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Abstract Herein, a label-free and double recognition–amplification (LDRA) strategy for carcinoembryonic antigen (CEA) detection was developed, based on a new designed dual-function messenger probe (DMP) coalescing with DNA tetrahedron probes (DTPs) and hybridization chain reaction (HCR). The DMP possess dual-function to replace CEA for specific interface hybridization and initiate hybridization chain reaction. The interfacial hybridization event was quantitatively converted to an electrochemical signal by using hemin/G-quadruplex (h-Gx) formed after the hybridization chain reaction. Self-assembled DNA tetrahedron probes, which were readily decorated on an electrode surface as a scaffold with rigid support and ordered orientation, enabled the highly efficient strands hybridization and greatly increased target accessibility as well as significantly decreased noise. The proposed assay integrated dual recognition processes and HCR signal amplification processes, achieving the identification of low concentration of CEA as detection limit of 18.2 fg mL−1 (S/N = 3) and wider linearity range of 0.0001 ng mL−1–50 ng mL−1. A new electrochemical sensing method was proposed for CEA detection and used in real clinical samples. The obtained results were good consistency with those of clinical diagnosis. Highlights • A new dual-function messenger probe (DMP) was designed for specific interface hybridization and initiate HCR. • The employment of DNA tetrahedron probes increased the probability of hybridization and reduced the background signal. • The synergetic combination of DMP and hybridization chain reaction (HCR) improved the sensitivity of the detection. • The proposed strategy was used to analysis CEA in real sample and achieved a detection limit as low as 18.2 fg/mL. [ABSTRACT FROM AUTHOR]

This work designed an artificial substrate peptide to synthesize peptide-hemin/G-quadruplex (peptide-DNAzyme) conjugates. In addition to enhancing catalytic activity of hemin/G-quadruplex, the peptide could also be induced and cleaved by prostate specific antigen (PSA). It was the first report on peptide-DNAzyme conjugates in application of the peptide biosensor. The polyethyleneimine-reduced graphene oxide@hollow platinum nanotubes (PEI-rGO@PtNTs) nanocomposites were cast on the glassy carbon electrode in order to form the interface of biocompatibility and huge surface area for bioprobes immobilization. In absence of PSA, the peptide-DNAzyme conjugates retained intact on the surface of the electrode to produce a strong response signal. But in presence of PSA, the peptide-DNAzyme conjugates were destroyed to release electron mediators, resulting in dramatical decrease of the electrochemicl signal. Therefore, the method had high sensitivity and super selectivity with the limit of detection calculated as 2.0 fg/mL. Furthermore, the strategy would be promising to apply for other proteases by transforming the synthetic peptide module of target. [ABSTRACT FROM AUTHOR]

Personal glucose meter (PGM) is one of the most commercially available POC (point-of-care) devices for monitoring the level of glucose reliably, yet its non-glucose quantification ability is limited since such strategy needs ingenious interface design and tedious enzyme conjugation. Herein, we constructed a portable and sensitive platform that can detect non-glucose target by combining enzyme-encapsulated zeolitic imidazole framework-90 (ZIF-90) with personal glucose meter. ZIF-90 is an ideal carrier and susceptor due to the extraordinary capability of packaging enzyme and stimuli-responsiveness. We selected adenosine-5′-triphosphate (ATP) as the target model of non-glucose analytes. Upon ATP-induced decomposition of MOF, the released enzyme (glucose oxidase or invertase) catalyzed substrate and gave rise to the change of the glucose concentration for PGM assay. This method determined ATP with a remarkably sensitivity of 233 nM and effective recovery in real serum samples. Our strategy provides a facile and practical approach for measuring the non-glucose target using PGM, and could potentially be applied in bimolecular detection in point-of-care diagnosis. [Display omitted] [ABSTRACT FROM AUTHOR]

Rapid and effective diagnosis of communicable disease is one of the critical issues of the modern society, especially for detecting different targets at the same time. In this work, a grafting homogenous electrochemical biosensing strategy is proposed by integrating of reverse proximity ligation and exonuclease III (Exo III) assisted target circulation to analyze hepatitis B (HBV) and human immunodeficiency (HIV). Specially, a two-wing nanodevice (TWD) with two detection paths is elaborately designed based on analogous proximity ligation assay. The reverse proximity ligation process provides a new way of signal conversion and amplification, what accomplished by demolishing the TWD in the presence of targets. Meanwhile, a vast number of signal probes are released via Exo III assisted target circulation. Then the signal probes are grafted on the universal sensing interface, which is decorated with graftable tetrahedron DNA (GTD). These lead to a highly amplified electrochemical signal. Compared with the conventional strategies, the grafting homogenous electrochemical biosensing strategy not only achieves convenient sensitive detection of multiple communicable diseases DNA simultaneously, but also performs well in the detection of sole target. This strategy effectively decreases the background, homogenizes the distribution of probes, and avoids the complex and time-consuming modification process of the working electrode, which holds great potential application in early diagnosis for communicable disease in the future. • A two wing nanodevice is constructed by using the principle of analogous proximity ligation assay. • By using the principle of reverse proximity ligation assay, a new manner for conversing and amplifying the electrochemical signal is demonstrated for the first time. • The graftable tetrahedron DNA is immobilized on the electrode to construct a universal grafting sensing interface. • This strategy can be used to detect multiple targets simultaneously, and can also perform well in detection of sole target. [ABSTRACT FROM AUTHOR]

Herein, a robust and highly ordered three-dimensional electrochemical DNA (3D E-DNA) biosensor was proposed, and its orientation was controlled from top down by poly adenine oligonucleotides (polyA-ODNs)-mediated rolling motor (PRM) and graftable tetrahedron DNA (GTD). The GTD with a grafting domain was immobilized on the electrode surface to construct a well-organized sensing interface and controlled the orientation and distribution of the whole system at the "bottom" of this biosensor. The polyA-ODNs regulated the direction and density of the leg DNA attached on PRM at the "top" of the biosensor. The motion was achieved through the target induced cyclic cleaving, which triggered the motor rolling rather than walk. Impressively, the duplex strand DNA (dsDNA) formed after grafting, as a girder, provided a stable support to the soft long single strand (ssDNA), which facilitated the formation of the catalytic center, elevated the efficiency of the rolling cleavage. Under the optimal conditions, the designed biosensor exhibited a lower limit of 0.17 nM and wide linear range from 0.5 nM to 1.5 μM for adenosine rapid detection. Unique dual orientation regulated characteristics of the system increased the probability hybridization enormously and improved the motion efficiency significantly, which offered new avenue of DNA nanomachines development in biosensor platform. • The 3D electrochemical DNA biosensor is highly ordered with the density and orientation are well controlled from top down. • The rolling motor is well-designed and triggered rolling by target induced cyclic cleaving. • A distinctive graftable tetrahedron DNA is proposed to constructed 3D sensing surface regulated the density of the whole system. • The graftable tetrahedron can be used to simultaneously construct different sensing strategies without re-synthesizing according to the target. • Poly adenine prompts the substrate DNA of rolling motor to adopt an upright conformation and program the direction and density of substrate DNA precisely. [ABSTRACT FROM AUTHOR]