Exponential Amplification Using Photoredox Autocatalysis

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 nonfluore...

Mô tả đầy đủ

Chi tiết về thư mục
Những tác giả chính: Kim, Seunghyeon, Martínez Dibildox, Alejandra, Aguirre-Soto, Alan, Sikes Johnson, Hadley
Tác giả khác: Massachusetts Institute of Technology. Department of Chemical Engineering
Định dạng: Bài viết
Ngôn ngữ:English
Được phát hành: American Chemical Society (ACS) 2021
Truy cập trực tuyến:https://hdl.handle.net/1721.1/131158
Miêu tả
Tóm tắt: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.