Switchable DNA-Based Peroxidases Controlled by a Chaotropic Ion**

Tanner G. Hoog; Matthew R. Pawlak; Lauren M. Aufdembrink; Benjamin R. Bachan; Matthew B. Galles; Nicholas B. Bense; Katarzyna P. Adamala; Aaron E. Engelhart

doi:10.1002/cbic.202200090

Switchable DNA-Based Peroxidases Controlled by a Chaotropic Ion**

Tanner G. Hoog, Matthew R. Pawlak, Lauren M. Aufdembrink, Benjamin R. Bachan, Matthew B. Galles, Nicholas B. Bense, Katarzyna P. Adamala, Aaron E. Engelhart

Research output: Contribution to journal › Article › peer-review

Abstract

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.

Original language	English (US)
Article number	e202200090
Journal	ChemBioChem
Volume	23
Issue number	9
DOIs	https://doi.org/10.1002/cbic.202200090
State	Published - May 4 2022

Bibliographical note

Funding Information:
Several figures in this manuscript were prepared using BioRender.com. We thank Loren Williams and George Perry for helpful discussions. The imaging apparatus used here was developed as part of the RockSat‐C 2018 sounding rocket program, sponsored by the Colorado Space Grant Consortium and NASA Wallops; we thank the NASA PAXC team members for helpful discussions. This work was supported by NASA Contract 80NSSC18K1139 under the Center for Origin of Life (to A.E.E. and K.P.A.).

Publisher Copyright:
© 2022 The Authors. ChemBioChem published by Wiley-VCH GmbH.

Keywords

DNA
chaotropes
electron transfer
nanotechnology
synthetic biology
Hemin
Peroxidases
G-Quadruplexes
Perchlorates

PubMed: MeSH publication types

Journal Article
Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.

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10.1002/cbic.202200090

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title = "Switchable DNA-Based Peroxidases Controlled by a Chaotropic Ion**",

abstract = "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.",

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author = "Hoog, {Tanner G.} and Pawlak, {Matthew R.} and Aufdembrink, {Lauren M.} and Bachan, {Benjamin R.} and Galles, {Matthew B.} and Bense, {Nicholas B.} and Adamala, {Katarzyna P.} and Engelhart, {Aaron E.}",

note = "Funding Information: Several figures in this manuscript were prepared using BioRender.com. We thank Loren Williams and George Perry for helpful discussions. The imaging apparatus used here was developed as part of the RockSat‐C 2018 sounding rocket program, sponsored by the Colorado Space Grant Consortium and NASA Wallops; we thank the NASA PAXC team members for helpful discussions. This work was supported by NASA Contract 80NSSC18K1139 under the Center for Origin of Life (to A.E.E. and K.P.A.). Publisher Copyright: {\textcopyright} 2022 The Authors. ChemBioChem published by Wiley-VCH GmbH.",

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AU - Galles, Matthew B.

AU - Bense, Nicholas B.

AU - Adamala, Katarzyna P.

AU - Engelhart, Aaron E.

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PY - 2022/5/4

Y1 - 2022/5/4

N2 - 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.

AB - 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.

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KW - electron transfer

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Switchable DNA-Based Peroxidases Controlled by a Chaotropic Ion**

Abstract

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Keywords

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