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This study reports a photoelectrochemical biosensor for dopamine-loaded liposome-encoded magnetic beads cleaved by clustered regularly interspaced short palindromic repeats (CRISPR)/Cas 12a system for the quantification of human papilloma virus (HPV)-related DNA using neodymium-doped BiOBr nanosheets (Nd-BiOBr) as a photoactive matrix. Magnetic beads and dopamine-loaded liposomes are covalently attached to the both ends of ssDNA to construct dumbbell-shaped dopamine-loaded liposome-encoded magnetic bead (DLL-MB) probes. When the guide RNA binds to the target HPV-16, the ssDNA will be cleaved by Cas12a, thereby degrading the double dumbbell probes. After magnetic separation, the dissolved DLLs are treated with Triton X-100 to release the dopamine (as an electron donor), which was then detected by an amplified photocurrent using the Nd-BiOBr-based photoelectrode.

This work reports on the proof-of-concept of a photoelectrochemical (PEC) biosensor with a horseradish peroxidase-single stranded DNA-encoded magnetic bead (MB-ssDNA-HRP) signal probe cleaved by the catalytic hairpin assembly (CHA)-mediated clustered regularly interspaced short palindromic repeats (CRISPR)-Cas12a system for the quantification of microRNA (miR-21) by using yolk-in-shell Au@CdS as a photoactive material.

In this work, a split-type dual-mode (colorimetric/photothermal) immunoassay method was designed for point-of-care testing (POCT) detection of mycotoxins (aflatoxin B

Acute myocardial infarction (AMI) survivors face a high risk of mortality as a result of increasing heart failure and irreparable myocardial injury. New portable methods for immediate diagnosis must be developed to provide patients with daily warnings. Herein, the development of a dual-mode photothermal-pyroelectric output system based on a point-of-care platform for rapid AMI detection is reported. Termed as Integrated Photothermal-Pyroelectric Biosensor for AMI (IPPBA), the method leverages cascade enzymatic amplification to convert the target signal into a thermal and pyrooelectric conversion of the testing process by delicate pyroelectric pervokite NaNbO

This work presented a point-of-care (POC) photoelectrochemical (PEC) biosensing for the detection of human papillomavirus-16 (HPV-16) on a portable electrochemical detection system by using CRISPR-Cas12a trans-cleaving the G-quadruplex for the biorecognition/amplification and a hollow In

Functional photothermal nanomaterials have gained widespread attention in the field of precise cancer therapy and early disease diagnosis due to their unique photothermal conversion properties. However, the relatively narrow temperature response range and the outputable accuracy of commercial thermometers limit the accurate detection of biomarkers. Herein, we designed a liposome-embedded Cu

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.

This work describes a novel and portable pressure-based point-of-care (POC) testing strategy for the sensitive and rapid detection of carcinoembryonic antigen (CEA) via a flexible pressure sensor constructed by three-dimensional (3D) polypyrrole (PPy) foam. Initially, platinum nanoparticles (PtNPs) were conjugated to the detection antibodies, which were used to form sandwich-type immunocomplexes with targets and capture antibodies in the reaction cell. Then, the carried PtNPs catalyzed the dissociation of hydrogen peroxide (H2O2) for the generation of oxygen (O2) in a sealed device, translating the biomolecule recognition event into gas pressure. With the increase of pressure, a flexible pressure sensor with 3D polypyrrole foam as the sensing layer was used to sensitively monitor the pressure variations in this system. Thus, the concentration of the target could be quantitatively determined by the pressure response. Under optimal conditions, the pressure-based immunosensor showed good sensing performance for CEA in the dynamic working range from 0.2 to 60 ng/mL with a detection limit of 0.13 ng/mL. The reproducibility, specificity, and accuracy compared with commercial enzyme-linked immunosorbent assay (ELISA) kit were also acceptable. Therefore, this work provides a promising approach for developing portable and sensitive POC testing in the future.

