DNA-Scaffolded Synergistic Catalysis
| Autor: | Edward B. Pimentel, Trenton M. Peters-Clarke, Joshua J. Coon, Jeffrey D. Martell |
|---|---|
| Rok vydání: | 2021 |
| Předmět: | |
| Zdroj: | J Am Chem Soc |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | We report DNA-scaffolded synergistic catalysis, a concept that combines the diverse reaction scope of synergistic catalysis with the ability of DNA to precisely pre-organize abiotic groups and undergo stimuli-triggered conformational changes. As an initial demonstration of this concept, we focus on Cu-TEMPO-catalyzed aerobic alcohol oxidation, using DNA as a scaffold to hold a copper co-catalyst and an organic radical co-catalyst (TEMPO) in proximity. The DNA-scaffolded catalyst maintained high turnover number upon dilution and exhibited 190-fold improvement in catalyst turnover number relative to the unscaffolded co-catalysts. By incorporating the co-catalysts into a DNA hairpin-containing scaffold, we demonstrate that the rate of the synergistic catalytic reaction can be controlled through a reversible DNA conformational change that alters the distance between the co-catalysts. This work demonstrates the compatibility of synergistic catalytic reactions with DNA scaffolding, opening future avenues in reaction discovery, sensing, responsive materials, and chemical biology. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|