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Mo5N6 nanosheets were synthesized by a nickel-induced growth method and were found to possess peroxidase-like activity in acidic condition and catalase-like activity in weak basic condition. In acidic condition, Mo5N6 nanosheets can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H2O2 to form a blue color product (TMBOX). At the co-existence of 4-aminophenol (4-AP), 4-AP can react with H2O2 and TMBOX, resulting in the decrease of TMBOX and the fading of blue color. Therefore, a facile, sensitive colorimetric method for the quantitative detection of 4-AP was developed. The linear range for 4-AP was 1.0 to 80.0 μmol⋅L‒1 (R2 = 0.999), and the detection limit was 0.56 μmol⋅L‒1 based on 3σ/k. Resorcinol, aniline, humic acid, and common ions and anions in surface water did not interfere the determination of 4-AP. This colorimetric method was applied to measure the 4-AP in real water sample from Wulong River in Fujian Province of China. The relative standard deviation for the determination of 4-AP was ranged from 0.03 to 1.88%, and the recoveries from spiked samples were ranged between 99.2 and 107.6%. The determination results were consistent with those obtained by HPLC.

A label-free electrochemical aptasensor is reported for sensitive detection of the 6-kDa early secreted antigenic target (ESAT-6). For the first time, the bimetallic organic framework (b-MOF) of Zr-MOF-on-Ce-MOF was decorated with nitrogen-doped graphene (NG) and applied as the matrix for electroactive toluidine blue (Tb) to form the NG@Zr-MOF-on-Ce-MOF@Tb nanohybrid. The prepared nanohybrid with excellent hydrophilicity, dispersibility, and large specific surface exhibited significant electrochemical response. This nanohybrid could be directly used for anchoring ESAT-6 binding aptamers (EBA) through the interaction between the 5′-phosphate group (PO43−) of EBA and Zr4+ of Zr-MOF. The signal response before and after incubating the ESAT-6 antigen has been evaluated by cyclic voltammetry at a scan rate of 100 mV s−1 from − 0.7 to 0.3 V (vs. SCE). Under optimal conditions, the proposed aptasensor displayed a wide linear range from 100 fg mL−1 to 10 ng mL−1 with a limit of detection (LOD) of 12 fg mL−1. The developed method showed good reproducibility with a relative standard deviation (RSD) of 2.27%. The aptasensor showed favorable results in the analysis of the real samples. With these merits, the aptasensor has exceptional potential as a diagnostic tool for tuberculosis in clinical practice.

Polyaniline (PANI) was functionalized by thiol-ene click chemistry to obtain carboxylic acid–tethered polyaniline (PCOOH). The versatility of PCOOH as an immobilization matrix was demonstrated by constructing four different biosensors for detection of metabolites and cancer biomarker. Immobilization efficiency of PCOOH was investigated by surface plasmon resonance and fluorescence microscopic analysis which revealed dense immobilization of biomolecules on PCOOH as compared to conventional PANI. A sandwich electrochemical biosensor was constructed using PCOOH for detection of liver cancer biomarker, α-fetoprotein (AFP). The sensor displayed sensitivity of 15.24 µA (ng mL−1)−1 cm−2, with good specificity, reproducibility (RSD 3.4%), wide linear range (0.25–40 ng mL−1) at − 0.1 V (vs. Ag/AgCl), and a low detection limit of 2 pg mL−1. The sensor was validated by estimating AFP in human blood serum samples where the AFP concentrations obtained are consistent with the values estimated using ELISA. Furthermore, utilization of PCOOH for construction of enzymatic biosensor was demonstrated by covalent immobilization of glucose oxidase, uricase, and horseradish peroxidase (HRP) for detection of glucose, uric acid, and H2O2, respectively. The biosensors displayed reasonable sensitivity (50, 148, 127 µA mM−1 cm−2), and linear ranges (0.1–5, 0.1–6, 0.1–7 mM) with a detection limit of 10, 1, and 8 µM for glucose, uric acid, and H2O2, respectively. The present study demonstrates the capability of PCOOH to support and enable oxidation of H2O2 generated by oxidase enzymes as well as HRP enzyme catalyzed reduction of H2O2. Thus, PCOOH offers a great promise as an immobilization matrix for development of high-performance biosensors to quantify a variety of other disease biomarkers. Carboxylic acid–tethered polyaniline synthesized by thiol-ene click chemistry was used as matrix to construct four different electrochemical biosensors for detection of cancer biomarker α-fetoprotein, glucose, uric acid, and H2O2.

Pathogenic bacteria can cause the outbreaks of disease and threaten human health, which stimulates the development of advanced detection techniques. Herein, a specific and sensitive electrochemical biosensor for Gram-negative bacteria was established based on the conductive polymer with artificial muscle properties. The effective recognition was achieved through the specific carbohydrate-carbohydrate interaction between gluconamide and lipopolysaccharide. The application of impulse voltage enhances the efficiency of recognition and shortens the detection time through the temporary deformation of the electrode surface, with a limit of detection (LOD) of 1 × 100 CFU/mL and a linear range of 1 × 100 − 1 × 106 CFU/mL for Escherichia coli (E. coli). In addition to the merits of low cost, high efficiency, and rapidity, the developed label-free electrochemical biosensor can also be applicable for other Gram-negative bacteria, owning promising potential in the application of portable devices and paving a potential way for the construction of electrochemical biosensors.

A proof-of-principle concept for free-electrodeposited anodic stripping voltammetry (ASV) sensing of Cu2+ is proposed by using Ti3C2Tx MXene/carbon black (Ti3C2Tx@CB) nanohybrids as electrode materials. Owing to the high adsorption and reduction capability of Ti3C2Tx towards Cu2+, Ti3C2Tx MXene enables Cu2+ to be immobilized and self-reduced directly to form Cu0 on the Ti3C2Tx@CB electrode surface. As a result an oxidation peak current appears from the re-oxidation of Cu0 via differential pulse voltammetry. Carbon black (CB) was introduced to prevent Ti3C2Tx Mxene aggregation and improve the related electron transfer as well as enhance their surface area. After optimizing various conditions, a considerable low limit of detection (4.6 nM) and a wide linear range (0.01–15.0 μM) for Cu2+ were achieved at the working potential from − 0.3 V to 0.0 V (vs SCE). Relative standard deviation (RSD) of eight individual Ti3C2Tx@CB electrodes is 3.72%, and the recoveries from tap water sample and lake water sample were in the ranges of 97.0–108% and 104–107%, respectively.

An AND-NAND logic pair is reported based on non-purified carbon quantum dots (CDs) for ascorbic acid (AA) detection. In the logic operation, molybdenum oxide nanosheets (MoO3 NSs) and AA are used as two signal inputs. In the presence of AA, MoO3 NSs are reduced to plasmonic molybdenum oxide, which decreases the CD fluorescence intensity because of a static quenching, dynamic quenching, and internal filtration effect. Meanwhile, the AA is oxidized to dehydroascorbic acid and forms fluorescent 3-(dihydroxyethyl) furo [3,4-b] quinoxaline-1-one with o-phenylenediamine from non-purified CDs. On this basis, an AND-NAND logic pair was constructed and used as a ratiometric fluorescence sensor for highly sensitive detection of AA. The method has a wide linear range of 0.05–50 μM, and a detection limit of 34 nM. In addition, it was used to detect AA in fresh fruit. Potential applications include chemical computing, optoelectronic devices, biomedical science, and environmental monitoring. 1. A ratiometric fluorescence sensor based on AND-NAND logic pair constructed by CDs and MoO3 NSs was successfully fabricated. 2. The ratiometric fluorescence sensor exhibited satisfactory linear range, high sensitivity, and good selectivity for AA. 3. The ratiometric fluorescence method was able to detect AA in fresh fruit with good results comparable to official fluorescence methods.