Organophosphorus pesticides (OPs) are extensively used worldwide as agrochemicals; however, excess use may threaten the health of humans. Thus, it is an urgent need to develop a sensitive method for determination of OPs. Herein, a simple and sensitive split-type electrochemical method was developed by using MnO2 nanoflower-electron mediator as a signal transduction element. The MnO2 nanoflower-electron mediator was synthesized and shows an excellent electrochemical signal attributed to the high specific surface area of MnO2 nanoflower. Meanwhile, the inhibition of OPs on butyrylcholinesterase (BChE) was carried out in the homogeneous system. In the absence of target molecule, a large number of thiocholines (TCh) were yielded from hydrolysis of acetylthiocholine (ATCh) by BChE. The MnO2 nanoflower was cracked, and subsequently, multiple electron mediator molecules were released from the platform after treated with TCh, thus decreasing the electrochemical response. Furthermore, the inhibition of OPs on BChE resulted in the reduced generation of TCh, thus inducing the recovery of electrochemical signal. Under the optimal experimental, dichlorvos can be detected in a wide range of 10−6–10−10 M, with a detection limit of 3 × 10−10 M. Moreover, the assay was successfully used to analyze dichlorvos in cucumber juice and pear juice, showing a great promising potential for detecting organophosphorus pesticides in complex samples.

2,4,6-Trinitrophenol (TNP) is widely used in our daily life; however, excessive use of TNP can lead to a large number of diseases. Therefore, it is necessary to find an effective method to detect TNP. Herein, the rapid fluorescence quenching by TNP was developed for the fluorometric determination of TNP in aqueous medium based on the internal filter effect. Nitrogen-sulfur-codoped carbon nanoparticles (N,S-CNPs), synthesized by a one-pot solvothermal method with the precursors of L-cysteine and citric acid, were applied for the determination of TNP as a fluorescent probe. The excitation peak center of N,S-CNPs and the emission peak center are 340 nm and 423 nm, respectively. The probe can be used in a variety of conditions to detect TNP due to its relatively stable properties. Meanwhile, it has a fast response time ( 1 min), wide linear response range (0.1-40 μM), and low detection limit (43.0 nM). This probe still has excellent selectivity and high sensitivity. The method was also used to detect standard water samples with a satisfactory recovery rate, and it will be used in the application of pollutants and clinical diseases. Graphical abstract.

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

As a newly developed and powerful analytical method, the use of photoelectrochemical (PEC) biosensors opens up new opportunities to provide wide applications in the early diagnosis of diseases, environmental monitoring and food safety detection. The properties of diverse photoactive materials are one of the essential factors, which can greatly impact the PEC performance. The continuous development of nanotechnology has injected new vitality into the field of PEC biosensors. In many studies, much effort on PEC sensing with semiconductor materials is highlighted. Thus, we propose a systematic introduction to the recent progress in nanostructure-based PEC biosensors to exploit more promising materials and advanced PEC technologies. This review briefly evaluates the several advanced photoactive nanomaterials in the PEC field with an emphasis on the charge separation and transfer mechanism over the past few years. In addition, we introduce the application and research progress of PEC sensors from the perspective of basic principles, and give a brief overview of the main advances in the versatile sensing pattern of nanostructure-based PEC platforms. This last section covers the aspects of future prospects and challenges in the nanostructure-based PEC analysis field.

Methods based on enzyme labels or nano labels have been developed for immunoassays, but most of them have low sensitivity and are unsuitable for low-abundance protein diagnostics and biosecurity. Herein, an innovative quartz crystal microbalance (QCM) immunosensing method was designed for high-efficiency detection of carcinoembryonic antigen (CEA) from serum samples with colorectal cancer patients by using horseradish peroxidase (HRP) nanoparticles as the enhancer, accompanying enzymatic biocatalytic precipitation (EBCP) toward 4-chloro-1-naphthol (4-CN) on an anti-CEA capture antibody-conjugated QCM probe. Initially, HRP nanospheres were synthesized on the basis of the reverse micelle method with the assistance of glutaraldehyde cross-linking, and then covalently conjugated onto polyclonal anti-CEA detection antibodies. The QCM immunosensing probe was prepared by immobilizing monoclonal anti-CEA capture antibodies on an l-cysteine-modified gold substrate. In the presence of target CEA, a sandwich-type immunoreaction was carried out between capture antibody and detection antibody, thereby resulting in the attachment of HRP nanospheres on the gold probe. Upon addition of 4-CN in the QCM cell, the carried HRP nanospheres catalyzed the 4-CN oxidation to produce an insoluble precipitate on the gold electrode, thus causing a change in the frequency. Relative to the conventional HRP-labeled strategy and direct antigen-antibody reaction, improved analytical features were obtained with HRP nanospheres. With the HRP nanosphere labeling method, the factors influencing the performance of the immunoassay were also studied. The covalent conjugation of antibodies with HRP nanospheres and the gold substrate achieved a good repeatability and intermediate precision down to 10.7%. Under optimum conditions, the frequency variation of the QCM immunoassay was proportional to the target CEA concentration within a dynamic linear range of 0.01-100 ng mL-1 with a detection limit (LOD) of 7.8 pg mL-1. In addition, the developed QCM immunoassay showed high specificity and long-term storage stability, and could be used for the analysis of human serum samples with consistent results in comparison with those obtained from the commercial enzyme-linked immunosorbent assay (ELISA) method.

