查看更多>>摘要：Dual-signal strategy has great potential in improving the accuracy and sensitivity of cancer biomarker determination. However, most sensors based on nanomaterials as signal amplification usually output single detectable signal. It is still a challenge to achieve dual-signal sensing of biomarkers with nanomaterials as signal amplification. Herein, MnO@C nanocomposite was prepared with Mn-MOF-74 as precursor by pyrolysis. It possesses bidirectional electrocatalytic ability toward both oxidation and reduction of H2O2 for its fully exposed crystal facets. After loading AuNPs, MnO@C@AuNPs can connect aptamer (Apt) via Au-S and then as a signal amplification for the construction of sandwich-type aptasensor for dual-signal electrochemical sensing of cancer biomarker. Thus, taking mucin 1 (MUC1) as a model system. The aptasensor has the parallel output of differential pulse voltammetry (DPV) and chronoamperometry responses based on oxidation and reduction of H2O2, respectively, which implemented sensitive and accurate measurements to avoid false results. The linear response ranges of 0.001 nM-100 nM (detection limit of 0.31 pM) for DPV technique and 0.001 nM-10 nM (detection limit of 0.25 pM) for chronoamperometry technique were obtained. It opens up a new way to design elegant dual-signal aptasensors with potential applications in early disease diagnosis.
Papavasileiou, Anastasios, VTrachioti, Maria G.Hrbac, JanProdromidis, Mamas, I...
9页
查看更多>>摘要：Saliva represents one of the most useful biological samples for non-invasive testing of health status and diseases prognosis and therefore, the development of advanced sensors enabling the determination of biomarkers in unspiked human whole saliva is of immense importance. Herein, we report on the development of a screen printed graphite sensor modified with carbon nanomaterials generated by spark discharge for the determination of guanine and adenine in unspiked human whole saliva. The designed sensor was developed with a "green", extremely simple, fast (16 s), fully automated "linear mode" sparking process implemented with a 2D positioning device. Carbon nanomaterial-modified surfaces exhibit outstanding electrocatalytic properties enabling the determination of guanine and adenine over the concentration range 5 1000 nM and 25 1000 nM, while achieving limits of detection (S/N 3) as low as 2 nM and 8 nM, respectively. The sensor was successfully applied to the determination of purine bases in unspiked human whole saliva following a simple assay protocol based on ultrafiltration that effectively alleviates biofouling issues. Recovery was 96-108%.
查看更多>>摘要：Asymptomatic infection of COVID-19 is a global threat for public health. Unfortunately, the study about metabolic dysregulation of asymptomatic infection is barely investigated. Here, we performed carboxylic submetabolome profiling of serum from 62 asymptomatic and 122 control individuals, by a highly sensitive chemical isotope labelling method. Twenty-one discriminative carboxylic features, including 12-hydroxyeicosatetraenoic acid, cholic acid, glycoursodeoxycholic acid and 15,16-dihydroxyoctadeca-9,12-dienoic acid were discovered to be dysregulated in asymptomatic patients. This panel containing 21 carboxylic features could accurately identify asymptomatic patients based on a random forest model, providing an accuracy of 85.7% with only 3.6% false positive rate and 7.1% false negative rate. The dysregulated metabolites found in asymptomatic patients covered several important pathways, such as arachidonic acid metabolism, synthesis of bile acid, beta-oxidation of fatty acids, activation of macrophage and platelet aggregation. This work provided valuable knowledge about serum biomarkers and molecular clues associated with asymptomatic COVID-19 patients.
查看更多>>摘要：Determination of urinary or serum N-acetyl-beta-D-glucosaminidase (NAG) activity as a tissue damage indicator is widely used in diagnosis of various pathologies, including diabetic nephropathy. Early and rapid biomarker detection is an important element of medical diagnosis, facilitating prompt therapeutic decisions and prognosis evaluation. Herein, we present a modified sensing approach for a rapid and reliable NAG activity determination in complex media using surface-enhanced Raman spectroscopy (SERS). Porous silicon (PSi) Fabry-Pe ' rot interferometers were redesigned as sensitive SERS platforms utilizing the vast inherent surface area for silver (Ag) nanoparticles embedment. Interaction of the porous nanostructures with specific NAG-enzymatic products produces an indicative spectral fingerprint proportional in magnitude to its concentration. The sensitivity of Ag-PSi SERS substrates was evaluated in complex matrices presenting sufficient limits of detection compared with other advanced assays and techniques (0.07, 0.47 and 0.50 mU mL(-1) for urine, milk and plasma, respectively). The augmented optical performance revealed recovery values of 96-109%, indicating successful and selective NAG recognition in biological fluids. Finally, the potential applicability of the suggested prototype for real-life scenarios was evaluated in vivo, in a model of insulin-dependent diabetes induced in sheep. Overall, the robust data confirm the application of SERS analysis for early diagnosis of pathology and for evaluation of clinical responses to pharmacological treatments.
