ChemRxiv
These are preliminary reports that have not been peer-reviewed. They should not be regarded as conclusive, guide clinical practice/health-related behavior, or be reported in news media as established information. For more information, please see our FAQs.
Kim-combined.pdf (3.18 MB)

Exponential Amplification Using Photoredox Autocatalysis

preprint
submitted on 23.04.2021, 01:49 and posted on 23.04.2021, 10:50 by Seunghyeon Kim, Alejandra Martinez Dibildox, Alan Aguirre-Soto, Hadley Sikes
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 non-fluorescent eosin Y derivative (EYH2) 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 EYH2 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 EYH2 degradation, we successfully improved EYH2- 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 photo-induced 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

Funding

Singapore National Research Foundation

MISTI Mexico

Kwanjeong Educational Foundation

CONACYT Postdoctoral Research Award (263622)

History

Email Address of Submitting Author

sikes@mit.edu

Institution

Massachusetts Institute of Technology

Country

USA

ORCID For Submitting Author

0000-0002-7096-138X

Declaration of Conflict of Interest

no conflict of interest

Version Notes

Version One

Exports