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. 2020 Jul 27;59(31):12951-12957.
doi: 10.1002/anie.202003251. Epub 2020 May 20.

Strong Visible-Light-Absorbing Cuprous Sensitizers for Dramatically Boosting Photocatalysis

Kai-Kai Chen  1 , Song Guo  1 , Heyuan Liu  2 , Xiyou Li  2 , Zhi-Ming Zhang  1 , Tong-Bu Lu  1
Affiliations

Strong Visible-Light-Absorbing Cuprous Sensitizers for Dramatically Boosting Photocatalysis

Kai-Kai Chen et al. Angew Chem Int Ed Engl. .

Abstract

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 CuI complex with an electronically conjugated bridge, resulting in the first SVLA CuI 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 CuI 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 CuI complex and a backward triplet-triplet energy transfer greatly contribute to the long-lived and Bodipy-localized triplet excited state.

Keywords: copper; light harvesting; oxidation; photocatalysis; photosensitizers.

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