Switchable DNA‐Based Peroxidases Controlled by a Chaotropic Ion

Here we demonstrate a switchable DNA electron‐transfer catalyst, enabled by selective destabilization of secondary structure by the denaturant, perchlorate. The system is comprised of two strands, one of which can be selectively switched between a G‐quadruplex and duplex or single‐stranded conformat...

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Bibliographic Details
Published in:Chembiochem : a European journal of chemical biology 2022-05, Vol.23 (9), p.e202200090-n/a
Main Authors: Hoog, Tanner G., Pawlak, Matthew R., Aufdembrink, Lauren M., Bachan, Benjamin R., Galles, Matthew B., Bense, Nicholas B., Adamala, Katarzyna P., Engelhart, Aaron E.
Format: Article
Language:English
Subjects:
Catalysis
Catalysts
chaotropes
Deoxyribonucleic acid
Destabilization
Dilution
DNA
DNA structure
electron transfer
G-Quadruplexes
Hemin
nanotechnology
Perchlorate
Perchlorates
Perchloric acid
Peroxidase
Peroxidases
Protein structure
Secondary structure
Switching
synthetic biology
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Summary:Here we demonstrate a switchable DNA electron‐transfer catalyst, enabled by selective destabilization of secondary structure by the denaturant, perchlorate. The system is comprised of two strands, one of which can be selectively switched between a G‐quadruplex and duplex or single‐stranded conformations. In the G‐quadruplex state, it binds hemin, enabling peroxidase activity. This switching ability arises from our finding that perchlorate, a chaotropic Hofmeister ion, selectively destabilizes duplex over G‐quadruplex DNA. By varying perchlorate concentration, we show that the DNA structure can be switched between states that do and do not catalyze electron‐transfer catalysis. State switching can be achieved in three ways: thermally, by dilution, or by concentration. The chaotropic anion perchlorate selectively destabilizes guanine‐rich double stranded DNA, allowing it to form a G‐quadruplex that can complex with hemin, forming a peroxidase DNAzyme. This affords a pH‐ and ATP‐independent means of switching DNA secondary structure and controlling electron‐transfer reactions.
ISSN:1439-4227
1439-7633
DOI:10.1002/cbic.202200090