the foulants, which lower the interaction between the zwitterionic peptides and foulants. Besides, the loop-like zwitterionic peptides avoid the aggregation of the chains and bind more water, improving the hydrophilicity and antifouling performance. Altogether, this study provides a more comprehensive understanding of the conformation effect of zwitterionic peptides on their antifouling properties, which may contribute to designing novel antifouling materials in various biomedical applications.

Effects of Crystallite Sizes of Pt/HZSM-5 Zeolite Catalysts on the Hydrodeoxygenation of Guaiacol.

Herein, Pt/HZSM-5 zeolite catalysts with different crystallite sizes ranging from nanosheet (~2 nm) to bulk crystals (~1.5 µm) have been prepared for the hydrodeoxygenation of guaiacol, and their effects on the reaction pathway and product selectivity were explored. HZSM-5 zeolites prepared by seeding (Pt/Z-40: ~40 nm) or templating (Pt/NS-2: ~2 nm) fabricated intra-crystalline mesopores and thus enhanced the reaction rate by promoting the diffusion of various molecules, especially the bulky ones such as guaiacol and 2-methoxycyclohexanol, leading to a higher cyclohexane selectivity of up to 80 wt % (both for Pt/Z-40 and Pt/NS-2) compared to 70 wt % for bulky HZSM-5 (Pt/CZ: ~1.5 µm) at 250 °C and 120 min. Furthermore, decreased crystallite sizes more effectively promoted the dispersion of Pt particles than bulky HZSM-5 (Pt/Z-400: ~400 nm and Pt/CZ). The relatively low distance between Pt and acidic sites on the Pt/Z-40 catalyst enhanced the metal/support interaction and induced the reaction between the guaiacol molecules adsorbed on the acidic sites and the metal-activated hydrogen species, which was found more favorable for deoxygenation than for hydrogenation of oxygen-containing molecules. In addition, Pt/NS-2 catalyst with a highly exposed surface facilitated more diverse reaction pathways such as alkyl transfer and isomerization.

Nontoxic Black Phosphorus Quantum Dots Inhibit Insulin Amyloid Fibrillation at an Ultralow Concentration.

Amyloid are protein aggregates formed by cross ß structures assemblies. Inhibiting amyloid aggregation or facilitating its disassembly are considered to be two major effective therapeutic strategies in diseases involving peptide or protein fibrillation such Alzheimer's disease or diabetes. Using thioflavin-T fluorescence, far-UV circular dichroism spectroscopy, and atomic force microscopy, we found nontoxic and biocompatible black phosphorus quantum dots (BPQDs) appear to have an exceptional capacity to inhibit insulin aggregation and to disassemble formed mature fibrils, even at an ultralow concentration (100 ng/mL). The inhibition of fibrillation persists at all stages of insulin aggregation and increases PC12 cells survival when exposed to amyloid fibrils. Molecular dynamics simulations suggest that BPQDs are able to stabilize the α-helix structure of insulin and obliterate the ß-sheet structure to promote the fibril formation. These characteristics make BPQDs be promising candidate in preventing amyloidosis, disease treatment, as well as in the storage and processing of insulin.

Three-dimensional printing of black phosphorous/polypyrrole electrode for energy storage using thermoresponsive ink.

Three-dimensional (3D) printing techniques bring the possibility of making electronic devices in any desired shape and dimensions. Here, we report on a printable black phosphorous nanosheet/polypyrrole composite ink for constructing a high-performance supercapacitor (SC) electrode. The printed BPNS/PPy electrode shows a good energy storage performance with a specific capacitance of up to 417 F g-1 and an excellent cycling stability.

Synergy between Zwitterionic Polymers and Hyaluronic Acid Enhances Antifouling Performance.

Challenges associated with nonspecific adsorption of proteins on sensor surfaces have steered the development of novel antifouling materials and strategies. Inspired by human synovial fluid composition and structure, we designed synergistic antifouling coatings with mixtures of hyaluronic acid (HA) and a zwitterionic bottlebrush polymer (BB). Using a fast and convenient online surface modification method, the polymers were immobilized on the Au surface, significantly increasing its hydrophilicity. Using surface plasmon resonance (SPR), a 10:1 ratio of HA to BB was found optimal to provide the best antifouling performance. Bovine serum albumin (BSA) adsorption on HA-BB coated surfaces was 0.2 ng/cm2, which was 60 times lower than BB or HA alone and 25 times lower than the commonly accepted ultralow adsorption limit (<5 ng/cm2), demonstrating the synergistic effect of HA and BB against nonspecific protein adsorption. This was found to be independent of BSA concentration up to physiological concentrations. Furthermore, the antifouling performance of HA-BB coated surfaces was tested against milk and serum, showing almost 92% lower protein adsorption than that on bare surfaces, suggesting the potential efficacy of this antifouling coating in real life settings.