Exploiting innovative sensing mechanisms and their rational implementation for selective and sensitive detection has recently become one of the mainstream research directions of photoelectrochemical (PEC) bioanalysis. In contrast to existing conventional strategies, this study presents a new liposome-mediated method via

An effective signal amplification strategy based on temperature-amplification synergistic pressure was designed for the sensitive detection of carcinoembryonic antigen (CEA) by using a noncontact point-of-care testing (POCT) aptasensor with a flexible pressure sensor based on a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-modified sponge (PEDOT:PSS-sponge). In the biological recognition system, target analyte triggered the release of platinum nanoparticle-labeled complementary DNA (Pt-cDNA) from CEA aptamer-conjugated magnetic beads. On the basis of the unique characteristics of platinum nanoparticles (e.g., catalytic ability for H

C-reactive proteins (CRPs; an acute-phase protein) in patients with initial acute cerebral infarction neurological rehabilitation prediction have a significant correlation. In this work, a simple and sensitive anodic-stripping voltammetric (ASV) immunosensing system was innovatively designed for the quantitative screening of target CRPs using biomimetic-mineralized bifunctional antibody-Cu3(PO4)2 nanoflowers as molecular tags. In this system, a monoclonal anti-CRP antibody-anchored microtiter plate was utilized to specifically capture target CRPs from the sample. For detection, a sandwiched immunoreaction mode was employed with the antibody-Cu3(PO4)2 nanoflowers in the presence of analytes. Subsequent ASV measurement of copper ions (Cu2+) released under acidic conditions from the bifunctional nanoflowers was conducted at an in situ prepared mercury film electrode. The introduction of hybrid nanoflowers greatly increased the loading amount of copper ions on the molecular tag, thereby amplifying the detectable signal of electrochemical immunoassay. Meanwhile, factors influencing the analytical properties of the electrochemical immunoassay were investigated in detail. By combining the high-efficiency nanohybrids with signal amplification, the dynamic concentration range of electrochemical immunoassay spanned from 0.01 ng mL-1 to 100 ng mL-1 toward the target CRP. The limit of detection was calculated to be 0.0079 ng mL-1 at 3Sblank criterion. Intra- and interassay imprecisions (relative standard deviations: RSDs) were less than or equal to 6.72%. Good anti-interference ability, long-term storage stability, and acceptable accuracy for the evaluation of human serum specimens were observed during a series of procedures to determine the target protein. In addition, the bifunctional nanoflower-based immunosensing system offers promise for the simple, cost-effective analysis of disease-related proteins.

Sensitive and accurate miRNAs assay is critical for early diagnosis of non-small-cell lung carcinomas (NSCLC). Herein, we demonstrate a photothermal and electrochemical dual-readout assay method for miRNA detection based on a novel biocatalysis-mediated MOF-to-prussian blue (PB) transformation (BMMPT) strategy and the catalytic hairpin assembly (CHA) amplification strategy. It is found that the Fe

