Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 31, Pages 12951-12957Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202003251
Keywords
copper; light harvesting; oxidation; photosensitizers; photocatalysis
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Funding
- National Key R&D Program of China [2017YFA0700104]
- National Natural Science Foundation of China [21703155, 21722104, 21671032]
- Natural Science Foundation of Tianjin City of China [18JCQNJC76500, 18JCJQJC47700, 17JCQNJC05100]
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Developing strong visible-light-absorbing (SVLA) earth-abundant photosensitizers (PSs) for significantly improving the utilization of solar energy is highly desirable, yet it remains a great challenge. Herein, we adopt a through-bond energy transfer (TBET) strategy by bridging boron dipyrromethene (Bodipy) and a Cu-I complex with an electronically conjugated bridge, resulting in the first SVLA Cu-I PSs (Cu-2 and Cu-3). Cu-3 has an extremely high molar extinction coefficient of 162 260 m(-1) cm(-1) at 518 nm, over 62 times higher than that of traditional Cu-I PS (Cu-1). The photooxidation activity of Cu-3 is much greater than that of Cu-1 and noble-metal PSs (Ru(bpy)(3)(2+) and Ir(ppy)(3)(+)) for both energy- and electron-transfer reactions. Femto- and nanosecond transient absorption and theoretical investigations demonstrate that a ping-pong energy-transfer process in Cu-3 involving a forward singlet TBET from Bodipy to the Cu-I complex and a backward triplet-triplet energy transfer greatly contribute to the long-lived and Bodipy-localized triplet excited state.
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