Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 16, Pages 5343-5346Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b02443
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Funding
- Swiss National Science Foundation [200021-146231/1]
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Photoinduced multielectron transfer and reversible accumulation of redox equivalents is accomplished in a fully integrated molecular heptad composed of four donors, two photosensitizers, and one acceptor. The second reduction of the dibenzo[1,2]dithiin acceptor occurs more easily than the first by 1.3 V, and this potential inversion facilitates the light-driven formation of a two-electron reduced state with a lifetime of 66 ns in deaerated CH3CN. The quantum yield for formation of this doubly charge-separated photoproduct is 0.5%. In acidic oxygen-free solution, the reduction product is a stable dithiol. Under steady-state photoirradiation, our heptad catalyzes the two-electron reduction of an aliphatic disulfide via thiolate-disulfide interchange. Exploitation of potential inversion for the reversible light-driven accumulation of redox equivalents in artificial systems is unprecedented and the use of such a charge-accumulated state for multielectron photoredox catalysis represents an important proof-of-concept.
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