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...
| Main Authors: | , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
American Chemical Society (ACS)
2021
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| Online Access: | https://hdl.handle.net/1721.1/131158 |
| _version_ | 1811088195685711872 |
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| author | Kim, Seunghyeon Martínez Dibildox, Alejandra Aguirre-Soto, Alan Sikes Johnson, Hadley |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Kim, Seunghyeon Martínez Dibildox, Alejandra Aguirre-Soto, Alan Sikes Johnson, Hadley |
| author_sort | Kim, Seunghyeon |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T13:57:46Z |
| format | Article |
| id | mit-1721.1/131158 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T13:57:46Z |
| publishDate | 2021 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1311582022-10-01T18:18:17Z Exponential Amplification Using Photoredox Autocatalysis Kim, Seunghyeon Martínez Dibildox, Alejandra Aguirre-Soto, Alan Sikes Johnson, Hadley Massachusetts Institute of Technology. Department of Chemical Engineering 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. 2021-08-09T22:46:52Z 2021-08-09T22:46:52Z 2021-07 2021-04 2021-08-05T18:25:15Z Article http://purl.org/eprint/type/JournalArticle 0002-7863 1520-5126 https://hdl.handle.net/1721.1/131158 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 en http://dx.doi.org/10.1021/jacs.1c04236 Journal of the American Chemical Society Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) Other repository |
| spellingShingle | Kim, Seunghyeon Martínez Dibildox, Alejandra Aguirre-Soto, Alan Sikes Johnson, Hadley Exponential Amplification Using Photoredox Autocatalysis |
| title | Exponential Amplification Using Photoredox Autocatalysis |
| title_full | Exponential Amplification Using Photoredox Autocatalysis |
| title_fullStr | Exponential Amplification Using Photoredox Autocatalysis |
| title_full_unstemmed | Exponential Amplification Using Photoredox Autocatalysis |
| title_short | Exponential Amplification Using Photoredox Autocatalysis |
| title_sort | exponential amplification using photoredox autocatalysis |
| url | https://hdl.handle.net/1721.1/131158 |
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