This work reports a photoelectrochemical (PEC) biosensing platform for the sensitive and specific screening of thrombin by using graphene oxide-coated copper-doped zinc oxide quantum dots (Cu0.3Zn0.7O-GO QDs) as the photoactive materials and glucose oxidase-encapsulated DNA nanoflowers (GOx-DFs) for signal amplification. Interestingly, the coated graphene oxide nanosheets on the surface of the Cu0.3Zn0.7O QDs could cause the charge to transfer rapidly and ameliorate the photocorrosion. The doped copper into the quantum dots could enhance the absorption of visible light by tuning the band gap of ZnO QDs, therefore increasing the photocurrent under visible irradiation. Upon addition of target thrombin, a sandwiched reaction was carried out between thrombin aptamer and GOx-DFs, accompanying the formation of nanocomposites with the magnetic microparticles (MMPs)/thrombin/GOx-DFs. Followed by magnetic separation, the carried GOx oxidized glucose to H2O2, thus resulting in the increasing photocurrent of the Cu0.3Zn0.7O-GO QD-modified electrode. Under optimum conditions, the developed PEC biosensing platform exhibited good analytical performance with a linear range of 50–10 000 fM thrombin and a limit of detection of 29 fM. Impressively, our strategy offers a new horizon in developing bridge-connected graphene-coated nanomaterials and novel signal amplification strategy for the development of PEC biosensors.

Sensors based on colorimetry, fluorescence, and electrochemistry have been widely employed to detect acetylcholinesterase and its inhibitors, however, there are only a minority of strategies for AChE detection based on photothermal method. This work reports a versatile dual-mode colorimetric and photothermal biosensing platform for acetylcholinesterase (AChE) detection and its inhibitor (paraoxon-ethyl, a model of AChE inhibitors) monitor based on Fe-N-C/H

Early diagnosis of cancers relies on the sensitive detection of specific biomarkers, but most of the current testing methods are inaccessible to home healthcare due to cumbersome steps, prolonged testing time, and utilization of toxic and hazardous substances. Herein, we developed a portable self-powered photoelectrochemical (PEC) sensing platform for rapid detection of prostate-specific antigen (PSA, as a model disease-related protein) by integrating a self-powered photoelectric signal output system catalyzed with chemiluminescence-functionalized Au nanoparticles (AuNPs) and a phosphomolybdic acid (PMA)-based photochromic visualization platform. TiO2-g-C3N4-PMA photosensitive materials were first synthesized and functionalized on a sensor chip. The sensor consisted of filter paper modified with a photocatalytic material and a regional laser-etched FTO electrode as an alternative to a conventional PEC sensor with a glass-based electrode. The targeting system involved a monoclonal anti-PSA capture antibody-functionalized Fe3O4 magnetic bead (mAb1-MB) and a polyclonal anti-PSA antibody (pAb2)-N-(4-aminobutyl)-N-ethylisoluminol-AuNP (ABEI-AuNP). Based on the signal intensity of the chemiluminescent system, the photochromic device color changed from light yellow to heteropoly blue through the PMA photoelectric materials integrated into the electrode for visualization of the signal output. In addition, the electrical signal in the PEC system was amplified by a sandwich-type capacitor and readout on a handheld digital multimeter. Under optimum conditions, the sensor exhibited high sensitivity relative to PSA in the range of 0.01-50 ng mL-1 with a low detection limit of 6.25 pg mL-1. The flow-through chemiluminescence reactor with a semiautomatic injection device and magnetic separation was avoid of unstable light source intensity inherent in the chemiluminescence process. Therefore, our strategy provides a new horizon for point-of-care analysis and rapid cost-effective clinical diagnosis.

A simple thermal aptasensing platform was devised for the sensitive detection of organophosphate pesticides (using malathion as a model target) based on the efficient self-heating reaction of a warming pad with a switchable target responsive enzyme-encapsulated three-dimensional (3D) DNA hydrogel using a portable thermometer as a signal readout in this work. The existence of the target malathion would open the catalase-3D network and lots of catalase was released from the hydrogel, which could efficiently convert H2O2 to an O2 molecule. The product O2 is the critical condition for the self-heating of the warming pad. Thereafter, the temperature was enhanced with the increasing amount of O2. The strategy displays outstanding specificity, reproducibility and stability. Moreover, this method can be easily extended to monitor other molecules using different aptamer sequences in practical applications.

