Microfluidic Immunosensing Platform Based on a Rolling Circle Amplification-Assisted DNA Dendrimer Probe for Portable and Sensitive Detection of Allergen-Specific IgE.

The robust point-of-care platform for sensitive, multiplexed, and affordable detection of allergen-specific IgE (sIgE) is an urgent demand in component-resolved diagnostics. Here, we developed a microfluidic immunosensing platform based on a rolling circle amplification-assisted DNA dendrimer probe for sensitive detection of multiple sIgEs. The versatile multichannel microfluidic whole blood analytical device integrates cell filtration, recombinant antigen-modified magnetic enrichment, and DNA dendrimer probe-amplified signal transduction for portable on-chip analysis. Three sIgEs against common oyster allergens were simultaneously detected in blood samples by simple smartphone-based imaging without any pretreatment. The quantitative detection of multiple allergen-specific antibodies on the platform was achieved with limits of detection of less than 50 pg/mL, exhibiting superior sensitivity compared to most point-of-care testing. The detection results of 55 serum samples and 4 whole blood samples were 100% consistent with the ELISA results, confirming the accuracy and stability of our platform. Additionally, the reversible combination of hexahistidine6-tag and Ni-IMAC magbead was elegantly utilized on the immunosensing platform for desired reversibility. With the advantages of general applicability, high sensitivity, and reversibility, the DNA dendrimer-based microfluidic immunosensing platform provides great potential for the portable detection of immune proteins as a point-of-care platform in disease diagnostics and biological analysis.

Light-Driven Photocatalytic-Photothermal Synergetic System for Portable and Sensitive Nucleic Acid Quantification.

Photosensitizers and photothermal agents have attracted increasing attention for in vitro diagnosis, but the combination remains challenging. Herein, a light-driven photocatalytic-photothermal synergetic system integrated microfluidic distance-based analytical device (PCPT-µDAD) for visual, portable, sensitive, and quantitative detection of targets was developed. Target DNA was recognized and initiated the hybridization chain reaction to form a double-stranded DNA/SYBR Green I (dsDNA/SG-I) complex. By applying the photosensitization of the dsDNA/SG-I complex and the photothermal effect of oxidized 3,3',5,5'-tetramethylbenzidine, the target concentration can effectively translate into a visual distance signal readout. Importantly, the light-driven PCPT-µDAD greatly improves the controllability of catalytic reactions and signal amplification efficiency. The light-driven PCPT-µDAD shows a low limit of detection (fM level), good stability, and high reproducibility for nucleic acid detection.

CunO/Au heterostructure dendrimer anchored on Cu foam as dual functional catalytic nanozyme for glucose sensing by enzyme mimic cascade reaction.

Multifunctional catalytic performance plays a crucial role in bio-applications through the diversity and durability of artificial nanozymes. An effective synergy with sufficient accessible active sites and high specific surface area is a challenge for composite catalysts, especially to avoid uncontrollable aggregation and structural instability. Here, we fabricated a CunO/Au heterostructure dendrimer on copper foam (CunO/Au HD/CF) as dual functional catalytic nanozyme to achieve enzyme mimic cascade reactions for efficient colorimetric analysis. A highly porous CF skeleton-based CuO nanowire array (CuO NWA) with a large specific surface area supported an efficient load capacity to assemble sufficient CunO/Au HD by electrodeposition. The bimetallic Au-Cu nanozyme successfully achieved an oxidase-like and peroxidase-like cascade catalysis by a target-responsive sensing mechanism. Due to the confirmed catalytic performance of selectivity, anti-interference ability, and reproducibility, a CunO/Au HD/CF-based quantitative analytical method was developed for glucose detection with a wide linear range and considerable detection limit of 8.4 µM. The robust nonenzymatic catalytic strategy for colorimetric detection not only confirmed the dual functional catalytic activity of CunO/Au HD/CF, but also showed great potential for applications in clinical diagnostics and biochemical analysis.

Corrigendum to "Cobalt metal-organic framework modified carbon cloth/paper hybrid electrochemical button-sensor for nonenzymatic glucose diagnostics" [Sens. Actuators B Chem. 329 (2021) 129205].

[This corrects the article DOI: 10.1016/j.snb.2020.129205.].

Cobalt metal-organic framework modified carbon cloth/paper hybrid electrochemical button-sensor for nonenzymatic glucose diagnostics.

In the growing pandemic, family healthcare is widely concerned with the increase of medical self-diagnosis away from the hospital. A cobalt metal-organic framework modified carbon cloth/paper (Co-MOF/CC/Paper) hybrid button-sensor was developed as a portable, robust, and user-friendly electrochemical analytical chip for nonenzymatic quantitative detection of glucose. Highly integrated electrochemical analytical chip was successfully fabricated with a flexible Co-MOF/CC sensing interface, effectively increasing the specific area and catalytic sites than the traditional plane electrode. Based on the button-sensor, rapid quantitative detection of glucose was achieved in multiple complex bio-matrixes, such as serum, urine, and saliva, with desired selectivity, stability, and durability. With the advantages of low cost, high environment tolerance, ease of production, our nanozyme-based electrochemical analytical chip achieved reliable nonenzymatic electrocatalysis, has great potential for the application of rapid on-site analysis in personalized diagnostic and disease prevention.