A core–shell QDs@mSiO2@y-AuNCs nanoprobe was prepared, and a new ratiometric fluorescent sensor for thiram detection was developed. The mechanism of thiram sensing was investigated using FTIR, surface-enhanced Raman, XPS spectra, etc. The sensing of thiram was mainly ascribed to the formation of Au–S bonds between thiram and Au atoms on y-AuNCs surface, resulting in the dissociation of 11-MUA ligand from the y-AuNCs surface and the charge transfer between thiram and y-AuNCs. In the ratiometric fluorescence detection of thiram based on QDs@mSiO2@y-AuNCs, a linear range of 0.5–60 ng/mL was obtained with a LOD of 0.19 ng/mL. Compared with the fluorescence detection based on y-AuNCs, the ratiometric fluorescence detection of thiram demonstrated 3-fold enhanced sensitivity. The improvement was ascribed to two aspects: the fluorescence emission of y-AuNCs was enhanced after they were loaded onto the QDs@mSiO2 nanoparticles; the ratiometric detection mode provided more precise sensing. The detection of thiram can be completed immediately after mixing the nanoprobe with thiram. Good recoveries of thiram in apple and pear samples were achieved. All the above results demonstrated the high potential of this method in practical applications.

A simple and efficient method was used to synthesize norepinephrine-induced AuPd aerogels (AuPd-NE) with dual enzyme properties, i.e. glucose oxidase-like property, and peroxidase-like property. Thus, AuPd-NE aerogels can be considered as a tandem nanozyme with tandem enzyme-like activity. In the presence of AuPd-NE aerogels, glucose can be decomposed into gluconic acid and H2O2. Then, H2O2 will continue to decompose into ·OH and H2O. The generated ·OH will oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue products of ox-TMB. Accordingly, an enzyme-free method based on AuPd-NE aerogels was proposed for sensitive colorimetric detection of glucose. The linear range of the developed method was 30 to 250 μM, and the limit of detection was 10 μM. The method presents reliable applicability for blood glucose detection in human serum samples. This study will deepen the understanding of tandem nanozymes and then rationally design tandem nanozymes for many fascinating biomedical applications. A simple, sensitive and reliable one-pot enzyme-free colourimetric assay for glucose was developed

A versatile surface-enhanced Raman scattering (SERS) assay has been established that can realize rapid and sensitive determination of sildenafil (SIL) and pioglitazone hydrochloride (PIO) adulteration in healthcare products. Metal–organic frameworks-silver nanoparticles (MOFs-AgNPs) with SERS activity were successfully prepared via in situ synthesis AgNPs on the MOFs surface. By virtue of the adsorptivity of MOFs, the MOFs-AgNPs could effectively concentrate the drug molecules on the electromagnetic enhancement areas of AgNPs. Moreover, the MOFs-AgNPs substrate exhibited more sensitive SERS activity than classical AgNPs with linear range of 1.0 × 10–7–1.0 × 10–5 mol L−1 for SIL and 8.0 × 10–7–3.0 × 10–5 mol L−1 for PIO and limit of detection (LOD) of 4.8 × 10–8 mol L−1 for SIL and 1.4 × 10–7 mol L−1 for PIO. The designed method realized the determination of SIL and PIO in commercial tablets and healthcare products with recoveries of 93.8–108.0% and 93.0–104.0%, respectively, with relative standard deviation (RSD) of 2.7–4.1% and 2.2–4.2%, respectively. The present system displayed little interference effect on determination. This work provides a multifunctional route for the determination of other drugs via the SERS technology.

Water soluble N, S-doped carbon dots (N, S-CDs) with orange emission were synthesized from basic fuchsin and sulfosalicylic acid by the typical hydrothermal route. Based on the inner filter effect (IFE), the prepared N, S-CDs can be innovatively developed as an effective "signal-off" multifunctional sensing platform for sensitive determination of tetracycline antibiotics (for example, chlortetracycline (CTC)) and quercetin. The proposed sensor was utilized to realize the determination of CTC in water and milk samples and quercetin in beer sample (λex = 375 nm, λem = 605 nm) with satisfactory recoveries and relative standard deviations (RSD). The linear range and detection limit (LOD) of CTC is 1.24-165 μM and 32.36 nM, respectively. For quercetin, the linear ranges are 0.98-34 μM and 34-165 μΜ, and the LOD is 6.87 nM (3σ/m). By virtue of the good biocompatibility and long-wavelength emission, N, S-CDs were also used in the imaging of oocystis cells and yeast cells, which demonstrated promising applicability for bio-imaging and sensing. In this paper, N, S-doped carbon dots (N, S-CDs) with orange emission (λem = 605 nm) were synthesized from basic fuchsin and sulfosalicylic acid. Based on the inner filter effect (IFE), the prepared N, S-CDs can be innovatively developed as an effective "signal-off" multifunctional sensing platform for the sensing of tetracycline antibiotics (for example: chlortetracycline (CTC)) and quercetin. The sensor has been successfully applied to the determination of CTC in water and milk samples and quercetin in beer sample (λex = 375 nm, λem = 605 nm). The linear range and detection limit (LOD) of CTC is 1.24-165 μM and 32.36 nM respectively. For quercetin, the linear ranges are 0.98-34 μM and 34-165 μΜ, and the LOD is 6.87 nM (3σ/m). In addition, due to the characteristics of good biocompatibility and long-wavelength emission, the N, S-CDs were also used in the imaging of oocystis cells and yeast cells, which demonstrated promising applicability for bioimaging and sensing.

A facile, economic, and portable test kit based on target-responsive hydrogel with smartphone detection was fabricated for the accurate determination of dichlorvos in tap water and food samples. Carbon dots (CDs) and CdTe quantum dots (QDs) embedded hydrogel were employed as indicator, and fluorescence of CdTe QDs (645 nm) was dynamically quenched by Cu2+ while that of CDs (490 nm) were non-response for Cu2+, em erging a typical ratiometric fluorescence signal. Acetylcholinesterase hydrolyzed acetylthiocholine to generate thiocholine that bound with Cu2+ strongly via S-Cu-S bond. Dichlorvos as competitive inhibitor for acetylcholinesterase prevented the generation of thiocholine, which blocked the formation of Cu-thiocholine complex and changed the ratiometric fluorescence signal. The signal of the test kit, which was recorded by smartphone’s camera, was transduced by ImageJ software into the color parameter that was linearly proportional to the logarithm of dichlorvos concentration. This portable test kit showed wide linear range of 1 to 40 ppb and low detection limit of 0.38 ppb for dichlorvos. This test kit exhibited rapid sample-to-answer detection time (50 min) of dichlorvos in tap water and food samples, and the recoveries were in the range 81.3 to 111% with relative standard deviations of less than 9.1%.

Three-dimensional flowerlike Au@(MoS2/GO/o-MWNTs) nanohybrids (abbreviated as AMGMs) were synthesized and then introduced into an electrochemiluminescence (ECL) system as a new co-reaction accelerator for the ultrasensitive prostate-specific antigen (PSA). The AMGMs not only served as a substrate with good conductivity and a large specific surface area for loading abundant primary antibodies but also acted as an effective co-reaction accelerator; the co-reaction accelerator could interact with a co-reactant rather than the luminophore to boost the generation of free radical intermediates, thereby producing abundant excited states of luminophores to amplify the ECL signal response. Additionally, an anticipated signal amplification strategy based on the hybridization chain reaction (HCR) was developed by gathering a large amount of a DNA initiator on gold nanoparticles. These gathered DNA initiators could generate multiple DNA concatemers and attach more signal molecules, which resulted in outstanding exponential signal amplification. Consequently, the ECL immunosensor demonstrated high sensitivity, with a linear range from 0.1 pg mL−1 to 50 ng mL−1 and a detection limit of 0.028 pg mL−1. In addition, the immunosensor displayed excellent stability and selectivity. It was evaluated by analyzing human serum sample. The recovery obtained was 98.80–112.00% and the RSD was 1.73–3.12%, indicating the immunosensor could be applied to the simultaneous detection of PSA in human serum samples.

