Selective and Efficient Photocatalytic CO2 Reduction to CO Using Visible Light and an Iron-Based Homogeneous Catalyst

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DOI 10.1021/ja510290t
Authors Julien Bonin, Marc Robert, Mathilde Routier,
Submitted 14.11.2014
Published online 20.11.2014
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Abstract

Summary

The photochemical reduction of CO2 to CO was shown using the iron complex Fe(DHPP)Cl (100671) in combination with the photosensitizers Ir(ppy)3 (100843) or 9-Anthracenecarbonitrile (100936). Turnover numbers (TONs) of up to 140 and a selectivity of 93% for CO were reached in acetonitrile after 55 h of irradiation. The experiments were conducted under visible-light irradiation (λ > 400 nm) with TEA (see section SEDs below) as sacrificial electron donor.

Advances and special progress

The authors reported one of the highest TONs in homogeneous photocatalysis at that time in this study without detecting significant degradation of the catalyst or sensitizer. In addition, they reported the use of a cheap organic photosensitizer for CO2 conversion with a slightly lower TON (60), but higher selectivity (100%).

Additional remarks

Content of the published article in detail

The article contains results of a study for the reduction of CO2 to CO using an iron complex and an iridium-based or organic photosensitizer. The catalytic system performs best (referring to the TON of CO production) in acetonitrile with photosensitizer Ir(ppy)3 (100843).

Catalyst

Fe(DHPP)Cl (100671)

Photosensitizer

Ir(ppy)3 (100843) 9-Anthracenecarbonitrile (100936)

Investigation

catcat conc [µM]PSPS conc [mM]e-De-D conc [M]solvent A..TON CO..
(edit)1.Fe(DHPP)Cl0.002Ir(ppy)30.2TEA0.36MeCN140
(edit)2.Fe(DHPP)Cl0.002Molecule:100936 0.2TEA0.36MeCN40
(edit)3.Fe(DHPP)Cl0.002Molecule:100936 0.2TEA0.05MeCN60

Investigation-Name: photocatalytic conversion of CO2 to CO

Sacrificial electron donor

In this study, the experiments were done with the sacrificial electron donor TEA (TEA (100505)).

Additives

In this study, no additives were tested.

Investigations