Abstract
In this work, we established a dynamic DNA self-assembly activated hemin-mimetic enzyme system for versatile fluorescent biosensing. The DNA-grafted hemin was utilized not only as the module for dynamic DNA-assembly but also as the tunable mimetic enzyme. In the presence of targets, the entropy-driven dynamic DNA-assembly circuit was initiated and the tagged hemin dimmers with suppressed catalytic activity were disaggregated into activated hemin monomers. Then activated hemin-mimetic enzymes can catalyze non-fluorescent tyramine into fluorescent dityramine, providing a simple, fast and enzyme-free signal amplification strategy for fluorescent biosensing. The designed method was successfully applied to detect target DNA at concentration down to 78 pM with dynamic range from 0.1 to 50 nM in 40 min. Moreover, it was extended to detect small molecule cocaine based on specific aptamer recognition with a detection limit of 4.85 μM in 70 min. Our proposed system showed simple design of oligonucleotides modules for DNA-assembly, preferable mimic enzyme activation mechanism and fast biosensing without extra hemin addition. Thus, this work presented a simple and versatile target-triggered DNA-hemin enzyme assembly system for high-efficiency and enzyme-free signal transduction which would become a potential tool for universal biosensing application.
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