Aptamer- or antibody-based sensing protocols have been reported for detecting carcinoembryonic antigen (CEA), but most exhibit complicated procedures or multiple reactions. In this work, we developed a one-step aptasensing protocol for the spectrometric determination of CEA based on 4-nitrophenol (4-NP)-loaded magnetic mesoporous silica nanohybrids (MMSNs) for bioresponsive controlled-release applications. To fabricate such a responsive–controlled sensing system, single-stranded complementary oligonucleotides relative to the CEA-specific aptamer were first modified on the aminated MMSN. Thereafter, 4-NP molecules blocked the pores with the assistance of the aptamers via a hybridization reaction. The introduced target CEA specifically reacted with the hybridized aptamer, thus detaching from the MMSN to open the gate. The loaded 4-NP molecules were released from the pores, as determined using ultraviolet–visible (UV–vis) absorption spectroscopy after magnetic separation. Under optimum conditions, the absorbance increased with an increase in the target CEA in the sample and exhibited a good linear relationship within the dynamic range of 0.1–100 ng mL−1, with a detection limit of 46 pg mL−1. Moreover, this system also displayed high specificity, good reproducibility, and acceptable accuracy for analyzing human serum specimens, in comparison with a commercialized human CEA-enzyme-linked immunosorbent assay (ELISA) kit.

Herein, we explore a general Cu

Taking advantage of the high-efficiency indiscriminate ssDNA cleavage activity of Cas12a in combination with the diffusivity difference of methylene blue (MB)-labeled probes (short oligonucleotides/mononucleotides) toward the negatively-charged indium tin oxide (ITO) electrode, a simple, immobilization-free, highly sensitive, and homogeneous electrochemical biosensor for the detection of human papillomavirus (HPV-16) has been fabricated. At the core of the detection process, Cas12a employed ssDNA trans-cleavage capability to achieve short-strand nucleotide cleavage, while MB-labeled probes served as high-efficiency homogeneous electrochemical emitters to achieve differential pulse voltammetric (DPV) signal. Specifically, due to strong electrostatic repulsion, MB-labeled short oligonucleotides (reporter) cannot diffuse freely to the surface of the negatively charged ITO electrode, and only weak electrochemical signals can be detected. The presence of the target HPV-16 can activate the Cas12a complex to perform indiscriminate ssDNA cleavage of the reporter to produce MB-labeled mononucleotides. The MB-labeled mononucleotides with a smaller size have almost no negative charge, so they very easily diffuse to the surface of the ITO electrode and result in an enhanced electrochemical signal response. Different electrochemical responses (DPV peak intensity) of the CRISPR-Cas12a-assisted amplification strategy can be obtained through the diffusion rate of different MB-labeled DNA on the electrode, which is also positively correlated with the input HPV-16 concentration. Given the unique combination of the CRISPR-Cas12a system with the homogeneous electrochemical solution phase, the detection limit is determined to be 3.22 pM (wide dynamic working range from 0.01 nM to 100 nM) and the two-step detection workflow could be completed within 50 min at ambient temperature, which is superior to that of the HPV-based biosensors previously reported.

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.

With the introduction of gas-based contactless electrochemical biosensors lies the prospects of separating the sensing interface from the bioassembly platform, enhancing stability, and exploring si...

An all-solid-state metal-mediated Z-scheme photoelectrochemical (PEC) immunoassay was designed for sensitive detection of prostate-specific antigen (PSA) by using WO3-Au-CdS nanocomposite as photoactive material and copper ion (Cu2+) as an inhibitor. The Z-scheme PEC system comprising of CdS nanoparticle (photosystem I; PS I), WO3 nanorod (photosystem II; PS II) and gold nanoparticle (Au NP; solid electron mediator) was reasonably established by a simple and green synthetic method. As an important part of Z-scheme system, the sandwiched gold nanoparticles between electron donor materials and hole provider materials could accelerate electron transfer from positive conduction band (CB) of WO3 to negative valence band (VB) of CdS, thus resulting in high-efficient separation of the carriers. In the presence of target PSA, a sandwiched immunoreaction was executed between capture antibody-coated microplate and CuO nanoparticle-labeled detection antibody. Thereafter, CuO nano labels were dissolved into Cu2+ ions under acidic condition to decrease the photocurrent of Z-scheme WO3-Au-CdS thanks to the formation of exciton trapping center of CuxS (x = 1,2) on the surface. Under optimum conditions, Z-scheme PEC immunoassay exhibited good photocurrents toward target PSA within a linear range of 0.01–50 ng mL−1 at a limit of detection of 1.8 pg mL−1. Moreover, the Z-scheme PEC immunoassay had high selectivity and accuracy. Importantly, this method provides a new horizon for detection of disease-related biomarkers with high sensitivity.