Early diagnosis of hepatitis C virus (HCV) infection is essential to prevent disease from spreading and progression. Herein, a novel electrochemical biosensor was developed for ultrasensitive detection of HCV core antigen (HCVcAg) based on terminal deoxynucleotidyl transferase (TdT) amplification and DNA nanowires (DNW). After sandwich-type antibody-antigen recognition, the antibody-conjugated DNA was pulled to the electrode surface and further extended into a long DNA sequence by robust TdT reaction. Then, large numbers of methylene blue-loaded DNW (MB@DNW) as signal labels are linked to the extended DNA sequence. This results in an amplified electrochemical signal for HCVcAg determination, typically measured at around -0.25 V (Ag/AgCl). Under the optimum conditions, the proposed biosensor achieved a wide linear range for HCVcAg from 0.1 to 312.5 pg/mL with a low limit of detection of 32 fg/mL. The good practicality of the biosensor was demonstrated by recovery experiment (recoveries from 98 to 104% with RSD of 2.5-4.4%) and comparison with enzyme-linked immunosorbent assay (ELISA). Given the highlighted performance, the biosensor is expected to act as a reliable sensing tool for HCVcAg determination in clinics. Schematic representation of the ultrasensitive electrochemical biosensor based on terminal deoxynucleotidyl transferase (TdT) amplification linked with methylene blue-loaded DNA nanowires (MB@DNW), which can be applied to the determination of hepatitis C virus core antigen (HCVcAg) in clinical samples. dTTPs, 2'-deoxythymidine 5'-triphosphate.

A photoelectrochemical (PEC) biosensor capable of detecting cytokeratin 19 fragment 21-1 (CYFRA21-1) was optimized by taking advantage of the powerful conjugate repeats of horseradish peroxidase and tyramine (HRP-tyramine)–triggered enzymatic biocatalytic precipitation (BCP) on high-performance BiVO4/Ag3VO4/SnS2 photoelectrodes. Compared with the ubiquitous BCP strategy, we identified a design supporting conjugate repeats generated by HRP and tyramine–triggered immeasurable insoluble precipitates in the presence of hydrogen peroxide and 4-chloro-1-phenol (4-CN), and the steric hindrance improved sensitivity. Moreover, by virtue of BiVO4, Ag3VO4, SnS2 excellent level matching structure and chemical stability, a heterojunction (BiVO4/Ag3VO4/SnS2) with high light absorption efficiency has been successfully prepared. The novel heterostructure system of BiVO4/Ag3VO4/SnS2 with high detection current and low background signal exhibited high-performance PEC determination. Generally, the hitherto untapped biosensor resource realized the sensitive detection of CYFRA21-1 with a wide linear range from 50 fg/mL to 200 ng/mL, and a detection limit of 15 fg/mL, which illustrated the potential for biotechnological applications.

A gold nanoparticle (AuNP)–based sensing strategy based on rapid reduction of Au(I→0) is proposed. As a proof-of-concept study, the proposed sensing principle is designed for simultaneous and colorimetric detection and discrimination of multiple proteins. In the presence of H2O2, the target proteins could reduce Au(I) (i.e. HAuCl2) to AuNPs with different sizes, shapes and dispersion/aggregation states, thus resulting in rapidly colorimetric identification of different proteins. The optical response (i.e. color) of AuNPs is found to be characteristic of a given protein. The color response patterns are characteristic for each protein and can be quantitatively differentiated by statistical techniques. The sensor array is capable of discriminating proteins at concentrations as low as 0.1 μg/mL with high accuracy. A linear relationship was observed between the total Euclidean distances and protein concentration, providing the potential for protein quantification using this sensor array. The limit of detection (LOD) for catalase (Cat) is 0.08 μg/mL. The good linear range (from 0 to 8 μg/mL) has been used for the quantitative assay of Cat. To show a potentially practical application, this method was used to detect and discriminate proteins in human urine and tear samples.

A flexible free-standing electrochemical biosensor to detect carcinoembryonic antigen (CEA) is described based on a conducting polypyrrole (PPy) nanocomposite film electrode. The conducting PPy composite was constructed by the sandwiched structure formed by PPy doped with pentaerythritol ethoxylate (PEE) and 2-naphthalene sulfonate (2-NS-PPy) separately via electropolymerization. Gold nanoparticles (AuNPs) were fixed on the PPy composite film by electrodeposition and then connected to CEA aptamer through self-assembly to construct a free-standing electrochemical biosensor breaking away from additional soft substrates and current collector. This PPy composite film-based electrochemical biosensor exhibits satisfying sensing performance for CEA detection, with a linear range from 10−10 g/mL to 10−6 g/mL and a detection limit of 0.033 ng/mL, good specificity and long-term sensing stability (96.8% of the original signal after 15 days). The biosensor also presents acceptable reproducibility with 1.7% relative standard deviation. Moreover, this electrochemical biosensor owns the deformation stability that could bear various deformations (twisting, folding, and knotting) without affecting device’s sensing performance. It can even maintain 99.4% of the original signal under 25% strain deformation. Due to the superior sensing performance, high stability (mechanical deformation and long-term storage), and flexibility, this free-standing electrochemical biosensor proves huge potential in application of flexible and wearable electronics.

A sensitive voltammetric sensor has been developed for hazardous methyl parathion detection (MP) using graphene oxide@Ce-doped TiO2 nanoparticle (GO@Ce-doped TiO2 NP) electrocatalyst. The GO@Ce-doped TiO2 NPs were prepared through the sol-gel method and characterized by various physicochemical and electrochemical techniques. The GO@Ce-doped TiO2 NP–modified glassy carbon electrode (GCE) addresses excellent electrocatalytic activity towards MP detection for environmental safety and protection. The developed strategy of GO@Ce-doped TiO2 NPs at GCE surfaces for MP detection achieved excellent sensitivity (2.359 μA μM−1 cm−2) and a low detection limit (LOD) 0.0016 μM with a wide linear range (0.002 to 48.327 μM). Moreover, the fabricated sensor shows high selectivity and long-term stability towards MP detection; this significant electrode further paves the way for real-time monitoring of environmental quantitative samples with satisfying recoveries.

A sandwich-format electrochemiluminescence (ECL) immunosensor has been developed for alpha-fetoprotein (AFP) detection based on the use of ordered mesoporous carbon-molybdenum disulfide (OMC-MoS2) as a sensor platform and cuprous oxide @ ordered mesoporous carbon-Ru(bpy)32+ (Cu2O@OMC-Ru) composites as signal tags. OMC alongside MoS2 plays a synergistic role in improving the electrochemical performance of the electrode in the electron transfer process. The uniform cubic-shaped Cu2O@OMC-Ru nanocrystals display excellent luminous efficiency, with a signal amplification strategy of OMC-MoS2 synergistic enhancement and Cu2O@OMC which is capable of immobilizing more Ru(bpy)32+ serving as a tracing tag to label antibodies. A detectable ECL emission at a Cu2O@OMC-Ru nanocrystals modified electrode is initiated at an applied voltage of +1.15 V (scanning range: 0–1.2 V), in the presence of the tripropylamine (TPA) as coreactant. With the increase in AFP concentration, the loading of Cu2O@OMC-Ru at the electrode increases. Afterward, the ECL detection of AFP shows a wide linear range from 0.1 pg/mL to 10 ng/mL with a correlation coefficient of 0.9964 and a detection limit of 0.011 pg/mL (S/N = 3) under the optimal experimental conditions. The recoveries were in the range 91.2–97.1% with RSD varying from 4.8 to 8.5%. Overall, the novel immunosensor has been successfully applied to the analysis of human serum samples, indicating a great potential for application in clinical diagnostics.

