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Wearable biosensors for real-time and non-invasive detection of biomarkers are of importance in early diagnosis and treatment of diseases. Herein, a high-performance wearable biosensing platform was proposed by combining a three-dimensional hierarchical porous Au hydrogel-enzyme electrode with high biocompatibility, activity, and flexibility and soft-MEMS technologies with high precision and capability of mass production. Using glucose oxidase as the model enzyme, the glucose sensor exhibits a sensitivity of 10.51 μA mM-1 cm-2, a long durability over 15 days, and a good selectivity. Under the mechanical deformation (0 to 90°), it is able to maintain an almost constant performance with a low deviation of

Wearable biosensors as a user-friendly measurement platform have become a rapidly growing field of interests due to their possibility in integrating traditional medical diagnostics and healthcare management into miniature lab-on-body analytic devices. This paper demonstrates a flexible and skin-mounted band that combines superhydrophobic-superhydrophilic microarrays with nanodendritic colorimetric biosensors toward in situ sweat sampling and analysis. Particularly, on the superwettable bands, the superhydrophobic background could confine microdroplets into superhydrophilic microwells. On-body investigations further reveal that the secreted sweat is repelled by the superhydrophobic silica coating and precisely collected and sampled onto the superhydrophilic micropatterns with negligible lateral spreading, which provides an independent “vessel” toward cellphone-based sweat biodetection (pH, chloride, glucose and calcium). Such wearable, superwettable band-based biosensors with improved interface controllability could significantly enhance epidemical sweat sampling in well-defined sites, holding a great promise for facile and noninvasive biofluids analysis.

Bioinspired superwettable micropatterns that combine superhydrophobicity and superhydrophilicity have been proved to exhibit outstanding capacity in controlling and patterning microdroplets and possessed new functionalities and possibilities in emerging sensing applications. Here, we introduce a flexible tape-based superhydrophilic-superhydrophobic tape toward on-site heavy metals monitoring. On such a superwettable tape, capillarity-assisted superhydrophilic microwells allow directly anchoring indicators in fixed locations and sampling into a test zone via simple dip-pull from an origin specimen solution. In contrast, the superhydrophobic substrate could confine the microdroplets in the superhydrophilic microwells for reducing the amount of analytical solution. The tape-based microchip also displays excellent flexibility against stretching, bending, and torquing for expanding wearable and portable sensing devices. Qualitative and quantitative colorimetric assessments of multiplex heavy metal analyses (chromium, copper, and nickel) by the naked eye are also achieved. The superwettable tape-based platforms with a facile operation mode and accessible signal read-out represent unrevealed potential for on-site environmental monitoring.

In recent years, delivery systems based on the incorporation of thiols/disulfides have been extensively explored to promote the intracellular delivery of biological cargoes. However, it remains unclear about the detailed processes of thiol-disulfide exchanges taking place on the cell surface and how the exchange reactions promote the cellular uptake of cargoes bearing thiols or disulfide bonds. In this work, we report the rational design of biscysteine motif-containing peptide probes with substantially different ring-closing property and how these peptide probes were employed to explore the thiol-disulfide exchanges on the cell surface. Our results show that extensive thiol-disulfide exchanges between peptides and exofacial protein thiols/disulfides are involved in the cellular uptake of these peptide probes, and importantly glutathione (GSH) exported from the cytosols participates extensively in the exchange reactions. Cysteine-glycine-cysteine (CGC)-containing peptide probes can be more efficiently taken up by cells compared to other probes, and we suggested that the driving force for the superior cellular uptake arises from very likely the unique propensity of the CGC motif in forming doubly bridged disulfide bonds with exofacial proteins. Our probe-based strategy provides firsthand information on the detailed processes of the exchange reactions, which would be of great benefit to the development of delivery systems based on the extracellular thiol-disulfide exchanges for intracellular delivery of biologics.