查看更多>>摘要：Amitriptyline and its metabolite, Nortriptyline are commonly used tricyclic antidepressant (TCA) drugs that are electrochemically active. In this work, the performance characteristics of a plasticized PVC membrane-coated glassy carbon (GC) electrode are described for the voltammetric quantification of Amitriptyline and Nortriptyline in whole blood. The highly lipophilic Amitriptyline and Nortriptyline preferentially partition into the plasticized PVC membrane where the free drug is oxidized on the GC electrode. The concentrations of the drugs in the membrane are orders of magnitude larger than in the sample solution, resulting in superb limit of detection (LOD) of the membrane-coated voltammetric sensor: 3 nmol/L for Amitriptyline and 20 nmol/L for Nortriptyline. Conversely, hydrophilic components of the sample solution, e.g., proteins, the protein-bound fraction of the drugs, and electrochemically active small molecules are blocked from entering the membrane, which provides exceptional selectivity for the membrane-coated sensor and feasibility for the measurements of Amitriptyline in whole blood. In this work, the concentrations of Amitriptyline and Nortriptyline were determined in whole blood using the sensor and the results of our analysis were compared to the results of the standard HPLC-MS method. Based on our experience, the one-step voltammetric methods with the membrane-coated sensor may become a real alternative to the significantly more complex HPLC-MS analysis.
查看更多>>摘要：Biothiols, associated with multiple physiological and pathological processes, have structural similarities. Monitoring Biothiols selectively in organisms is of great significance. Burdened by the aggregation-caused quenching (ACQ) effect, the applications of conventional biothiols fluorescent probes are extremely limited. Herein, we developed a "turn-on" type aggregation-induced emission (AIE) fluorescent probe BQM-NBD, which was composed of a BQM-OH fluomphore molecule with AIE effect and the recognition group 7-nitro-1,2,3-benzoxadiazole (NBD). Non-fluorescent BQM-NBD produces strong fluorescence after the addition of cysteine (Cys) or homocysteine (Hcy). BQM-NBD exhibited excellent linearity for selective detection of Cys (0-100 Mm) and Hcy (0-50 mu M) with detection limits of 6.0 x 10(-8) M and 8.4 x 10(-8) M, respectively. Simultaneously, after treatment with glutathione (GSH), it appeared no fluorescence. The results demonstrated BQM-NBD exhibited good selectivity to Cys/Hcy. Furthermore, BQM-NBD was successfully performed in the imaging of Cys in living cells with low cytotoxicity, which provides a feasible strategy for the selective detection of Cys in the living system.
查看更多>>摘要：Nowadays, molecularly imprinted polymers (MIPs) coated silica stationary phases (SPs) have aroused great attention, owing to their good properties of high selectivity, good stability, facile synthesis procedure and low cost. In this study, zidovudine imprinted polymers coated silica stationary phases (MIPs/SiO2 SPs) were synthesized by surface imprinting technique using zidovudine as the template molecule, methacrylic acid as the functional monomer, ethylene glycol dimethacrylate as the cross-linking agent, azobisisobutyronitrile as the initiator, and bare silica spheres (particle size, 5 mu m; pore size, 20 nm) as substrates. In the process, reagents with low concentration were used to prepare thin layer of MIPs coating on the surface of silica microbeads. The properties of the materials were characterized by scanning electron microscope (SEM), fourier transform infrared spectrometer (FT-IR), carbon elemental analysis and N-2 adsorption-desorption experiment. The obtained SPs were packed into stainless steel columns (2.1 mm x 150 mm) via a slurry method. The prepared columns were applied for separation of nucleoside analogues with similar chemical structures and strong polarity. The retention mechanism of MIPs/SiO2 SPs for nucleoside analogues was investigated carefully. And the chromatographic performances of the resulting MIPs based SPs were superior to those of the commercial SPs. Furthermore, the synthesized MIPs/SiO2 SPs possessed great potentials in separation of ginsenosides. This investigation demonstrated that MIPs based SPs were successfully synthesized and provided a new approach to polar compounds separation and analysis.