This work reports a strategy for glutathione-loaded liposome-encoded magnetic beads initiated by palindromic fragment-mediated single-chain amplification (PFMSCA) for high-precision quantification of a low-abundance aminoglycoside antibiotic (kanamycin; Kana) by using In2O3–ZnIn2S4 (IO-ZIS) as a photoactive matrix. In this strategy, a Kana-recognition region, primer-like palindromic fragment, and polymerization/nicking template are reasonably integrated into one oligonucleotide (hairpin HP1) for target recognition, magnetic separation, and target amplification. Upon target Kana introduction, the Kana-aptamer region in HP1 specifically recognizes the Kana and triggers the palindromic tails intramolecular self-hybridization, amplifying a large number of short fragments in the presence of Klenow fragment polymerase and Nt.BbvCI. The as-generated nick fragments act as a linker to introduce the free hairpin HP2-functionalized glutathione-loaded liposomes (HP2-GLL) onto the surface of the hairpin HP3-modified m...

Herein a versatile photoelectrochemical (PEC) bioanalysis platform for sensitive and specific screening of low-abundance antibiotics (kanamycin, Kana, used in this case) was innovatively designed using rGO-Bi2WO6-Au as photoactive matrix and target-induced branched hybridization chain reaction (t-bHCR) for efficient signal amplification. To realize the high-performance of our PEC bioanalysis system, rational introduction of reduced graphene oxide (rGO) and Au nanoparticles (Au NPs) greatly accelerated the electron transfer and enhances photoactivity. As expected, the ternary nanocomposite (i.e., rGO-Bi2WO6-Au) system with cascade energy level exhibited intense PEC signal responses thanks to multistep electron-transfer (MET) mechanism. Upon sensing the target Kana, t-bHCR is readily implemented, thus resulting in the assembly of numerous CuS nanoparticle (CuS NP). As a result, the loading CuS NPs from hyper-branched structure boosted the electron donors (ascorbic acid) consumption and enhanced the steric hindrance, synergistically decrease the photoelectric response. Under the optimized testing conditions, the t-bHCR-based PEC bioanalysis exhibited superior analytical performance with a linear range of 1 pM to 5 nM target Kana and limit of detection down to 0.78 pM. Additionally, favorable stability, great anti-interference ability and satisfactory accuracy for the analysis of actual samples were acquired. Impressively, the concept of t-bHCR-mediated provides an alternative to construct PEC bioanalysis and inspire more interest in the design of advanced PEC bioanalysis through nucleic acid-related signal amplification.

A new split-type photoelectrochemical (PEC) immunosensing platform was designed for sensitive detection of aflatoxin B1 (AFB1) in foodstuffs, coupling with enzymatic hydrolysate-triggered etching reaction of cobalt oxyhydroxide (CoOOH) on cadmium sulfide (CdS) nanoparticles-functionalized interface. Initially, the photosensitive electrode was prepared by coating CoOOH nanosheets on the surface of CdS nanoparticles to quench the photocurrent. Thereafter, a competitive-type enzyme immunoreaction was carried out on monoclonal anti-AFB1 antibody-conjugated magnetic bead by using alkaline phosphatase (ALP)-labeled bovine serum albumin-AFB1 (AFB1-BSA) conjugate as the competitor. With the formation of immunocomplex, the carried ALP hydrolyzed ascorbic acid 2-phosphate (AAP) into ascorbic acid (AA) and phosphate. The former ascorbic acid produced etched or dissolved CoOOH nanosheets into Co2+ ions, thus resulting in the exposure of CdS nanoparticles on the surface to enhance the photocurrent of the modified electrode. Under optimum conditions, the photocurrent decreased linearly with the increasing AFB1 concentration in the dynamic range of 0.01–10 ng mL−1, and the limit of detection was 2.6 pg mL−1. The precision of this method (expressed as RSD) was ±8.6%. In addition, the accuracy was monitored by analyzing spiked food samples, and gave the well-matched results with the referenced ELISA method.

