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Sequential Deoxygenation of CO2 and NO2- via Redox-Control of a Pyridinediimine Ligand with a Hemilabile Phosphine.

ABSTRACT: The deoxygenation of environmental pollutants CO2 and NO2- to form value-added products is reported. CO2 reduction with subsequent CO release and NO2- conversion to NO are achieved via the starting complex Fe(PPhPDI)Cl2 (1). 1 contains the redox-active pyridinediimine (PDI) ligand with a hemilabile phosphine located in the secondary coordination sphere. 1 was reduced with SmI2 under a CO2 atmosphere to form the direduced monocarbonyl Fe(PPhPDI)(CO) (2). Subsequent CO release was achieved via oxidation of 2 using the NOx- source, NO2-. The resulting [Fe(PPhPDI)(NO)]+ (3) mononitrosyl iron complex (MNIC) is formed as the exclusive reduction product due to the hemilabile phosphine. 3 was investigated computationally to be characterized as {FeNO}7, an unusual intermediate-spin Fe(III) coupled to triplet NO- and a singly reduced PDI ligand.

SUBMITTER: Lewine HR 

PROVIDER: S-EPMC10520972 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature

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Sequential Deoxygenation of CO<sub>2</sub> and NO<sub>2</sub><sup>-</sup> via Redox-Control of a Pyridinediimine Ligand with a Hemilabile Phosphine.

Lewine Hanalei R HR   Teigen Allison G AG   Trausch April M AM   Lindblom Kaitlyn M KM   Seda Takele T   Reinheimer Eric W EW   Kowalczyk Tim T   Gilbertson John D JD  

Inorganic chemistry 20230905 37

The deoxygenation of environmental pollutants CO<sub>2</sub> and NO<sub>2</sub><sup>-</sup> to form value-added products is reported. CO<sub>2</sub> reduction with subsequent CO release and NO<sub>2</sub><sup>-</sup> conversion to NO are achieved via the starting complex Fe(<sup>PPh</sup>PDI)Cl<sub>2</sub> (<b>1</b>). <b>1</b> contains the redox-active pyridinediimine (PDI) ligand with a hemilabile phosphine located in the secondary coordination sphere. <b>1</b> was reduced with SmI<sub>2</sub>  ...[more]

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