Rapid detection of ultratrace pollutants in complex matrixes is a great challenge for studying their environmental behaviors and impacts. In this work, a method is developed by combining covalent organic framework (COF) based solid phase microextraction (SPME) with constant flow desorption ionization mass spectrometry for rapid detection of trace tetrabromobisphenol A (TBBPA) in multiple water media. The limits of detection and qualification are 0.92 and 3.1 ng L–1 for TBBPA, respectively. The linear range is between 0.01 and 10 μg L–1 (R2 = 0.9992), and the relative standard deviations with single fiber and multiple fibers are 6.4% and 6.7% (0.1 μg L–1, n = 9), respectively. The detection of nanogram per liter levels of TBBPA in tap water, river water, seawater, and beverage can be achieved in 7 min.

Intracellular H2O2 plays an important role in regulating a variety of cellular functions. Fluorescent probes that can make response to intracellular levels of H2O2 would provide valuable tools for revealing the functions of H2O2 in living organisms. However, traditional pH-insensitive probes and lysosome-targetable probes can only provide spatially nonspecific visualization of intracellular H2O2 and specific sensing of lysosomal H2O2, respectively. In this work, we developed a H2O2-responsive and pH-switchable fluorescent probe (HP-L1) which can make response sequentially to intracellular H2O2 and lysosomal pH. The fluorescent probe is comprised of a H2O2-responsive boronate moiety and a pH-switchable spirobenzopyran fluorophore. When the probe was applied for intracellular H2O2 sensing, only fluorescent emission from lysosomes is visible, and the fluorescence from other regions is not able to be obviously detected, which is due to the pH-switchable property of the spirobenzopyran fluorophore. Thus, the developed fluorescence probe enables the spatially confined (i.e., lysosome-specific) visualization of the intracellular H2O2. We envisioned that this kind of fluorescent probe (or the proposed sensing strategy) would allow the visualization of the overall levels of intracellular H2O2 without interferences of possible fluorescent signals from other sources (e.g., dyes for cellular staining and multiplex analysis).

Study on the processes of the thiol-mediated disulfide exchange reactions on the cell surface is not only important to our understanding of extracellular natural bioreduction processes but to the development of novel strategies for the intracellular delivery of synthetic bioactive molecules. However, disulfide-bonded probes have their intrinsic inferiority in exploring the detailed exchange pathway because of the bidirectional reactivity of disulfide bonds toward reactive thiols. In this work, we developed thioether-bonded fluorescent probes that enable us to explore thiol-mediated thioether (and disulfide) exchange reactions on the cell surface through fluorescence recovery and/or cell imaging. We demonstrated that our thioether-bonded probes can be efficiently cleaved through thiol-thioether exchanges with exofacial protein thiols and/or glutathione (GSH) efflux. The exchanges mainly take place on the cell surface, and GSH efflux-mediated exchange reactions can take place without the requirement of pre-exchanges of the probes with cell surface-associated protein thiols. On the basis of our founder methodology, for the first time we demonstrated the interplay of exofacial protein thiols and GSH efflux on the cleavage of external thioether-bonded compounds. Moreover, given that an understanding of the process of GSH efflux and the mechanism on which it relies is crucial to our understanding of the cellular redox homeostasis and the mechanism of multidrug resistance, we expect that our thioether-bonded probes and strategies would greatly benefit the fundamental study of GSH efflux in living cells.

We describe and illustrate a three-step data-processing approach that enables individual congener groups of chlorinated paraffins (CPs) to be resolved in mass spectra obtained from either of two soft ionization methods: electron capture negative ionization mass spectrometry (ECNI-MS) or atmospheric pressure chemical ionization mass spectrometry (APCI-MS). In the first step, general fragmentation pathways of CPs are deduced from analysis of mass spectra of individual CP congeners. In the second step, all possible fragment ions in the general fragmentation pathways of CPs with 10 to 20 carbon atoms are enumerated and compared to mass spectra of CP mixture standards, and a deconvolution algorithm is applied to identify fragment ions that are actually observed. In the third step, isotope permutations of the observed fragment ions are calculated and used to identify isobaric overlaps, so that mass intensities of individual CP congener groups can be deconvolved from the unresolved isobaric ion signal intensities in mass spectra. For a specific instrument, the three steps only need to be done once to enable deconvolution of CPs in unknown samples. This approach enables congener group-level resolution of CP mixtures in environmental samples, and it opens up the possibility for quantification of congener groups.