Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 26, Issue 41, Pages 9005-9011Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202001494
Keywords
charge transfer; Lewis pairs; photochemistry; radicals; electron transfer
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Funding
- Council for Chemical Sciences of The Netherlands Organization for Scientific Research (NWO/CW)
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Archetypal phosphine/borane frustrated Lewis pairs (FLPs) are famed for their ability to activate small molecules. The mechanism is generally believed to involve two-electron processes. However, the detection of radical intermediates indicates that single-electron transfer (SET) generating frustrated radical pairs could also play an important role. These highly reactive radical species typically have significantly higher energy than the FLP, which prompted this investigation into their formation. Herein, we provide evidence that the classical phosphine/borane combinations PMes(3)/B(C6F5)(3)and PtBu3/B(C6F5)(3)both form an electron donor-acceptor (charge-transfer) complex that undergoes visible-light-induced SET to form the corresponding highly reactive radical-ion pairs. Subsequently, we show that by tuning the properties of the Lewis acid/base pair, the energy required for SET can be reduced to become thermally accessible.
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