Sensitive Electrochemical Sensor for Glycoprotein Detection Using a Self-Serviced-Track 3D DNA Walker and Catalytic Hairpin Assembly Enzyme-Free Signal Amplification

Abstract

Approaches for the detection of targets in the cellular microenvironment have been extensively developed. However, developing a method with sensitive and accurate analysis for noninvasive cancer diagnosis has remained challenging until now. Here, we reported a sensitive and universal electrochemical platform that integrates a self-serviced-track 3D DNA walker and catalytic hairpin assembly (CHA) triggering G-Quadruplex/Hemin DNAzyme assembly signal amplification. In the presence of a target, the aptamer recognition initiated the 3D DNA walker on the cell surface autonomous running and releasing DNA (C) from the triple helix. The released DNA C as the target-triggered CHA moiety, and then G-quadruplex/hemin, was formed on the surface of electrode. Eventually, a large amount of G-quadruplex/hemin was formed on the sensor surface to generate an amplified electrochemical signal. Using N-acetylgalactosamine as a model, benefiting from the high selectivity and sensitivity of the self-serviced-track 3D DNA walker and the CHA, this designed method showed a detection limit of 39 cell/mL and 2.16 nM N-acetylgalactosamine. Furthermore, this detection strategy was enzyme free and exhibited highly sensitive, accurate, and universal detection of a variety of targets by using the corresponding DNA aptamer in clinical sample analysis, showing potential for early and prognostic diagnostic application.

Electrochemical Monitoring of Sphingosine-1-phosphate-Induced ATP Release Using a Microsensor Based on an Entropy-Driven Bipedal DNA Walker

“…Nevertheless, the application of microelectrodes for ATP detection still poses a significant challenge due to the nonelectroactive and the low abundance of ATP in the complex nervous system. DNA walkers, as an effective signal amplification strategy, can autonomously traverse a predetermined nucleic acid track to capture or release signal molecules, thereby amplifying the signal. − For instance, Miao and Tang developed a bipedal DNA walker using an amplified electrochemical strategy for miRNA detection, achieving a remarkably low limit of detection of 10 aM . Additionally, they introduced DNA nanostructure transitions to prepare a DNA bipedal walking nanomachine, incorporating dual-signal amplification for direct detection of circulating tumor DNA.…”

Rolling Circle Amplification/G‐Quadruplex‐Based Dual‐Signal Ratiometric Electrochemical Aptasensor for Ultrasensitive Detection of Pathogenic Bacteria

“…[13][14][15] For example, as has been reported, most electrochemical biosensors use a single electrochemical signal for bacterial detection, reflecting the concentration through the output of a single signal, and this single signal output is often susceptible to internal or external factors such as electrodes, instruments and environment, that can result in poor stability, reproducibility, and reliability of the results. [16][17][18] In order to overcome the above problems, recent efforts have been made to exploit dual signal outputs in electrochemical sensors, namely, the ratio-sensing strategy. [19][20][21] Ratiometric electrochemical sensors take advantage of dual electrochemical signals and use the ratio of two signals as the output signal, rather than the absolute value of a single signal, compared to traditional single-signal strategies, thereby reducing background signal interference and improving reproducibility, accuracy, and sensitivity of detection.…”

Enzyme-free electrochemical sensor platforms based on transition metal nanostructures for clinical diagnostics

“…, the enzyme-free electrochemical detection of lactic acid and glucose has received serious consideration and made significant development in recent years. 28,29 Over recent years, there have been several enzyme-free electrochemical sensors utilizing a variety of nanostructured materials, comprising noble metallic nanoparticles (gold (Au), platinum (Pt), silver (Ag), and their alloy metals), 30–32 transition metal oxides (copper oxide (CuO), nickel oxide (NiO), manganese oxide (MnO 2 ), Co 3 O 4 , and their nanocomposites), 33,34 graphene nanocomposites, 35 metal–organic frameworks, 36,37 and transition metal chalcogenides, 15,38–45 were developed. As depicted in Fig.…”