Photocatalytic CO2 Reduction Using an Osmium Complex as a Panchromatic Self‐Photosensitized Catalyst: Utilization of Blue, Green, and Red Light

Author:

Kamada Kenji1ORCID,Jung Jieun1ORCID,Yamada Chihiro1,Wakabayashi Taku1ORCID,Sekizawa Keita2ORCID,Sato Shunsuke2ORCID,Morikawa Takeshi2ORCID,Fukuzumi Shunichi3ORCID,Saito Susumu14ORCID

Affiliation:

1. Department of Chemistry, Graduate School of Science Nagoya University Furo, Chikusa 464-8602 Nagoya Japan

2. Toyota Central Research and Development Laboratories, Inc. 480-1192 Nagakute Japan

3. Department of Chemistry, Faculty of Pure and Applied Science University of Tsukuba 1-1-1 Tennoudai 305-8571 Tsukuba Ibaraki Japan

4. Integrated Research Consortium on Chemical Sciences (IRCCS) Nagoya University Furo, Chikusa 464-8602 Nagoya Japan

Abstract

AbstractThe photocatalytic reduction of carbon dioxide (CO2) represents an attractive approach for solar‐energy storage and leads to the production of renewable fuels and valuable chemicals. Although some osmium (Os) photosensitizers absorb long wavelengths in the visible‐light region, a self‐photosensitized, mononuclear Os catalyst for red‐light‐driven CO2 reduction has not yet been exploited. Here, we discovered that the introduction of an Os metal to a PNNP‐type tetradentate ligand resulted in the absorption of light with longer‐wavelength (350–700 nm) and that can be applied to a panchromatic self‐photosensitized catalyst for CO2 reduction to give mainly carbon monoxide (CO) with a total turnover number (TON) of 625 under photoirradiation (λ≥400 nm). CO2 photoreduction also proceeded under irradiation with blue (λ0=405 nm), green (λ0=525 nm), or red (λ0=630 nm) light to give CO with >90 % selectivity. The quantum efficiency using red light was determined to be 12 % for the generation of CO. A catalytic mechanism is proposed based on the detection of intermediates using various spectroscopic techniques, including transient absorption, electron paramagnetic resonance, and UV/Vis spectroscopy.

Funder

Japan Society for the Promotion of Science

Ministry of Education, Culture, Sports, Science and Technology

Japan Science and Technology Corporation

Asahi Glass Foundation

Ministry of the Environment, Government of Japan

Publisher

Wiley

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