A facile one-pot method for synthesis of bovine serum albumin (BSA)-gold nanoclusters (AuNCs) has been developed. The formation of BSA-AuNCs took only 30 s under mild conditions. BSA-AuNCs exhibited strong orange-yellow fluorescence, and the excitation and emission peaks were at 370 nm and 564 nm, respectively. In the process of forming BSA-AuNCs, the molecular chain of BSA has not been destroyed. Moreover, there were a large number of Au cations on the surface of BSA-AuNCs, which had strong oxidizing abilities. The reason for the ultrabright fluorescence of BSA-AuNCs was attributed to the Au(0)@Au(I)@Au(III)-ligand structure on the surface of BSA. In order to evaluate the fluorescence performance of BSA-AuNCs, BSA-AuNCs was used as a probe, realizing the sensitive and selective determination of glutathione (GSH) in a wide linear range of 0.01-0.48 μM and a detection limit of 3.3 nM. The proposed method not only offers a brand-new scheme for synthesizing BSA-AuNCs, but also provides a platform for studying the interaction between metal core and proteins. A facile one-pot method to synthesize ultrabright fluorescent BSA-AuNCs in tens of seconds has been introduced by mixing BSA suspension, KSCN, and HAuCl

A novel photoelectrochemical (PEC) sensor based on “Z-scheme” TiO2@Au@CdS and molecularly imprinted polymer (MIP) was developed for the non-invasive detection of uric acid (UA). The “Z-scheme” material, consisting of an electron-transfer system (Au) and two isolated photochemical systems (CdS, TiO2), was synthesized by chemical deposition method and it worked as a substrate for electro-polymerization of MIP. Due to the high photoelectric conversion efficiency provided by TiO2@Au@CdS and specific imprinting effect afforded by MIP, the sensor displayed desirable sensing performance with the merits of sensitivity, selectivity, repeatability, and stability. The linear range for UA detection is from 1 nM to 9 μM with the detection limit of 0.3 nM (S/N = 3). Moreover, the assay was successfully utilized to measure UA in human tears and offered a reliable result. The incorporation of MIP and “Z-scheme” material into a PEC sensor system is expected to provide a promising strategy for detecting other small molecules.

Nanocomposites can offer a platform to conjugate biorecognition features of aptamer with unique size-dependent properties of a given material, which can autoprobe the binding event based on their electroactive characteristics. Herein, we design electroactive switchable aptamer probes based on co-doped single-phase semiconducting materials employing the cyclic voltammetry method to record the current signal at each step of electrochemical characterization. To do so, we utilized a facile hydrothermal method assisted by co-precipitation method such as Co-Fe-co-doped Ba0.5Sr0.5Zr0.1Y0.1O3-δ (CF-BSZY) and tuned the alignment of the energy band structure of the material to amplify the output of the electrochemical signal. At various steps, changes occurred in the electrochemical properties at the surface of CF-BSZY. The binding of the ssDNA with prepared materials enhances the current signal by the interaction with the target (ochratoxin A (OTA)) depressing the current signal and facilitating the construction of a novel design of electrochemical aptasensor. As a proof of concept, an electrochemical aptasensor for the detection of ochratoxin A (OTA) in rice samples has been developed. The electrochemical aptasensor provides a limit of detection (LOD) of 0.00012 μM (0.12 nM), with a linear range from 0.000247 to 0.74 μM and sound OTA recovery in real samples. The developed aptasensor is simply designed and is free of oligonucleotide labeling or decorative nanoparticle modifications. The proposed mechanism is generic in principle with the potential to translate any type of aptamer and target binding event into a detectable signal; hence, it can be largely applied to various bioreceptor recognition phenomena for subsequent applications.

A portable biosensor has been developed based on microfluidic particle accumulation for visual quantification of copper ions. A copper-dependent DNAzyme is used to connect magnetic microparticles (MMPs) and polystyrene microparticles (PMPs), forming “MMPs-DNAzyme-PMPs.” When copper ions are present, the DNAzyme is cleaved, allowing free PMPs to be released from the MMPs-DNAzyme-PMP complex. Using a capillary-flow-based microfluidic device, the MMPs-DNAzyme-PMPs are first separated by a magnetic chamber, allowing the free PMPs to continue flowing until being trapped at a particle dam with a narrowing nozzle. Therefore, as a thermometer-like display, the copper level can be visually quantified by the accumulation length of the free PMPs in the trapping microchannel. The limit of detection (LOD) is 33 nM determined by the linear range of 25–100 nM, which is 900 times lower than the prevalent standard (~30 μM) in Hong Kong. The system shows excellent selectivity (> 1000-folds) against other heavy metal ions and abilities to adapt to multiple water environmental conditions. Tests on tap water samples and three local natural water sources in Hong Kong manifest that the device can effectively monitor the quality of freshwater with >70% recovery and 26.16% RSD.

The potential of functionalized polypyrrole nanowires (PPyNWs) are demonstrated as a platform for lable-free miRNA detection using electrochemical impedance spectroscopy (EIS). MicroRNAs (miRNAs) detection methods and sensors are mainly challenged by very low concentrations in physiological samples and high similarity among family members. Herein, a sensitive and selective miRNA biosensor was constructed based on electrochemically synthesized PPyNWs, which were functionalized with polyamidoamine dendrimer (PAMAM) by an electro-oxidation method. The prepared PPyNWs/PAMAM hybrid combines the excellent electrical conductivity of conducting polymer PPyNWs with high surface to volume ratio of PAMAM. DNA probes were immobilized onto the PPyNWs/PAMAM hybrid for the construction of the miRNA biosensor. Using the sensitive EIS technique to monitor DNA/miRNA hybridization, the developed biosensor demonstrated excellent sensing performances, such as wide linear range (10−14 M-10−8 M) and low detection limit (0.34 × 10−14 M). Even more encouraging, the response sensitivity of the biosensor was 3.12 times higher than that of the bulk PPy-modified sensor, which proved that the microstructure of the PPy nanowires array can greatly improve the performance of the biosensor.

Vitamin D (VD) deficiency is a global health concern due to its serious health impacts, and at present, the monitoring of VD status is expensive. Here, a novel immunosensor for sensitive and label-free detection of 25-hydroxy vitamin D3 (25VD3) is reported. Nanostructured cerium(IV) oxide (nCeO2) was anchored onto carbon cloth (CC) via electrophoretic deposition to fabricate a nanoplatform (nCeO2/CC). Subsequently, bioactive molecules (anti-25VD3 and BSA) were introduced to fabricate the nanobioplatform BSA/anti-25VD3/nCeO2/CC as an immunosensor. The analytical performance of the developed immunosensor was studied towards 25VD3 detection. The immunosensor provides a broad linear range of 1-200 ng mL-1, high sensitivity of 2.08 μA ng−1 mL cm−2, a detection limit of 4.63 ng mL−1, and a response time of 15 min, which is better than that of previous reports. The biosensor exhibited high selectivity, good reproducibility, and excellent stability for about 45 days. The potential application of the proposed immunosensor was observed for real serum samples towards 25VD3 detection that demonstrated a high correlation with the conventional enzyme-linked immunosorbent assay. Graphical abstract Supplementary Information The online version contains supplementary material available at 10.1007/s00604-021-04751-y.

