This work reports a contactless photoelectrochemical biosensor based on an ultraviolet-assisted gas sensor (UV–AGS) with a homemade three-dimensional (3D)-SnS2 nanosheet-functionalized interdigitated ...electrode. After rigorous examination, it was found that the gas responsiveness accelerated and the sensitivity increased using the UV irradiation strategy. The effects of the interlayer structure and the Schottky heterojunction on the gas-sensitive response of O2 and NH3 under UV irradiation were further investigated theoretically by 3D electrostatic field simulations and first-principles density functional theory to reveal the mechanism. Finally, a UV–AGS device was developed to quantify the blood ammonia bioassay in a small-volume whole blood sample by alkalizing blood to release gas-phase ammonia with a linear range of 25–5000 μM with a limit of detection (LOD) of 29.5 μM. The device also enables a rapid immunoassay of human cardiac troponin I (cTnI) with a linear range of 0.4–25.6 ng/mL and an LOD of 0.37 ng/mL using a urease-labeled antibody as the immune recognition molecule. Both analyses showed satisfying specificity and stability, suggesting that the device can be applied to practical assays and is of great potential to increase the value of gas-sensitive sensors in chemical biosensing.
A paper-based visual fluorescence immunoassay is presented for the detection of matrix metalloproteinase-7 (MMP7) that is related to renal cancer. The method is based on the distance-dependent ...fluorescence quenching of CdTe quantum dots (QDs) on a nitrocellulose membrane by Ag
+
following a sandwich-type immunoreaction on microtiter wells using silver nanoparticle (AgNP)–labeled secondary antibody– and primary antibody–coated microtiter wells. The silver nanoparticles captured in the well are dissolved with HNO
3
, while the quenching effect of QDs is based on silver ion-exchange reaction under 365-nm excitation light irradiation. Increasing concentration of released Ag
+
, thus higher concentration of the protein, leads to an increased distance of quenching on the nitrocellulose membrane. The paper-based immunoassay by combination of AgNP-assisted ion-exchange reaction with QD gives good distance-dependent responses and allows the detection of MMP7 at a concentration as low as 7.3 pg mL
−1
. The coefficients of variation are less than 6.9% and 12.4% for intra-assay and inter-assay, respectively. High specificity and long-term stability are achieved during the assay. Importantly, the testing of human serum samples using our strategy shows well-matched results with commercial human MMP7 ELISA kits.
Graphical abstract
A distance-dependent visual immunoassay is developed for the determination of serum matrix metalloproteinase-7 on CdTe quantum dot–impregnated paper with silver ion-exchange reaction.
Dysbiosis of human gut microbiota is associated with a wide range of metabolic disorders, including gestational diabetes mellitus (GDM). Yet whether gut microbiota dysbiosis participates in the ...etiology of GDM remains largely unknown.
Our study was initiated to determine whether the alternations in gut microbial composition during early pregnancy linked to the later development of GDM, and explore the feasibility of microbial biomarkers for the early prediction of GDM.
This nested case-control study was based upon an early pregnancy follow-up cohort (ChiCTR1900020652). Gut microbiota profiles of 98 subjects with GDM and 98 matched healthy controls during the early pregnancy (10-15 weeks) were assessed via 16S rRNA gene amplicon sequencing of V4 region. The data set was randomly split into a discovery set and a validation set, the former was used to analyze the differences between GDM cases and controls in gut microbial composition and functional annotation, and to establish an early identification model of GDM, then the performance of the model was verified by the external validation set.
Bioinformatic analyses revealed changes to gut microbial composition with significant differences in relative abundance between the groups. Specifically,
, and
were enriched in the GDM group, whereas
group, etc. remained dominant in the controls. Correlation analysis revealed that GDM-enriched genera
and
were positively correlated with fasting blood glucose levels, while three control-enriched genera (
, and
) were the opposite. Further, GDM functional annotation modules revealed enrichment of modules for sphingolipid metabolism, starch and sucrose metabolism, etc., while lysine biosynthesis and nitrogen metabolism were reduced. Finally, five genera and two clinical indices were included in the linear discriminant analysis model for the prediction of GDM; the areas under receiver operating characteristic curves of the training and validation sets were 0.736 (95% confidence interval: 0.663-0.808) and 0.696 (0.575-0.818), respectively.