查看更多>>摘要：Characterization of alkaloids and new compound discovery become increasing challenging for Gelsemium elegans Benth. (G. elegans), due to the lack of an effective separation method. In this study, we developed a new online heart-cutting + comprehensive (HC) RPLC x RPLC system with pH difference, which was coupled to a mass detector to realize the separation and characterization of alkaloids from G. elegans. 18 Gelsemium standards were used to construct the RPLC x RPLC system with pH difference (pH 3 and 11), and good orthogonality (correlation coefficient 0.3) was obtained. A heart-cutting valve was introduced into the traditional online comprehensive RPLC x RPLC system to remove principal components and improve detection of minor components. The online HC RPLC x RPLC system achieved good resolving power (effective peak capacity 687) in condition of optimized practical factors, like the first-and second-dimension flow rates, modulation period and elution gradient et al. Finally, a total of 256 alkaloids were grouped and tentatively identified, among which 156 were unreported, including a new alkaloid type in G. elegans and many dimeric indole alkaloids, which was an important supplement to the study on chemical constituents of G. elegans.
查看更多>>摘要：Cyclobutane pyrimidine dimers (CPDs) are the major DNA photoproducts of thymine-thymine dinucleotides upon ultraviolet (UV) irradiation. Failure in the repair of damaged DNA may lead to DNA replication errors, DNA mutations, and even cell death. Photoreactivation can mediate the repair of UV-induced DNA lesions by photolyases upon UVA (315-400 nm) or blue light (400-500 nm) irradiation. Herein, the UVC (254 nm)-induced DNA damage and photoenzymatic repair of the CPD products were simultaneously monitored by electrochemical impedance spectroscopy (EIS). The UVC-damaged dT(20) was first immobilized on the gold electrode, and the specific recognition by the anti-CPD antibody leads to significantly increased EIS signals. The electron transfer resistance (R-et) values were linearly proportional to the concentrations of damaged dT(20) ranging from 0.005 to 0.1 mu M, and a detection limit of 3.06 nM was achieved. Using surface plasmon resonance, the equilibrium dissociation constant (K-D) between the CPDs in dT(20) and anti-CPD antibody was estimated to be (3.32 +/- 0.31) x 10-12 M, indicating the strong binding affinity. Evidenced by EIS, the CPDs in the damaged dT(20) could be repaired by the attached DNA photolyase under UVA (365 nm) photoexcitation, and the detachment of the photolyase from the DNA strand was accomplished after completion of the repair process. The repair efficiency was calculated to be 70.0% by EIS, being consistent with that of 71.4% by UV spectroscopy. The electrochemical method is simple, sensitive and straightforward, holding great potential for assaying other types of DNA lesions and their repair processes.
查看更多>>摘要：The assessment of DNA methylation level is an important indicator for the diagnosis and treatment of some diseases. DNA methylation assays are usually based on nucleic acid amplification strategies, which are timeconsuming and complicated in operation procedures. Herein, we proposed a sensitive lanthanide-labelled ICPMS method for DNA methylation analysis that exploited the feature of Human 8-oxoGuanine DNA Glycosylase (hOGG1), which specifically recognizes 8-oxo-G/5mC base pairs to effectively distinguish methylated DNA. A low limit of detection of 84 pM was achieved, and a 0.1% methylation level can be discriminated in the mixture, without any amplification procedure. Compared with commonly used nucleic acid amplification strategies, this proposed method is time-saving and low probability of false positive. Moreover, this work has been successfully validated in human serum samples, the recovery rates is between 96.7% and 105%, and the relative standard deviation (RSD) is in the range of 3.0%-3.5%, indicating that this method has the potential to be applied in clinical and biological samples quantitative analysis.
NSTL
Elsevier