Bovine serum albumin-coated titanium dioxide modified electrochemical interface for enantioselective discrimination of D/L-aspartic acid.

Due to the similar physicochemical properties, the discrimination of chiral isomers faces huge challenges in drug production and biochemical analysis. Herein, the bovine serum albumin-coated titanium dioxide (bovine serum albumin [BSA]/TiO2 ) was modified as a novel electrochemical interface for efficient, simple, and enantioselective discrimination of aspartic acid enantiomers (D/L-Asp) based on the electrochemical impedance spectroscopy (EIS). Utilizing the structural characteristics of large cavity and high specific surface area, TiO2 material provided sufficient space for adequate loading of BSA. The BSA/TiO2 electrochemical interface was successfully fabricated to support abundant chiral recognition sites. The enantioselective discrimination of D/L-Asp was achieved on the interface with a good linear relationship against the impedance difference in the concentration range from 1 to 1000 nM with the detection limit of 0.37 nM for L-Asp and 0.94 nM for D-Asp, reaching the identification coefficient (Ic = KL /KD ) of 1.85. The proposed interface is easy to form with a stable formation of BSA in TiO2 microporous architecture, which maintained the desired stability and reproducibility. For the unknown racemic solution, Ic levels of different enantio-ratios of D/L-Asp were effectively obtained to evaluate the chiral percentage of racemic sample. The possible mechanism of chiral recognition by density function theory (DFT) was confirmed with a stronger adsorption to L-Asp in accordance with our experiment results, reinforcing the validity of our presented interface. The BSA/TiO2 electrochemical interface with robust enantioselective discrimination of D/L-Asp has great potential for the practical application in pharmaceutical surveillance and food security.

Differential potential ratiometric sensing platform for enantiorecognition of chiral drugs.

A versatile, robust and efficient differential potential ratiometric sensing platform was developed for enantioselective recognition of dual chiral targets based on a composite membrane of molecularly imprinted polymers (MIPs) and reduced graphene oxide (rGO) modified glassy carbon electrode (GCE). The functional chitosan-based MIPs and rGO were compatibly immobilized on the GCE with high selectivity and efficient signal amplification. Moreover, via the systematic optimization of series conditions, a distinct potential difference (PD), reaching 135 mV, was obtained between the R-/S-prop based on the MIPs/rGO/GCE. In a controllable concentration range from 50 µM to 1000 µM, different ratios of R-/S-prop were linearly related to the peak potentials (Eps) in the racemic mixture. Using this low-cost reversible electrochemical platform, both Prop enantiomers were simultaneously identified with high repeatability and time-based stability. This novel semi-quantitative electrochemical sensing platform was established to rapidly quantify the ratio of S-/R-prop by Ep for the chiral drug recognition with great potential for practical applications in fields of pharmacological detection and clinical analysis.

Sensitive detection of L-5-hydroxytryptophan based on molecularly imprinted polymers with graphene amplification.

A novel electrochemical sensor was presented for the determination of L-5-hydroxytryptophan (L-5-HTP) based on a graphene-chitosan molecularly imprinted film modified on the surface of glassy carbon electrode (GR-MIP/GCE). The morphology and composition of the imprinted film were observed in field emission scanning electron microscopy (FESEM), raman spectroscopy and fourier transform infrared (FTIR). The properties of the sensor were evaluated by electrochemical techniques. Under the optimal conditions, the peak currents of L-5-HIP were found to be linear in the concentration range of 0.05-7.0 µM, while the sensor also exhibited great features such as low detection limit of 6.0 nM (S/N = 3), superb selectivity against the structural analogues, good antidisturbance ability among coexisting components, excellent repeatability and stability. Moreover, the proposed method had been applied to the detection of L-5-HTP in human blood serum with a satisfactory recoveries ranging from 90.6% to 105.6%.

Xanthine microsensor based on polypyrrole molecularly imprinted film modified carbon fiber microelectrodes.

A molecularly imprinted polymers (MIPs) microsensor was presented as a carbon fiber microelectrode (CFME) coating for specifically recognizing xanthine (Xan). The polymeric film was obtained based on the imprinted procedure of electropolymerization of pyrrole in the presence of the template molecule Xan by cyclic voltammetry, and template was removed by magnetic stirring. Under the optimum conditions, a satisfactory molecularly binding selectivity of Xan was obtained from the MIPs microsensor with an imprinting factor (IF) of 6.63 and a linear response to concentration in certain ranges. The ranges are from 4.0 × 10⁻6 to 6.0 × 10⁻5 M and from 8.0 × 10⁻5 to 2.0 × 10⁻³ M with a detection limit of 2.5 × 10⁻7 M. Meanwhile, good stability (relative standard deviation [RSD] = 3.2%, n = 10) and reproducibility (RSD = 2.0%, n = 10) were observed, and recoveries ranging from 96.9 to 102.5% were calculated when applied to Xan determination in real blood serum samples.