This work presented an innovative and rationally engineered palindromic molecular beacon (PMB) based "Z-scheme" photoelectrochemical (PEC) biosensing protocol for the selective screening of kanamycin (Kana) through DNA hybridization-induced conformational conversion. Interestingly, the ingeniously designed PMB integrated the multifunctional elements including recognition region, primer-like palindromic fragment, and polymerization-nicking template. The cosensitized structures consisted of CdS quantum dot functionalized hairpin DNA2 (QD-HP2) and region-selectively deposited gold nanoparticles onto {001} facets of bismuth oxychloride (BiOCl-Au). Compared with BiOCl-Au alone, the attachment of CdS QDs onto BiOCl-Au (i.e., BiOCl-Au-CdS QDs) exhibited evidently enhanced photocurrent intensity thanks to the synergistic effect of Z-scheme BiOCl-Au-CdS QDs. After incubation with target Kana, Kana-aptamer binding could induce the exposure of PMB region for hairpin DNA1 (HP1). The exposed palindromic tails hybridized with each other (like a molecular machine) to consume the substrates (dNTPs) and fuels (enzyme) for the releasing of numerous nick fragments (Nick). The as-generated nick fragments could specifically hybridize with the complementary region of QD-HP2, thus resulting in decreasing photocurrent because of the increasing spatial distance for electron transfer between two-type photosensitizers. Under optimum conditions, the PMB-based sensing system exhibited satisfying photocurrent responses toward target Kana within the working range from 50 to 5000 fM at a low detection limit of 29 fM. Impressively, the concept of a palindromic fragment-mediated primer-free biosensing strategy offers a new avenue for advanced development of efficient and convenient biodetection systems.

The synthesis of NH3 heavily relies on the Haber-Bosch process suffering from a large amount of CO2 emission and energy consumption. Possessing eco-friendly and sustainable characteristics, electrochemical reduction is considered as a promising candidate for artificial N2 fixation under ambient conditions, but efficient electrocatalysts are crucial for the N2 reduction reaction (NRR). In this communication, we report that perovskite La2Ti2O7 nanosheets behave as an efficient NRR electrocatalyst with excellent selectivity under ambient conditions. In 0.1 M HCl, this catalyst achieves a high NH3 yield rate of 25.15 μg h-1 mgcat.-1 with a faradaic efficiency of 4.55% at -0.55 V vs. a reversible hydrogen electrode. Notably, it also shows high electrochemical stability.

Methods based on the photothermal effect (a common phenomenon in nature) have been widely applied in different fields; however, their application in bioanalysis has lagged behind. Herein, we designed a near-infrared (NIR) photothermal immunoassay for the qualitative or quantitative detection of prostate-specific antigen (PSA) using titanium carbide (Ti3C2) MXene quantum dot (QD)-encapsulated liposomes with high photothermal efficiency. This system involves a sandwich-type immunoreaction and photothermal measurements. Ti3C2 MXene QDs were utilized as innovative photothermal signal beacons and were encapsulated in liposomes for the labeling of the secondary antibody. The assay was carried out by coupling a low-cost microplate with a homemade 3D printed device. Under NIR-laser irradiation, the Ti3C2 MXene QDs converted the light energy into heat, and a shift in temperature corresponding with the analyte concentration was obtained on a handheld thermometer. Under optimal conditions, the Ti3C2 MXene QD-based photothermal immunoassay exhibited a dynamic linear range from 1.0 ng mL-1 to 50 ng mL-1 with a limit of detection of 0.4 ng mL-1 for PSA detection. Also, we constructed portable equipment using a portable near-infrared imaging camera to collect visual thermal data for the semi-quantitative analysis of the target PSA within 3 min. The specificity, reproducibility and accuracy of the photothermal immunoassay were acceptable. Importantly, our strategy opens new opportunities for protein point-of-care (POC) testing and biosecurity diagnostics.

