An integrated Re(I) photocatalyst and sensitizer that activates the formation of formic acid from reduction of CO2

Abstract

Summary

A photochemical reduction of CO₂ to CO was shown using the nickel complex [Ni(bpet)(MeCN)2][ClO4]2 (100824) as catalyst in combination with the ruthenium-based photosensitizer Ru(bpy)3Cl2 (100787). Turnover numbers (TONs) over 700 and a selectivity of >99% for CO were reached in dimethylacetamide/water. The experiments were conducted under visible-light irradiation (λ = 450 nm) using BIH as sacrificial reductants (see section SEDs below).

Advances and special progress

A nickel catalyst inspired by the CODH enzyme (carbon monoxide dehydrogenase) was employed for the photocatalytic reduction of CO₂ with the back then highest reported TON values among nickel complexes in systems with [Ru(bpy)₃]²⁺.

Additional remarks

The binding of CO₂ to the nickel(0) species was identified as the potential rate-determining step of the reduction.

Content of the published article in detail

The article contains results for the reduction of CO₂ to CO under visible-light catalysis using a nickel complex as a catalyst. The catalytic system performs best (referring to the TON of CO production) in dimethylacetamide/water.

Catalyst

[Re(bpy)2(CO)2][OTf] (100760)

Toller Artikel über das Molekül [Ru(bpy)3][PF6] (100808), das total tolle Dinge kann.

Photosensitizer

[Ru(bpy)3][PF6] (100808)

Investigation

REDIRECT Study on the concentration of catalystInvestigation-Name: Table 1

Sacrificial electron donor

In this study, the experiments were done with the sacrificial electron donor TEOA (100507).

Additives

In this study, no additives were tested.