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Published November 11, 2019 | Supplemental Material + Submitted
Journal Article Open

Regulating Transition‐Metal Catalysis through Interference by Short RNAs

Abstract

Herein we report the discovery of a Au^I–DNA hybrid catalyst that is compatible with biological media and whose reactivity can be regulated by small complementary nucleic acid sequences. The development of this catalytic system was enabled by the discovery of a novel Au^I-mediated base pair. We found that Au^I binds DNA containing C-T mismatches. In the Au^I–DNA catalyst's latent state, the Au^I ion is sequestered by the mismatch such that it is coordinatively saturated, rendering it catalytically inactive. Upon addition of an RNA or DNA strand that is complementary to the latent catalyst's oligonucleotide backbone, catalytic activity is induced, leading to a sevenfold increase in the formation of a fluorescent product, forged through a Au^I-catalyzed hydroamination reaction. Further development of this catalytic system will expand not only the chemical space available to synthetic biological systems but also allow for temporal and spatial control of transition-metal catalysis through gene transcription.

Additional Information

© 2019 Wiley-VCH. Issue Online: 04 November 2019. Version of Record online: 21 August 2019. Accepted manuscript online: 16 July 2019. Manuscript revised: 24 June 2019. Manuscript received: 01 May 2019. Financial support was generously provided by the Packard Foundation and Pew Charitable Trusts (to H.M.N.). We thank Prof. F. Dean Toste (UC Berkeley) for inspiration and Dr. Jeff Vieregg (University of Chicago) for useful discussions. We thank the UCLA Molecular Instrumentation Center for NMR instrumentation and Mass Spectrometry. This material is based on work supported by the National Institutes of Health under instrumentation grant no. 1S10OD016387-01. The authors declare no conflict of interest.

Attached Files

Submitted - regulating-transition-metal-catalysis-through-interference-by-short-rn-as.pdf

Supplemental Material - anie201905333-sup-0001-misc_information.pdf

Files

anie201905333-sup-0001-misc_information.pdf

Additional details

Created:
August 22, 2023
Modified:
October 23, 2023