Carbon dot/Co-MOF nanocoral mediated fluorescence-scattering ratiometric sensor for highly sensitive detection of alkaline phosphatase.

Abnormal expression of alkaline phosphatase (ALP) in serum has received considerable attention in health monitoring and disease diagnosis. However, conventional optical analysis based on a single signal must compromise background interference and limited sensitivity in trace analysis. As an alternative candidate, the ratiometric approach depends on the self-calibration of two independent signals in a single test to minimize interferences from the background for accurate identification. Here, a carbon dot/cobalt-metal organic framework nanocoral (CD/Co-MOF NC) mediated fluorescence-scattering ratiometric sensor has been developed for simple, stable, and highly sensitive detection of ALP. ALP-responsive phosphate production was used to coordinate cobalt ion and collapse the CD/Co-MOF NC, resulting in the recovery of fluorescence signal from dissociative CDs and the decrease of second-order scattering (SOS) signal from the cracked CD/Co-MOF NC. The ligand-substituted reaction and the optical ratiometric signal transduction provide a rapid and reliable chemical sensing mechanism. The ratiometric sensor effectively converted ALP into a ratio signal of fluorescence-scattering dual emission throughout a wide linear concentration range of six orders of magnitude with a detection limit of 0.6 mU/L. In addition, self-calibration of fluorescence-scattering ratiometric method can reduce background interference and improve sensitivity in serum, approaching recoveries of ALP from 98.4% to 101.8%. Due to the above advantages, the CD/Co-MOF NC mediated fluorescence-scattering ratiometric sensor readily provides rapid and stable quantitative detection of ALP as a promising in vitro analytical method for clinical diagnostics.

A urea electrochemical sensor based on molecularly imprinted chitosan film doping with CdS quantum dots.

An improved imprinted film-based electrochemical sensor for urea recognition was developed using CdS quantum dots (QDs) doped chitosan as the functional matrix. The microstructure and composition of the imprinted films depicted by scanning electron microscopy (SEM), attenuated total reflection infrared (ATR-IR), X-ray diffraction (XRD), and electrochemical impedance spectroscopy (EIS) indicated the fabricated feasibility of the nanoparticle doped films via in situ electrodeposition. Differential pulse voltammetric responses under the optimal fabrication conditions showed that the sensitivity of CdS QDs-MIP (molecularly imprinted polymer) electrochemical sensor was enhanced from the favorable electron transfer and magnified surface area of CdS QDs with a short adsorption equilibrium time (7 min), wide linear range (5.0 × 10(-12) to 4.0 × 10(-10) M and 5.0 × 10(-10) to 7.0 × 10(-8) M), and low detection limit (1.0 × 10(-12) M). Meanwhile, the fabricated sensor showed excellent specific recognition to template molecule among the structural similarities and coexistence substances. Furthermore, the proposed sensor was applied to determine the urea in human blood serum samples based on its good reproducibility and stability, and the acceptable recovery implied its feasibility for practical application.

Gold nanodendrite-based differential potential ratiometric sensing strategy for enantioselective recognition of DOPA.

Numerous chiral drugs have been developed for neurological diseases, but chiral drug safety and pharmacological research still faces great challenges in enantioselectivity and sensitivity of chiral analysis. A rapid, stable and high-efficiency gold nanodendrite-based electrochemical sensing method was proposed as a versatile differential potential ratiometric strategy for highly selective chiral recognition of dual 3,4-dihydroxyphenylalanine (DOPA) enantiomers. Using simple electrochemical deposition, the gold nanodendrite (AuND) membrane was steadily modified on the glassy carbon electrode (GCE) with high specific chiral identifiability and robust signal amplifiability. Based on a sequence of systematic optimization, an apparent potential difference (PD) was detected up to 108 mV from oxidation peaks of DOPA enantiomers. Furthermore, according to a regulatable concentration range from 10 µM to 100 µM, different proportions of L-/d-DOPA had a good linear relationship with corresponding peak potentials (Eps) in the racemic mixture. Superior to traditional enantiorecognition of single chiral drug, both DOPA enantiomers enabled to be simultaneously distinguished with high repeatability, selectivity, and anti-interference ability on the AuND/GCE. This unique semi-quantitative AuND-based potential sensing strategy was proposed to efficiently quantify the proportion of L-/d-DOPA for chiral drug recognition, emerging positive potential for numerous applications in pharmacology and clinical diagnosis.