Journal
ACS NANO
Volume 14, Issue 7, Pages 8317-8327Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c02329
Keywords
detachable DNA circuit; intermolecular triplex; pH-responsive; resettable self-assembly; spherical nucleic acids
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Funding
- National Natural Science Foundation of China [21991132]
- Fundamental Research Funds for the Central Universities [WK2060200026]
- China Postdoctoral Science Foundation [2018M630708]
- National Postdoctoral Program for Innovative Talents [BX20180285]
- Foundations of Educational Committee of Anhui Province [KJ2019A0719]
- Excellent Talent Foundation of Education Department of Anhui Province [gxyq2019066]
- 136 talent plan of Hefei Normal University
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Toehold-mediated strand displacement reaction, the fundamental basis in dynamic DNA nanotechnology, has proven its extraordinary power in programming dynamic molecular systems. Programmed activation of the toehold in a DNA substrate is crucial for building sophisticated DNA devices with digital and dynamic behaviors. Here we developed a detachable DNA circuit by embedding a pH-controlled intermolecular triplex between the toehold and branch migration domain of the traditional linear substrate. The reaction rate and the on/off state of the detachable circuit can be regulated by varying the pHs. Similarly, a two-input circuit composed of three pH-responsive DNA modules was then constructed. Most importantly, a resettable self-assembly system of spherical nucleic acids was built by utilizing the high detachability of the intermolecular triplex structure-based DNA circuit. This work demonstrated a dynamic DNA device that can be repeatedly operated at constant temperature without generating additional waste DNA products. Moreover, this strategy showed an example of recycling waste spherical nucleic acids from a self-assembly system of spherical nucleic acids. Our strategy will provide a facile approach for dynamic regulation of complex molecular systems and reprogrammable nanoparticle assembly structures.
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