A photothermal immune-imaging assay was innovatively designed for the visual quantitative detection of cancer biomarkers by coupling CuxS nanocrystals with a portable infrared thermal imager on a smartphone. The rolling circle amplification (RCA) technique was used for the formation of a CuxS nanocrystal concatemer, thus opening up new territories in immunoassay development.

An innovative visible light-driven photoelectrochemical (PEC) immunosensing system was reasonably established for the sensitive detection of prostate-specific antigen (PSA) by using perovskite metal oxide@gold nanoparticle heterostructures (BaTiO3/Au) as the photoactive materials. When plasmonic Au nanoparticles were directly decorated on BaTiO3, a several times surface plasmon resonance (SPR) enhancement of photocurrent density was induced via the injection of hot electrons from visible light-excited Au nanoparticles into the conduction band of BaTiO3, and the combination of BaTiO3 and Au nanoparticles was employed as a promising platform for developing a photoelectrochemical bioanalysis. As a proof of concept, PSA had been detected by the BaTiO3/Au nanocomposite-based PEC sensor. To design such an immunoassay protocol, a monoclonal anti-PSA capture antibody (cAb)-coated microplate and glucose oxidase/polyclonal anti-PSA detection antibody-modified gold nanoparticles (GOx–Au NP–dAb) were used as the immunoreaction platform and signal probe, respectively. Upon the addition of target PSA, a sandwiched immunocomplex was formed accompanying the immuno-recognition between the antigen and antibody, and then the carried GOx could oxidize glucose to produce H2O2. The photocurrent of the BaTiO3/Au nanocomposite-functionalized electrode amplified with increasing H2O2 concentration since H2O2 is considered as a good hole scavenger. On the basis of the above-mentioned mechanisms and the optimized conditions, the assembled PEC immunosensor was linear with the logarithm of the PSA concentration in the range of 0.01–40 ng mL−1 with a detection limit of 4.2 pg mL−1. It afforded rapid response, good precision, and high stability and specificity, implying its great promise in photoelectrochemical immunoassays. More generally, this system sets up an ideal PEC immunosensing system based on the BaTiO3/Au nanocomposites and represents an innovative and low-cost “signal-on” assay scheme for the practical quantitative screening of low-abundance proteins.

Oxygen-doped graphene (O–G) derived from sodium gluconate is identified as a promising candidate to effectively catalyze ambient electrohydrogenation of N2 to NH3. Electrochemical tests on O–G in 0.1 M HCl suggest a large NH3 yield of 21.3 μg h−1 mgcat.−1 and a high faradaic efficiency of 12.6% at −0.55 and –0.45 V vs. reversible hydrogen electrode, respectively, with strong electrochemical and structural stability in 0.1 M HCl. Density functional theory calculations reveal the NRR catalytic mechanism and suggest that both the CO and O–CO groups contribute more greatly to the NRR compared with the C–O group.

Aflatoxin B1 (AFB1) pollution is one of the most serious problems for food safety. In this paper, a split-type photoelectrochemical (PEC) immunoassay was designed for sensitive detection of AFB1 in foodstuffs by using amorphous TiO2 with all-inorganic perovskite CsPbBr3 nanocrystals (CsPbBr3/a-TiO2). The a-TiO2 layer not only improved the stability of CsPbBr3 nanocrystals, but also facilitated charge transfer, which resulted in the increasing photocurrent of the nanocomposites. Initially, a competitive-type enzyme immunoreaction was executed on a high-binding microplate between the analyte and alkaline phosphatase (ALP)-labeled AFB1-bovine serum albumin (AFB1–BSA) conjugate. Accompanied by the formation of the immunocomplex, the carried ALP triggered enzymatic hydrolysis to generate ascorbic acid (AA, as an electron donor) for increasing the photocurrent of the CsPbBr3/a-TiO2-modified electrode. Coupling with the competitive enzyme immunoassay, the photocurrent of the modified electrode decreased with the increase of target AFB1 concentration in a dynamic working range from 0.01 ng mL−1 to 15 ng mL−1 with a limit of detection (LOD) of 2.8 pg mL−1 under optimum conditions. Furthermore, the photoelectrochemical immunoassay was also utilized to detect AFB1 in peanut and corn samples, giving acceptable accuracy in comparison with the referenced AFB1 enzyme-linked immunosorbent assay (ELISA) method.