A flexible nano-engineered natural mineral (carbon dot doped natural microcline) based membrane (MCPV) has been developed, which can efficiently detect the presence of hexavalent chromium (Cr6+) and trivalent iron (Fe3+) ions in water by altering its fluorescence emission. Detailed characterization of the membrane was carried out using XRD, FT-IR spectroscopy, FESEM, TEM, and UV-Vis spectroscopy. Mechanical and temperature stabilities were also investigated. This new-generation sensor membrane is designed in such a way that it does not dissolve in water, keeping the water quality unaffected. The fluorescence studies were conducted at 414 nm and “turn-off” response was observed specifically for Fe3+ at 489 nm. A prominent red shift (530 nm) of the fluorescence maxima takes place when it comes to Cr6+. Figures of merit, such as LOD (8.7 μM for Cr6+ and 18.4 μM for Fe3+) and LOQ (29.1 μM for Cr6+ and 61.6 μM for Fe3+), were evaluated from the linear range (0–60 μM for Cr6+ and 0–30 μM for Fe3+) of the calibration curve (Stern-Volmer plots) showing high sensitivity of this sensing probe toward Cr6+ and Fe3+. Recovery and RSD calculations were done in various real-life water samples on intraday-interday basis to determine the accuracy of the sensor. This work validates the fact that the synthesized sensor membrane is capable of detecting these heavy metals in glutathione environment as well, which could be beneficial for early-stage carcinogen detection in living cells.

Unique Ni2CoS4-carbon nanofiber (CNF) composite nanostructures were fabricated using a simple electrospinning-assisted hydrothermal route and used for the rapid and accurate electrochemical oxidation of glucose in real samples at the trace level. Electrochemical impedance spectroscopy and cyclic voltammetry of unmodified and modified electrodes revealed low charge-transfer resistance and the excellent electrocatalytic sensing of glucose when using the Ni2CoS4-CNF at a low potential due to the combined benefits of the highly conductive Ni2Co2S4 anchored to the large surface area of the CNFs. Amperometric analysis of the fabricated sensor has shown an extremely low limit of detection (0.25 nM) and a large linear range (5–70 nM) for glucose at a working potential of 0.54 V (vs. Hg/HgO). The practicability of the Ni2CoS4-CNF for use in glucose determination was tested withl human saliva, blood plasma, and fruit juice samples. The Ni2CoS4-CNF/GCE showed acceptable recovery values for human saliva (99.1–100.8%), blood plasma (98.6–101.5%), and fruit juice (95.1–105.7%) samples. The proposed sensor also exhibited outstanding electroanalytical characteristics for glucose oxidation in these samples, including reusability, repeatability, and interference resistance, even in the presence of other biological substances and organic and inorganic metal ions.

The design and construction of a novel magnetic resonance sensor (MRS) is presented for bisphenol A (BPA) detection. The MRS has been built based on the core component of magnetic Fe3O4 nanoparticles (~ 40 nm), which were uniformly distributed in nanoporous carbon (abbreviated as Fe3O4@NPC). The synthesis was derived from the calcination of the metal organic framework (MOF) precursor of Fe-MIL-101 at high temperature. Fe3O4@NPC was confirmed with enhanced transversal relaxation with r2 value of 118.2 mM−1 s−1, which was around 1.7 times higher than that of the naked Fe3O4 nanoparticle. This enhancement is attributed to the excellent proton transverse relaxation rate of Fe3O4@NPC caused by the reduced self-diffusion coefficient of water molecules in the vicinity of Fe3O4 nanoparticles in the nanoporous carbon. BPA antibody (Ab) and antigen (Ag)-ovalbumin (OVA) were immobilized onto the Fe3O4@NPC to form Ab-Fe3O4@NPC and Ag-Fe3O4@NPC, respectively. These two composites can cause the three-dimensional assembly of Fe3O4@NPC via immunological recognition. The presence of BPA can compete with antigen-OVA to combine with Ab-Fe3O4@NPC, thereby breaking the assembly process (disassembly). The difference in the change of the T2 value before and after adding BPA can thus be used to monitor BPA. The proposed MRS not only revealed a wide linear range of BPA concentration from 0.05 to 50 ng mL−1 with an extremely low detection limit of 0.012 ng mL−1 (S/N = 3), but also displayed high selectivity towards matrix interferences. The recoveries of BPA ranged from 95.6 to 108.4% for spiked tea π, and 93.4 to 104.7% for spiked canned oranges samples, respectively, and the RSD (n = 3) was less than 4.4% for 3 successive assays. The versatility of Fe3O4@NPC with customized relaxation responses provides the possibility for the adaptation of magnetic resonance platforms for food safety development.

A new covalent organic framework (COF) has been prepared with 1,3,6,8-tetra(4-formyl phenyl) pyrene (TFPPy) and 2,6-diaminopyridine (DP) as building units through a Schiff base reaction by a simple tube oven heating procedure and the structure of the COF has been characterized in detail. The obtained DP-Py COF is employed to fabricate a novel electrochemical sensing platform for sensitive and selective determination of theophylline (TP) and caffeine (CAF) simultaneously through compounding with AuNPs; the peak positions of TP and CAF are 0.95 V and 1.28 V, respectively. The synergistic effect between DP-Py COF and AuNPs effectively enhances the analytical sensitivity for the target analytes. Under the optimized experimental conditions, the electrochemical sensing platform shows a sensitive voltammetric response and wide linear range to both TP and CAF, and the detection limits are 0.19 μM and 0.076 μM (S/N = 3), respectively. This method has been successfully used for the determination of TP and CAF in compound paracetamol capsules and black tea samples. The recovery and relative standard deviations (RSD) of TP are 99.3~101% and 97.6~101% and 1.3~2.0% and 1.3~2.1%, respectively, and the recovery and RSD of CAF are 96.1~102% and 99.4~104% and 2.8~3.9% and 1.7~3.2%, respectively. Compared with traditional detection methods, the constructed sensing platform has better performance and is expected to be widely used also in other real sample analyses.

A glassy carbon electrode (GCE) was modified with magnetic molecularly imprinted polymers (mMIPs) using catechin as a template, reduced graphene oxide (rGO), and zeolitic imidazolate frameworks-8 (ZIF-8) for the sensitive detection of catechin (mMIPs/rGO-ZIF-8/GCE). The prepared rGO, ZIF-8, and mMIPs exhibited typical structures and properties determined by various characterizations. The mMIPs showed good selectivity for catechin among several structural analogs. The mMIPs/rGO-ZIF-8/GCE showed a higher maximum peak current for catechin than that of a single component modified GCE. After the optimization of the material ratio, coating amounts, pH, and scan rate, the mMIPs/rGO-ZIF-8/GCE exhibited good selectivity, good linearity, and a low detection limit (LOD) for catechin. The linear range was 0.01 nmol/L-10 μmol/L and the LOD was 0.003 nmol/L (S/N = 3). The relative standard deviations for reproducibility and stability tests (n = 6) were 5.2% and 6.1%, respectively. A recovery between 99.1 and 101.3% was obtained in the detection of catechin in spiked samples. Based on these findings, the proposed mMIPs/rGO-ZIF-8/GCE could be developed further, and future research could be conducted on alternate fabrication strategies and methods to create more portable and practical electrochemical sensors. Graphical Abstract.

A photothermal immunoassay using a thermometer as readout based on polyaniline@Au organic-inorganic nanohybrids was built. Temperature output is acquired due to the photothermal effect of the photothermal nanomaterial. Polyaniline@Au organic-inorganic nanohybrids were synthesized by interfacial reactions with high photothermal conversion efficiency. A sandwich structure of the immunocomplex was prepared on a microplate for determination of carcinoembryonic antigen (CEA) by polyaniline@Au organic-inorganic nanohybrids as nanolabel. The released heat based on light-to-heat conversion from the photothermal nanolabel under NIR irradiation is detectable using the thermometer. The increased temperature is directly proportional to CEA concentration. The linear range of the photothermal immunoassay is 0.20 to 25 ng mL−1 with determination limit of 0.17 ng mL−1.