Sequential sandwich immunoassay for simultaneous detection in trace samples using single-channel surface plasmon resonance.

To analyze multiple analytes in trace samples, low-dosage and high efficiency are crucial in many common cases. Herein, we developed a facile method using a single-channel surface plasmon resonance (SPR)-based biosensor for the simultaneous detection of gentamicin (GEN) and melamine (MEL) in milk and serum with only one sample injection. Based on a sandwich immunoassay, non-interfering antibodies against GEN from mouse (AbGEN) and against MEL from rabbit (AbMEL) were chosen to capture the analytes. Secondary antibodies against mouse (AbM) and rabbit (AbR) were used to bind with AbGEN and AbMEL to determine the concentrations of GEN and MEL on a single channel of an SPR sensor. All of the detection process could be done in 10 min with 50 µL of sample injection. According to the response shifts of AbM and AbR, two standard curves for GEN and MEL were obtained successively, with the limit of detection (LOD) values at 4.4 ng mL-1 and 1.3 ng mL-1, respectively. Moreover, the feasibility was determined by spiking milk and serum samples with GEN and MEL, with recoveries in the range of 81.6%-118.0%. Importantly, the analytes can be substituted by others for much more applications. This method is also expected to multiply the detection efficiency of multi-channel SPR biosensors with low-dosage samples in the future.

Biomimetic Bottlebrush Polymer Coatings for Fabrication of Ultralow Fouling Surfaces.

Demand for long-lasting antifouling surfaces has steered the development of accessible, novel, biocompatible and environmentally friendly materials. Inspired by lubricin (LUB), a component of mammalian synovial fluid with excellent antifouling properties, three block polymers offering stability, efficacy, and ease of use were designed. The bottlebrush-structured polymers adsorbed strongly on silica surfaces in less than 10 minutes by a simple drop casting or online exposure method and were extremely stable in high-salinity solutions and across a wide pH range. Antifouling properties against proteins and bacteria were evaluated with different techniques and ultralow fouling properties demonstrated. With serum albumin and lysozyme adsorption <0.2 ng cm-2 , the polymers were 50 and 25 times more effective than LUB and known ultralow fouling coatings. The antifouling properties were also tested under MPa compression pressures by direct force measurements using surface forces apparatus. The findings suggest that these polymers are among the most robust and efficient antifouling agents currently known.

Adsorption-Desorption Behavior of Black Phosphorus Quantum Dots on Mucin Surface.

Black phosphorus quantum dots (BPQDs) as novel nanomaterials have many potential applications in biomedicine. However, the interaction of BPQDs with proteins and their biological effects and potential risks are still unclear. Here, mucin, which serves biologically as a physical barrier against foreign substances entering tissues, was chosen as a model substrate for studying the adsorption-desorption behavior of BPQDs using surface plasmon resonance sensing and a quartz crystal microbalance with dissipation monitoring. We found that the surface modification of BPQDs with poly(ethylene glycol)-amine (PEG-NH2) reduces the adsorption rate of the quantum dots but increases their adsorbed amount on the mucin surface. The pH value, ionic strength, and ionic valence also had significant effects on the adsorption behavior of BPQDs. Upon increasing the pH from 2 to 7, the amount of BPQD adsorption decreased from 14.1 to 3.2 ng/cm2. A high ionic strength and ionic valence (e.g., Mg2+, Al3+) also inhibit the surface adsorption of BPQDs. Furthermore, the adsorption-desorption mechanisms of BPQDs on the mucin surface were proposed. The adsorption-desorption behavior under different conditions may be attributed to the steric hindrance of PEG, the electrostatic interaction, and/or charge screening. These findings provide useful insights into the interfacial behavior of BPQDs before they enter the tissues.

Design of elution strategy for simultaneous detection of chloramphenicol and gentamicin in complex samples using surface plasmon resonance.