Gut bacterial dysbiosis in early pregnancy was found to be associated with the later development of GDM, and gut microbiota-targeted biomarkers might be utilized as potential predictors of GDM.
A self-powered temperature sensor based on Seebeck effect transduction was designed for photothermal–thermoelectric coupled immunoassay of α-fetoprotein (AFP). In this system, glucose oxidase ...(GOx)-conjugated detection antibody was first captured onto the microplate by target-induced sandwich-type immunoreaction. Thereafter, the as-generated hydrogen peroxide via the GOx–glucose system oxidized 3,3′,5,5′-tetrametylbenzidine (TMB) into photothermal product oxidized TMB (ox-TMB). Under near-infrared (NIR) laser irradiation, the temperature change of ox-TMB was read out in an electrical signal by the flexible thermoelectric module in a 3D-printed integrated detection device. Under optimal conditions, the photothermal–thermoelectric coupled immunoassay exhibited a limit of detection of 0.39 ng mL–1 AFP over a dynamic linear range from 0.5 to 60 ng mL–1. Impressively, such a strategy presented herein offers tremendous potentials for applying many other high-efficiency thermoelectric materials in ultrasensitive biosensors.
Accurate identification of acutely toxic and low-fatality mycotoxins on a large scale in a quick and cheap manner is critical for reducing population mortality. Herein, a portable photothermal ...immunosensing platform supported by a microelectromechanical microsystem (MEMS) without enzyme involvement was reported for point-of-care testing of mycotoxins (in the case of aflatoxin B
, AFB
) in food based on the precise satellite structure of Au nanoparticles. The synthesized Au nanoparticles with a well-defined, graded satellite structure exhibited a significantly enhanced photothermal response and were coupled by AFB
antibodies to form signal conversion probes by physisorption for further target-promoted competitive responses in microplates. In addition, a coin-sized miniature NIR camera device was constructed for temperature acquisition during target testing based on advanced MEMS fabrication technology to address the limitation of expensive signal acquisition components of current photothermal sensors. The proposed MEMS readout-based microphotothermal test method provides excellent AFB
response in the range of 0.5-500 ng g
with detection limits as low as 0.27 ng g
. In addition, the main reasons for the efficient photothermal transduction efficiency of Au with different graded structures were analyzed by finite element simulations, providing theoretical guidance for the development of new Au-based photothermal agents. In conclusion, the proposed portable micro-photothermal test system offers great potential for point-of-care diagnostics for residents, which will continue to facilitate immediate food safety identification in resource-limited regions.
A magnetic-assisted photoelectrochemical (PEC) and colorimetric (CL) dual-modal biosensing platform with high precision was established to monitor prostate-specific antigen (PSA) based on Bi2MoO6 ...nanosheets (BMO) by coupling the aptamer-guided hybridization chain reaction (HCR) with the hydrolysate-induced vulcanization reaction of Bi2MoO6 nanosheets. Upon addition of PSA, trigger DNA (tDNA) was released by the interaction between the target analyte and the aptamer and then further hybridized with anchor DNA (aDNA) conjugated on magnetic beads (MBs). The as-released tDNA initiated the target-assisted HCR in the presence of two alternating hairpin sequences (Bio-H1 and Bio-H2) to produce nicked long double-stranded DNA on the surface of MBs, where numerous alkaline phosphatase (ALP) enzymes could assemble with MBs through the biotin–avidin reaction, resulting in the hydrolysis of sodium thiophosphate (TP) to H2S. The as-produced H2S reacted with BMO to form vulcanized BMO (BMO-S), thus leading to obvious enhanced PEC performance under visible light with the color change from light yellow to brown. Having optimized the test conditions, the magnetic-assisted biosensing system holds a good quantitative diagnosis sensitivity area in a range of 5.0 pg mL–1–100 ng mL–1 with a calculated detection limit down to 3.5 pg mL–1. Meanwhile, a visual colorimetric assay on basis of the change in the color of the materials was also realized. Given the exceptional performance of the constructed biosensor, it may possess great promise as an advanced bioanalytical tool for practical applications.
