DNA-modulated single-atom nanozymes with enhanced enzyme-like activity for ultrasensitive detection of dopamine.
Zhihan WuWendong LiuHaijun LuHongyan ZhangZhe HaoFanghua ZhangRuizhong ZhangXiyan LiLibing ZhangPublished in: Nanoscale (2023)
Despite the current progress in optimizing and tailoring the performance of nanozymes through structural and synthetic adaptation, there is still a lack of dynamic modulation approaches to alter their catalytic activity. Here, we demonstrate that DNA can act as an auxiliary regulator via a straightforward incubation method with Fe-N-C single-atom nanozymes (SAzymes), causing a leap in the enzyme-like activity of Fe-N-C from moderate to a higher level. The DNA-assisted enhancement is attributed to the increased substrate affinity of Fe-N-C nanozymes through electrostatic attraction between the substrate and DNA. Based on the prepared DNA/Fe-N-C system, colorimetric sensors for dopamine (DA) detection were constructed. Surprisingly, the incorporation of DNA not only enabled the detection of DA in a low concentration range, but also greatly improved the sensitivity with a 436-fold decrease in detection limit. The quantitative determination of DA was achieved in two-segment linear ranges of 0.01-4 μM and 5-100 μM with an ultralow detection limit of 9.56 nM. The DNA/Fe-N-C system shows superior performance compared to the original Fe-N-C system, making it an ideal choice for nanozyme-based biosensors. This simple design approach has paved the way for enhancing nanozyme activity and is expected to serve as a general strategy for optimizing biosensor performance.
Keyphrases
- circulating tumor
- label free
- cell free
- single molecule
- loop mediated isothermal amplification
- gold nanoparticles
- real time pcr
- nucleic acid
- circulating tumor cells
- molecular dynamics
- uric acid
- sensitive detection
- aqueous solution
- nitric oxide
- amino acid
- wastewater treatment
- molecular dynamics simulations
- hydrogen peroxide