For the analysis of massive samples containing multiple analytes, the enhancement of detection efficiency is crucial. In this study, a facile method was developed for sequential detection of chloramphenicol (CAP) and gentamicin (GEN) in complex samples, e.g. milk, using a surface plasmon resonance (SPR)-based biosensor. Based on the immune inhibition format, two conjugates of antigen and bovine serum albumin (BSA)-denoted as CAP-BSA and GEN-BSA-were grafted on the same channel of the SPR sensor chip. Two standard curves for CAP and GEN were separately obtained by first mixing a single antibody with different concentrations of the relevant antigen. Moreover, different regeneration solutions were screened for sequential analysis. An alkaline solution was found to completely remove the antibody against GEN (AbGEN) from the chip, but it exhibited limited ability to dissociate the antibody against CAP (AbCAP). Therefore, alkaline solution and Gly-HCl solutions are successively applied to elute AbGEN and AbCAP, respectively. By gradual elutions, CAP and GEN concentrations were simultaneously calculated with limit of detection values of 5.28ng/mL and 2.26ng/mL, respectively. Furthermore, the spiking milk samples with CAP and GEN validated the assay with recoveries of 77.6-101.1%. Therefore, this method is expected to improve the detection efficiency of SPR biosensors.

A Review of Methods for Detecting Melamine in Food Samples.

Melamine is a synthetic chemical used in the manufacture of resins, pigments, and superplasticizers. Human beings can be exposed to melamine through various sources such as migration from related products into foods, pesticide contamination, and illegal addition to foods. Toxicity studies suggest that prolonged consumption of melamine could lead to the formation of kidney stones or even death. Therefore, reliable and accurate detection methods are essential to prevent human exposure to melamine. Sample preparation is of critical importance, since it could directly affect the performance of analytical methods. Some methods for the detection of melamine include instrumental analysis, immunoassays, and sensor methods. In this paper, we have summarized the state-of-the-art methods used for food sample preparation as well as the various detection techniques available for melamine. Combinations of multiple techniques and new materials used in the detection of melamine have also been reviewed. Finally, future perspectives on the applications of microfluidic devices have also been provided.

Dopamine-assisted deposition and zwitteration of hyaluronic acid for the nanoscale fabrication of low-fouling surfaces.

In this study, we proposed a bioinspired approach for the deposition and zwitteration of hyaluronic acid (HA) with a reduced glutathione (GSH) to form a composite layer that functions as a low fouling coating. A polyanion of the HA-dopamine conjugate (HADA) possessing catechol groups was synthesized by carbodiimide chemistry between HA and dopamine. Then, the dopamine conjugated biofunctional polymers (HADA) were grafted onto Au substrates via the transformation of catechol into a quinone group under mild oxidative conditions followed by a reaction with GSH to avoid undesired adhesion and also to shield the exposed Au substrate. Analysis of XPS spectra and wettability indicated that HADA and GSH were successfully grafted onto Au substrates. Surface plasmon resonance analysis showed that both HADA and further GSH modified surfaces exhibited reduced nonspecific adsorption. The attachment of GSH to HADA modified surfaces (HADA-G) resulted in better antifouling performance, with a low or ultralow protein adsorption of 0-7.51 ng cm-2 when exposed to single protein solutions, and a reduction in nonspecific adsorption from cow's milk to 10% compared to that of bare gold. The enhanced antifouling performance of HADA-G modified surfaces was likely due to the zwitterionic structure in GSH, which can induce stronger surface hydration through electrostatic interactions as well as the hydrogen bonding induced by HADA. Our results provide a facile and universal approach to surface modification and demonstrate the benefits of using a composite layer for the design of low fouling surfaces.

Development of a surface plasmon resonance immunosensor for detecting melamine in milk products and pet foods.

A sensitive and stable surface plasmon resonance (SPR) immunosensor based on the inhibition format was developed and validated for detecting melamine (MEL) in milk products and pet foods. The sensitivity and the limit of detection (LOD) of the proposed method for MEL were 2.32 × 10(-2) and 1.4 × 10(-3) µg/mL, respectively. The immunosensor was highly specific to MEL, which displayed only low cross-reactivity (CR) (<0.01%) for cyanuric acid, cyanuric chloride, and atrazine. The assay was validated for the detection of MEL in full-cream milk, skim milk powder, infant formula, dog food, and cat food. Most of the recovery results ranged between 76 and 115%. The sensitivities of the assay in each type of sample were 2.57 × 10(-2) µg/mL, 2.32 × 10(-2) µg/kg, 2.51 × 10(-2) µg/kg, 2.66 × 10(-2) µg/kg, and 2.68 × 10(-2) µg/kg, respectively, which were much lower than the maximum residue levels (MRLs) of MEL.