Combining energy and electron transfer in a supramolecular environment for the "green" generation and utilization of hydrated electrons through photoredox catalysis.

ABSTRACT: We present a new mechanism that sustainably produces hydrated electrons, i.e., extremely strong reductants, yet consumes only green photons (532 nm) and the bioavailable ascorbate as sacrificial donor. The mechanism couples an energy-transfer cycle, in which a light-harvesting ruthenium polypyridine complex absorbs a first photon and passes the excitation energy on to a pyrene-based redox catalyst, with an electron-transfer cycle, in which the resulting triplet is reductively quenched and the energy-rich aryl radical anion is finally ionized by a second photon. Thus separating the roles of primary and secondary absorber permitted choosing a redox catalyst with a nonabsorbing ground state but efficiently ionizable radical anion; the quantum yield of the ionization step in our complex

SUBMITTER: Kerzig C 

PROVIDER: S-EPMC6013799 | biostudies-literature | 2016 Jun

REPOSITORIES: biostudies-literature