A high-performance imipramine (IMPR) sensor has been developed based on metal chalcogenide-carbon composite materials. The antimony telluride-graphite nanofiber (Sb2Te3-GNF, hereafter SBT-GNF) composite was synthesized by the hydrothermal method and confirmed by X-ray powder diffraction (XRD) pattern. The morphology, crystalline lattice, and chemical states were characterized by HRTEM, SAED, and XPS analysis. The characterizations confirmed the formation of an effective composite, SBT-GNF. The SBT-GNF was fabricated as a disposable sensor electrode with a screen-printed carbon electrode (SPCE) and examined for the detection of IMPR by differential pulse voltammetry (DPV). The electroanalytical results of SBT-GNF are compared with the SBT and GNF, and the rational design of effective composite is discussed. SBT-GNF/SPCE showed a good linear range (0.01‑51.8 μM), sensitivity (1.35 ± 0.1 μA μM−1 cm−2), and low LOD (4 ± 2 nM). Moreover, the SBT-GNF/SPCE revealed high selectivity and high tolerance limit against potential interfering compounds in blood serum and urine samples. Therefore, this electrochemical sensor can be applicable for the detection of tricyclic antidepressant drug IMPR in clinical and pharmaceutical analysis.

A sensitive and rapid colorimetric biosensor has been developed for determination of amyloid-β peptide (Aβ) and study of amyloidogenesis based on the high peroxidase-like activity of porous bimetallic ZnO-Co3O4 nanocages (NCs). Due to the high binding ability of Aβ monomer to ZnO-Co3O4 NCs, the catalytic activity of ZnO-Co3O4 NCs can be significantly suppressed by Aβ monomer. This finding forms the basis for a colorimetric assay for Aβ monomer detection. The detection limit for Aβ monomer is 3.5 nM with a linear range of 5 to 150 nM (R2 = 0.997). The system was successfully applied to the determination of Aβ monomer in rat cerebrospinal fluid. Critically, the different inhibition effects of monomeric and aggregated Aβ species on the catalytic activity of ZnO-Co3O4 NCs enabled the sensor to be used for tracking the dynamic progress of Aβ aggregation and screening Aβ inhibitors. Compared with the commonly used thioflavin T fluorescence assay, this method provided higher sensitivity to the formation of Aβ oligomer at the very early assembly stage. Our assay shows potential application in early diagnosis and therapy of Alzheimer's disease (AD).

The aggregation of amyloid-β oligomers (AβOs) with extremely strong neurotoxicity has been proved to be the main pathogenesis of Alzheimer's disease (AD). For sensitive quantification of AβOs, a switchable electrochemical aptasensor is proposed. Metal organic framework carrying Au nanoparticles (AuNPs@CuMOF) has been used to label signaling displaced-probe (SD), which formed triple helix switch (THS) by hybridizing with label-free anti-AβOs aptamer (Apt) on the electrodeposited palladium electrode (EPd). Thus, a relatively strong response of differential pulse voltammetry (DPV) was produced (switch on). With the specific binding between AβOs and Apt, the DPV response obviously decreased, owing to destroyed structure of THS and the separation of AuNPs@CuMOF/SD from the EPd (switch off). The mode of "switch on-off" can dramatically enhance the AβOs-dependent DPV intensity change. As a result, the switchable EA exhibited excellent selectivity and sensitivity with the linear range from 0.5 fM to 500 fM and the detection limit of 0.25 fM. When evaluating the AβOs of artificial cerebrospinal fluid (aCSF) samples, the switchable EA exhibited desirable feasibility, and the results are basically consistent with the enzyme linked immunosorbent assay (ELISA). The work could provide a potential tool of the AD diagnosis and a bright future in clinical applications.

A non-invasive aptamer-based electrochemical biosensor using disposable screen-printed graphene electrodes (SPGEs) was developed for simple, rapid, and sensitive determination of cortisol levels. Selective detection of cortisol based on a label-free electrochemical assay was achieved by specific recognition of the cortisol DNA aptamer (CApt). The CApt was modified with streptavidin magnetic beads (MBs) before simple immobilization onto the electrode surface using a neodymium magnet. The electrochemical behavior of the aptamer-based biosensor was assessed by using electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) (vs Ag/AgCl). The specific binding between cortisol and CApt resulted in a decrease in charge transfer resistance (Rct) from EIS using [Fe(CN)6]3−/4− with increasing cortisol concentration. Under optimal conditions, a linear range from 0.10 to 100 ng/mL with a low detection limit (3SD/slope) of 2.1 pg/mL was obtained. Furthermore, the proposed biosensing system exhibited a satisfactory recovery in the range 97.4–109.2% with 5.7–6.6% RSD in spiked artificial human sweat. Regarding the applications of this tool, the aptamer-based biosensor has potential to be a versatile and point-of-care (POC) device for simple, sensitive, selective, disposable, and low-cost cortisol detection.

A rolling circle amplification chemiluminescence immunoassay (RCA-CLIA) was developed for precise quantitation of Aβ in plasma. Capture antibodies conjugated with magnetic beads and detection antibodies with collateral single-stranded DNA (ssDNA) were bound to Aβ42/Aβ40 antigens to form a typical double-antibody sandwich structure. The RCA reaction was triggered by the addition of ssDNA, which generated products with a large number of sites for the binding of acridinium ester (AE)-labeled detection probes, thereby realizing the purpose of the amplification. The RCA-CLIA method had higher sensitivity than conventional CLIA without loss of specificity. Under optimum conditions, the linear range of Aβ42 and Aβ40 detection was 3.9-140 pg/mL and 3.9-180 pg/mL, respectively, with corresponding low detection limits of 1.99 pg/mL and 3.14 pg/mL, respectively. Plasma Aβ42 and Aβ40 were detected in the blood of 21 AD patients and 22 healthy people, wherein this ratio could significantly distinguish AD patients from healthy individuals with a sensitivity of 90.48% and specificity of 63.64% for a cutoff value of 154. The Aβ42/Aβ40 ratio of plasma acts as an accurate indicator for AD diagnosis; therefore, detection of plasma Aβ using the RCA-CLIA exhibits great potential in noninvasive diagnosis and progressive assessment of AD.

A novel dual-functional nanoprobe was designed and synthesized by facile assembly of quinoline derivative (PEIQ) and meso-tetra (4-carboxyphenyl) porphine (TCPP) via electrostatic interaction for simultaneous sensing of fluorescence of Zn2+ and pH. Under the single-wavelength excitation at 400 nm, this nanoprobe not only exhibits “OFF-ON” green fluorescence at 512 nm by specific PEIQ-Zn2+ chelation, but also presents red fluorescence enhancement at 654 nm by H+-triggered TCPP release. The nanoprobe demonstrated excellent sensing performance with a good linear range (Zn2+, 1–40 μM; pH, 5.0–8.0), low detection limit (Zn2+, 0.88 μM), and simultaneous response towards Zn2+ and pH in pure aqueous solution within 2 min. More importantly, this dual-functional nanoprobe demonstrates the capability of discerning cancerous cells from normal cells, as evidenced by the fact that cancerous HepG2 cells in tumor microenvironment exhibit substantially higher red fluorescence and significantly lower green fluorescence than normal HL-7702 cells. The simultaneous, real-time fluorescence imaging of multiple analytes in a living system could be significant for cell analysis and tracking, cancer diagnosis, and even fluorescence-guided surgery of tumors.

