期刊
CHEMPHOTOCHEM
卷 5, 期 7, 页码 644-653出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cptc.202100034
关键词
bimetallic activation; carbon dioxide reduction; cooperative effects; photocatalysis; rhenium
资金
- German Research Foundation (Deutsche Forschungsgemeinschaft, DFG) [TS330/3-1]
- DFG under Germany's Excellence Strategy [EXC 2008/1-390540038-UniSysCat]
- priority program 2102 Light-controlled reactivity of metal complexes [DFG SCHW1454/9-1, KA 4671/2-1, TS330/4-1]
- Projekt DEAL
The study investigates the influence of additional photosensitizers on the catalytic performance of a dirhenium complex, highlighting that using [Ir(dFppy)(3)] results in faster CO2 to CO transformation compared to [Cu(xant)(bcp)]PF6. Emission quenching studies and IR spectroscopy provide insights into the electron transfer paths of the intermolecular systems.
Photosensitizing units have already been applied to enable light-driven catalytic reduction of CO2 with mononuclear rhenium complexes. However, dinuclear catalytic systems that are able to activate CO2 in a cooperative bimetallic fashion have only rarely been combined with photosensitizers. We here present detailed studies on the influence of additional photosensitizers on the catalytic performance of a dirhenium complex (Re2Cl2) and present correlations with spectroscopic measurements, which shed light on the reaction mechanism. The use of [Ir(dFppy)(3)] (Ir, dFppy=2-(4,6-difluorophenyl)pyridine)) resulted in considerably faster CO2 to CO transformation than [Cu(xant)(bcp)]PF6 (Cu, xant=xantphos, bcp=bathocuproine). Emission quenching studies, transient absorption as well as IR spectroscopy provide information about the electron transfer paths of the intermolecular systems. It turned out that formation of double reduced species [Re2Cl2](2-) along with an intermediate with a Re-Re bond ([ReRe]) can be taken as an indication of multi-electron storage capacity. Furthermore, under catalytic conditions a CO2-bridged intermediate was identified.
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