An interdigitated capacitance immunosensing system based enzymatic biocatalytic precipitation on micro-comb electrode was designed for the sensitive detection of prostate-specific antigen (PSA) by ...coupling Ti3C2 MXenes with tyramine signal amplification strategy. The immunosensor was prepared by immobilizing anti-PSA capture antibody on MXenes-coated interdigitated electrode, whereas gold nanoparticles heavily functionalized with horseradish peroxidase (HRP) and detection antibody were utilized as the signal-transducer tags. Introduction of interdigitated electrode was expected to enhance the sensitivity of capacitance immunosensor. This system mainly consisted of the sandwich-type immunoreaction, formation of tyramine-HRP repeats on gold nanoparticle and enzymatic biocatalytic precipitation. The concatenated HRP through the tyramine oxidized numerous 4-chloro-1-naphthol molecules into insoluble benzo-4-chlorohexadienone with the help of H2O2, and coated the modified immunosensor to keep free ions away from the electrode, thus causing the local alteration in the capacitance. Under optimum conditions, the change of the immunosensor in the capacitance increased with the increasing target PSA concentrations from 0.1 ng mL−1 to 50 ng mL−1 at a detection limit of 0.031 ng mL−1. Moreover, the interdigitated capacitance immunosensor showed good reproducibility, high specificity and acceptable accuracy for the analysis of human serum specimens in comparison with those obtained from commercial human PSA ELISA kit. Importantly, Ti3C2 MXenes-based interdigitated capacitance transducer open new opportunities for protein diagnostics and biosecurity.
•A capacitance immunosensor was fabricated for prostate-specific antigen.•Interdigitated micro-comb electrode used for the immobilization of antibody.•Ti3C2 MXenes utilized as the affinity support for biomolecular conjugation.•Enzyme label, nano label and tyramine-enzyme repeats used for the signal amplification.
The point-of-care (POC) method with affordability and portability for the sensitive detection of biological substances is an emerging topic in rapid disease screening and personalized medicine. In ...this work, we demonstrated a diverse responsive platform based on a dual-channel pressure sensor (DCPS). The DCPS had a multilayer flexible architecture consisting of a photonic hydrogel with chromatic transitions and a piezoresistive pressure sensor as the electrical data transmission unit, both of which had the property of pressure-induced mechanical stimulus feedback. By incorporating a platinum nanoparticles-labeled detection antibody (PtNPs-dAb) into the sandwich-type immunoreaction for the target carcinoembryonic antigen (CEA, as a model analyte), gas decomposition could be triggered by the addition of hydrogen peroxide (H2O2) to induce a significant increase under pressure in a closed chamber. Meanwhile, the DCPS enabled an accurate electrical signal output, and the photonic hydrogel converted spatiotemporal stimuli into eye-readable colorations with string brilliance. In this way, the target concentration could be quantificationally related to the electrical response and intuitively perceived through visible color alterations. Under optimal conditions, a sensitive determination of CEA was performed in a detectable range of 0.3–60 ng/mL with a limit of detection (LOD) of 0.13 ng/mL. In addition, the proposed protocol had satisfactory selectivity, accuracy, and reproducibility. Furthermore, an array-based immunoassay device was fabricated to conceptually validate its application potential in high-throughput biomedical detection and inspire a dual-signal POC diagnostic platform in a friendly way for resource-limited settings.
Luminescent carbon nanostructures (CNSs) have attracted great interest from the scientific community due to their photoluminescent properties, structural features, low toxicity, and a great variety ...of possible applications. Unfortunately, a few problems hinder their further development. These include the difficulties of separating a mixture of nanostructures after synthesis and the dependence of their properties on the environment and the aggregate state. The application of a silica matrix to obtain luminescent composite particles minimizes these problems and improves optical properties, reduces photoluminescence quenching, and leads to wider applications. We describe two methods for the formation of silica composites containing CNSs: inclusion of CNSs into silica particles and their grafting onto the silica surface. Moreover, we present approaches to the synthesis of multifunctional particles. They combine the unique properties of silica and fluorescent CNSs, as well as magnetic, photosensitizing, and luminescent properties via the combination of functional nanoparticles such as iron oxide nanoparticles, titanium dioxide nanoparticles, quantum dots (QDs), and gold nanoclusters (AuNCs). Lastly, we discuss the advantages and challenges of these structures and their applications. The novelty of this review involves the detailed description of the approaches for the silica application as a matrix for the CNSs. This will support researchers in solving fundamental and applied problems of this type of carbon-based nanoobjects.