Nitrogen, sulfur, phosphorus, and chlorine co-doped carbon nanodots (NSPCl-CNDs) were fabricated by acid-base neutralization and exothermic carbonization of glucose. The obtained NSPCl-CNDs possess excellent fluorescence properties and good biocompatibility. Curcumin (Cur) can dramatically quench the fluorescence of NSPCl-CNDs based on a synergistic effect of electrostatic interaction, inner filter effect, and static quenching, so a “turn-off” fluorescent probe for Cur detection was constructed with linear ranges of 0.24–13.16 μM and 13.62–57.79 μM. The LOD and LOQ of this fluorescent probe for Cur are 8.71 nM and 29.03 nM, respectively. More importantly, the fluorescence of the NSPCl-CNDs-Cur system can be recovered by europium ion (Eu3+), so a “turn-on” fluorescent probe for Eu3+ determination was established. The linear range, LOD, and LOQ for the detection of Eu3+ were 2.36–32.91 μΜ, 73.29 nM, and 244.30 nM, respectively. The proposed fluorescence methods were successfully utilized for Cur and Eu3+ determination in real samples with recoveries in the range 95.64–104.13% and 97.06–98.70%, respectively. Furthermore, the qualitative analysis of Cur can be realized by reagent strips with satisfying results. Finally, the as-constructed “off-on” fluorescent probe was successfully used to sequentially analyze Cur and Eu3+ at the cellular level. This method is simple and easy to implement, manifesting that NSPCl-CNDs have potential application value in fluorescent probing, food and drug testing, environmental monitoring, and cellular labeling.

A point-of-care (POC) immunoassay was established for the sensitive and rapid detection of pathogenic Escherichia coli O157:H7, using magnetic Fe3O4 organic-inorganic composites (Ab@Fe3O4) for immunomagnetic separation, nanozyme platinum nanoparticle (PtNp) organic-inorganic composites (Ap@PtNp) for signal amplification, and thermometer readings. Antibodies and Fe3O4 were incubated in Cu2+ phosphate buffer to synthesize the magnetic composite Ab@Fe3O4 with antibodies, to specifically capture E. coli O157:H7. Antimicrobial peptides and PtNp were incubated in Cu2+ phosphate buffer to synthesize the signal composites Ap@PtNp with antimicrobial peptides (magainin I), recognizing and labeling E. coli O157:H7. In the presence of E. coli O157:H7, magnetic microcomposites targeted bacteria and signal microcomposites to form the sandwich structure: Ab@Fe3O4-bacteria-Ap@PtNp for magnetic separation. Ap@PtNp of signal composites catalyzed H2O2 to generate thermo-signals (temperature rise), which were determined by a thermometer. This point-of-care bioassay detected E. coli O157:H7 in the linear range of 101–107 CFU mL−1 and with a detection limit of 14 CFU mL−1.

Testing gluten content in food, before it reaches the consumer, becomes a major challenge where cross-contamination during processing and transportation is a very common occurrence. In this study, a microfluidic electrochemical aptasensing system for the detection of gliadin has been proposed. The fabrication of the sensor involves its modification by using a combination of 2D nanomaterial molybdenum disulfide (MoS2)/graphene with the addition of gold (Au) nanoparticles. Aptamers, a short string of nucleotide bases that are very specific to gliadin, were used in this sensor as the biomarker. The electrochemical standard reduction potential of the ferro-ferricyanide indicator was found to be ~ 530 mV. This setup was integrated with a unique polydimethylsiloxane (PDMS)-based flexible microfluidic device for sample enrichment and portability. The results of this sensor show that the limit of detection was 7 pM. The total sample assay time was 20 min and a good linear range was observed from 4 to 250 nM with an R2 value of 0.982. Different flour samples sourced from the local market were tested and interfering molecules were added to ensure selectivity. The study shows promise in its applicability in real-time gliadin detection. Graphical abstract

A novel aluminum terephthalate/Fe2O3 nanocomposite was synthesized by the addition of Fe2O3 nanoparticles into a reaction solution containing aluminum terephthalate MOF. The synthesized nanocomposite was successfully used as a fiber coating material for solid-phase microextraction (SPME) of six organophosphorus compounds (OPPs) from river water, grape juice, and tea samples. The effect of different parameters on the efficiency of SPME including desorption temperature and time, extraction temperature and time, salt concentration, pH, and agitation were thoroughly studied. The OPPs were detected and determined using GC-MS. According to the findings, a wide linear range (0.15–800 μg kg−1), low limit of detection (0.04–10 μg kg−1), and high recoveries from spiked samples (87.5–112%) were achieved with low inter-day relative standard deviation (3.2–6.7%, n = 5). The MIL-53(Al)/Fe2O3 nanocomposite showed a high extraction ability towards OPPs, and hence, it can be considered a promising adsorbent for the extraction of various pesticides in complex matrices like tea and juice. Graphical abstract

A novel colorimetric sheet based on Griess reagent–doped mesoporous silica nanoparticles was developed for nitrite detection. Griess reagent was adsorbed on long–range ordered hexagonal mesoporous silica nanoparticles and developed ink–bottle pores with some disorder. When the modified nanoparticles were bound using starch to fabricate a thin (~ 313 μm) colorimetric sheet, spherical particles with a rougher surface and some distortion of their mesoporosity were observed. The sheet was used in conjunction with digital image colorimetry (DIC) and provides a wide linear range of 0.05 to 2.50 mg L−1 with a low detection limit (15.0 μg L−1–NO2−, equal to 4.5 μg L−1 NO2−–N), good inter-day precision (1.93%RSD), and excellent precision (2.67% relative error). The colorimetric sensors produced from the sheet costs only 0.04 USD each, while the DIC uses a standard smartphone for photographic detection. The method developed offers an easier and cheaper means of conducting rapid on-site determination of nitrite in water with reliable quantitative results.

An electrochemical immunosensor based on ferrocene (Fc)-functionalized nanocomposites was fabricated as an efficient electroactive signal probe to amplify electrochemical signals for Salmonella typhimurium detection. The electrochemical signal amplification probe was constructed by encapsulating ferrocene into S. typhimurium–specific antimicrobial peptides Magainin I (MI)-Cu3(PO4)2 organic-inorganic nanocomposites (Fc@MI) through a one-step process. Magnetic beads (MBs) coupled with antibody were used as capture ingredient for target magnetic separation, and Fc@MI nanoparticles were used as signal labels in the immunoassays. The sandwich of MBs-target-Fc@MI assay was performed using a screen-printed carbon electrode as transducer surface. The immunosensor platform presents a low limit of detection (LOD) of 3 CFU·mL−1 and a linear range from 10 to 107 CFU·mL−1, with good specificity and precision, and was successfully applied for S. typhimurium detection in milk.

Using gold and magnetic nanoparticles co-decorated reduced graphene oxide-tetraethylenepentamine (rGO-TEPA/Au-MNPs) as the magnetic platform for capturing the primary antibody (Ab1), separation and preconcentration of immunocomplex, a novel homogeneous electrochemical immunosensor was successfully developed. The newly prepared magnetic rGO-TEPA/Au-MNPs, compared with MNPs, exhibited better stability and enhanced electrical conductivity attributed to rGO-TEPA, and showed higher biorecognition efficiency due to AuNPs. In addition, Au@PtNPs were prepared and modified with secondary antibody (Ab2) as an efficient signal probe for signal readout. Using carcinoembryonic antigen (CEA) as a model analyte, the prepared immunosensor demonstrated satisfactory properties like high stability, good repeatability and selectivity, wide linear range (5.0 pg mL−1~200.0 ng mL−1) as well as low detection limit (1.42 pg mL−1). The homogenous electrochemical immunosensor was applied to the detection of CEA in human serum and was found to exhibit good correlation with the reference method. Thus, the proposed rGO-TEPA/Au-MNPs-based homogenous immunoassay platform might open up a new way for biomarker diagnosis.

