Heteroleptic Cu(I) Bipyridine Complexes as Redox Photosensitizers for Photocatalytic CO2 Reduction

The redox photosensitizing ability of heteroleptic Cu(I) complexes containing a 2,2′–bipyridine (bpy) derivative as an α–diimine ligand was investigated in a photocatalytic CO2 reduction. When combined with fac–Mn(bpy)(CO)3Br as a multi-electron catalyst, the reaction systems generated a mixture of...

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Published in:	Bulletin of the Chemical Society of Japan Vol. 96; no. 6; pp. 519 - 528
Main Authors:	Takeda, Hiroyuki, Takahashi, Kohei, Namiki, Yui, Ito, Akitaka, Kurosu, Masao, Muraoka, Takako, Asano, Motoko S
Format:	Journal Article
Language:	English
Published:	Tokyo The Chemical Society of Japan 15-06-2023 Chemical Society of Japan
Subjects:	Carbon dioxide Catalysts Charge transfer Coplanarity Electromagnetic absorption Electron transfer Ligands Light irradiation Photocatalysis Reducing agents Photocatalytic CO2 reduction Cu(I) complex Photosensitizer
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Abstract	The redox photosensitizing ability of heteroleptic Cu(I) complexes containing a 2,2′–bipyridine (bpy) derivative as an α–diimine ligand was investigated in a photocatalytic CO2 reduction. When combined with fac–Mn(bpy)(CO)3Br as a multi-electron catalyst, the reaction systems generated a mixture of CO and HCOOH to a similar extent to the case using a conventional Cu(I)–phenanthroline analog by visible light irradiation in the presence of a reductant. Incorporating phenyl (ph) groups at the 4,4′–positions of the bpy ligand significantly affected the redox-photosensitization of the Cu(I)–bpy complexes due to improved visible light absorption. Owing to coplanarity between the ph groups and bpy scaffold, the former effectively increased and shifted the lowest-energy metal-to-ligand charge transfer absorption into the visible region more than the case of Cu(I) phenanthroline analogs. Furthermore, photophysical measurements and quenching experiments demonstrated that the heteroleptic Cu(I)–bpy complexes underwent efficient photoinduced-electron transfer from the reductant, generating the corresponding one-electron reduced species. Electrochemical measurements also demonstrated that Cu(I)–bpy complexes had sufficient reducing power and stability to transfer the extra electron to the Mn-complex catalyst in the one-electron reduced state, thereby reproducing the original photosensitizer.
AbstractList	The redox photosensitizing ability of heteroleptic Cu(I) complexes containing a 2,2′–bipyridine (bpy) derivative as an α–diimine ligand was investigated in a photocatalytic CO2 reduction. When combined with fac–Mn(bpy)(CO)3Br as a multi-electron catalyst, the reaction systems generated a mixture of CO and HCOOH to a similar extent to the case using a conventional Cu(I)–phenanthroline analog by visible light irradiation in the presence of a reductant. Incorporating phenyl (ph) groups at the 4,4′–positions of the bpy ligand significantly affected the redox-photosensitization of the Cu(I)–bpy complexes due to improved visible light absorption. Owing to coplanarity between the ph groups and bpy scaffold, the former effectively increased and shifted the lowest-energy metal-to-ligand charge transfer absorption into the visible region more than the case of Cu(I) phenanthroline analogs. Furthermore, photophysical measurements and quenching experiments demonstrated that the heteroleptic Cu(I)–bpy complexes underwent efficient photoinduced-electron transfer from the reductant, generating the corresponding one-electron reduced species. Electrochemical measurements also demonstrated that Cu(I)–bpy complexes had sufficient reducing power and stability to transfer the extra electron to the Mn-complex catalyst in the one-electron reduced state, thereby reproducing the original photosensitizer.
Author	Muraoka, Takako Kurosu, Masao Takahashi, Kohei Namiki, Yui Ito, Akitaka Takeda, Hiroyuki Asano, Motoko S
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Snippet	The redox photosensitizing ability of heteroleptic Cu(I) complexes containing a 2,2′–bipyridine (bpy) derivative as an α–diimine ligand was investigated in a...
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SubjectTerms	Carbon dioxide Catalysts Charge transfer Coplanarity Electromagnetic absorption Electron transfer Ligands Light irradiation Photocatalysis Reducing agents
Title	Heteroleptic Cu(I) Bipyridine Complexes as Redox Photosensitizers for Photocatalytic CO2 Reduction
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