Exponential Amplification Using Photoredox Autocatalysis
Name
exponential-amplification-using-photoredox-autocatalysis.pdf
Description
Accepted version
Size
3.24 MB
Format
Adobe PDF
Checksum (MD5)
043ca9dd2b6b609b9b84fb0e81374548
Author(s)
Kim, Seunghyeon
Martínez Dibildox, Alejandra
Aguirre-Soto, Alan
Sikes Johnson, Hadley
Date Issued
July 2021
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Citation
Kim, Seunghyeon et al. "Exponential Amplification Using Photoredox Autocatalysis." Journal of the American Chemical Society 143, 30 (July 2021): 11544–11553. © 2021 American Chemical Society
Version
Author's final manuscript
Abstract
Exponential molecular amplification such as the polymerase chain reaction is a powerful tool that allows ultrasensitive biodetection. Here, we report a new exponential amplification strategy based on photoredox autocatalysis, where eosin Y, a photocatalyst, amplifies itself by activating a nonfluorescent eosin Y derivative (EYH³⁻) under green light. The deactivated photocatalyst is stable and rapidly activated under low-intensity light, making the eosin Y amplification suitable for resource-limited settings. Through steady-state kinetic studies and reaction modeling, we found that EYH³⁻ is either oxidized to eosin Y via one-electron oxidation by triplet eosin Y and subsequent 1e⁻/H⁺ transfer, or activated by singlet oxygen with the risk of degradation. By reducing the rate of the EYH³⁻ degradation, we successfully improved EYH³⁻-to-eosin Y recovery, achieving efficient autocatalytic eosin Y amplification. Additionally, to demonstrate its flexibility in output signals, we coupled the eosin Y amplification with photoinduced chromogenic polymerization, enabling sensitive visual detection of analytes. Finally, we applied the exponential amplification methods in developing bioassays for detection of biomarkers including SARS-CoV-2 nucleocapsid protein, an antigen used in the diagnosis of COVID-19.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Terms of Use
Creative Commons Attribution-Noncommercial-Share Alike
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DOI of Published Version
https://doi.org/10.1021/jacs.1c04236