Molecularly imprinted stir-bar coatings were created based on a hydroxylcucurbit[7]uril–paraquat inclusion complex. The inclusion complex that contained paraquat (PQ) as a template and monohydroxylcucurbit[7]uril ((OH)Q[7]) as a monomer was preassembled mainly through cavity inclusion interaction of (OH)Q[7] to form a one-dimensional self-assembly structure. The inclusion complex was anchored chemically on the surface of a glass stir bar with hydroxy-terminated poly(dimethylsiloxane) by the sol–gel technique to obtain a molecularly imprinted polymer-coated stir bar (MIP-SB). The molecularly imprinted coating showed specific adsorption for cationic PQ in aqueous media. Other quaternary amine compounds with a similar structure that coexisted in the solution, such as ethyl-viologen, diquat, and difenzoquat, were almost not extracted by the prepared MIP-SB. The sorptive capacity of the MIP-SB for PQ was nearly four times that of the non-imprinted stir bar (NIP-SB). The recognition mechanism indicated that the selectivity and extraction capacity resulted mainly from the imprinted cavity in the polymer that was formed by a one-dimensional assembly structure consisting of the (OH)Q[7]–PQ inclusion complex. The imprinted cavity was complementary to the PQ in shape, size, and functionality. A method to determine PQ in environmental water and vegetable samples was developed by combining MIP-SB sorptive extraction with HPLC-UV. The linear range was from 100 to 10,000 ng L−1 with a 8.2 ng L−1 detection limit for water samples and 0.02–0.85 mg kg−1 with a 0.005 mg kg−1 detection limit for vegetable samples. The limit of detection for both samples was lower than the EU-established maximum residual levels and that of other previously reported methods. The average recoveries were 70.0–96.1% with a relative standard deviation ≤ 7.6%, which showed the successful application in real sample analysis.

A rapid and sensitive colorimetric assay is described for Salmonella typhimurium (S. typhimurium) detection using urea/phenol red impregnated test paper. Aptamer-modified Fe3O4@Ag multifunctional hybrid nanoprobes (apt-Fe3O4@Ag NPs) were used to specifically captured S. typhimurium; the nanoprobes were quickly etched by H2O2 to form Ag+. The generated Ag+ can inhibit the urease-catalyzed hydrolysis reaction of urea to produce NH4+. Consequently, the as-prepared test paper displayed a yellow color. In the presence of S. typhimurium, the target bacteria can cause aggregation of apt-Fe3O4@Ag NPs, and the deposited Ag on the nanoprobe’s surface is shielded against H2O2-induced oxidative decomposition leading to reduced Ag+ production. The catalytic activity of urease cannot be inhibited completely by inadequate amount of Ag+. An obvious color change from yellow to pink can be monitored directly using our test paper as a result of increased NH4+. The entire assay procedure could be completed within 1 h. A limit of detection of 48 cfu/mL is achieved with a linear range of 1 × 102 to 1 × 106 cfu/mL. The recoveries of S. typhimurium spiked in pure milk samples were 92.48–94.05%.

For the first time, a fiber coating based on copper metal–organic framework was fabricated on an anodized stainless steel wire by an in situ electrosynthesis approach. The fiber was used for the preconcentration and determination of methamphetamine by headspace solid-phase microextraction followed by gas chromatography–flame ionization detection. The electrosynthesis of the fiber coating was performed under a constant potential of − 1.7 V by controlling the electrogeneration of OH− in a solution containing sodium nitrate as the probase, 1,2,4,5-benzenetetracarboxylate acid as the ligand and copper nitrate as the cation source. The coating was characterized using field emission scanning electron microscopy, energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, and thermogravimetric analysis. The effective parameters on the electrosynthesis, extraction, and desorption processes were thoroughly optimized. Under the optimized conditions, metamphetamine (MAP) was quantified over a linear range of 0.90–1000.0 ng mL−1 with R2 > 0.997. A limit of detection of 0.1 ng mL−1 was achieved, and intra- and inter-day relative standard deviations were found within the range 3.0–4.4% and 2.8–3.9%, respectively. Finally, the method was successfully applied to determination of MAP in urine samples with good recoveries in the range 85.0–102.5%.

A series of haptens were rationally designed for producing monoclonal antibodies specific for EC and a simple fluorescence immunoassay platform was developed for the sensitive determination of EC based on alkaline phosphatase (ALP)-triggered Cu+ quenching of CdSe quantum dots (QDs). It was noted that Cd as a fluorescence substrate in CdSe QDs can be selectively substituted by Cu+ that resulted in a more significant fluorescence quenching in comparison with Cu2+. Meanwhile, because ALP catalyzed ascorbic acid phosphate and then assisted the transformation of Cu2+ to Cu+, the change in fluorescence intensity was found to be proportional to ALP concentration. After simple magnetic separation, the sensitivity and linear range of the established assay were improved approximately 53-fold and an order of magnitude, respectively, when compared with the conventional ELISA. The proposed platform was able to both amplify the signal and eliminate matrix interferences, making it a promising to determine EC as well as other contaminants in complex food matrix in a highly sensitive and simple manner. Graphical abstract.

A series of three-dimensional magnetic covalent organic frameworks were designed and synthesized via monomer selection, coating thickness optimization, and composite strategy transformation. Their structure properties including morphology, functional group, surface area, and pore size were characterized. The relationship between the structural properties and analytical performance was systematically investigated by density functional theory calculation and batch extraction experiments for polycyclic aromatic hydrocarbons. It is proven that the extractant modified by monomer 1,4-phthalaldehyde provides a high affinity for high molecule weight polycyclic aromatic hydrocarbons and the right balance between extraction and elution efficiency. The relationship between coating thickness and mass transfer rate of polycyclic aromatic hydrocarbons was studied by accurate tuning of coating layers via layer-by-layer method. A mathematical model was derived and employed to determine that two coating layers were sufficient to provide the highest extraction efficiency with the shortest equilibrium time. The extractants synthesized by two different composite strategies (layer-by-layer and one-step) show opposite selectivity for polycyclic aromatic hydrocarbons. After optimization of the extraction conditions, dispersed solid-phase extraction coupled with gas chromatography-mass spectrometry method was developed providing a wide linear range (5–500 ng L−1), good linearity (R2 > 0.9923), high precision in intra-day (RSD%

An ultrasensitive sandwich electrochemiluminescence (ECL) biosensor was designed for determination of concanavalin A (ConA) through the specific carbohydrate-ConA interactions. Three-dimensional porous metal-organic framework (Zn-MOF) was synthesized, which loaded a large amount of luminescent reagents as luminol by encapsulating into its pores to form Zn-MOF@luminol complex. Interestingly, Zn-MOF also acted as the coreactant accelerator in the luminol-H2O2 ECL system. This Zn-MOF@luminol complex was used as the signal probe to achieve a super strong and stable ECL signal. In addition, three-dimensional hierarchical molybdenum disulfide nanoflower and multiwalled carbon nanotubes complex (MoS2NF@MWCNTs) with peroxidase-mimicking enzyme property were used as a substrate to modify the glassy carbon electrode to further enhance the ECL signal of luminol by promoting decomposition of H2O2 into reactive oxygen species (ROSs). In addition to the horseradish peroxidase (HRP) catalysis effect on the luminol ECL signal, a triple amplified ConA sandwich ECL sensor with high sensitivity sensor was constructed. The linear range for ConA detection was from 0.5 pg/mL to 100 ng/mL with a detection limit of 0.3 pg/mL (S/N = 3). The recovery test for ConA in human serum samples was performed with satisfactory results.