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Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts.


ABSTRACT: Alcohol-assisted hydrogenation of carbon monoxide (CO) to methanol was achieved using homogeneous molecular complexes. The molecular manganese complex [Mn(CO)2Br[HN(C2H4P i Pr2)2]] ([HN(C2H4P i Pr2)2] = MACHO- i Pr) revealed the best performance, reaching up to turnover number = 4023 and turnover frequency 857 h-1 in EtOH/toluene as solvent under optimized conditions (T = 150 °C, p(CO/H2) = 5/50 bar, t = 8-12 h). Control experiments affirmed that the reaction proceeds via formate ester as the intermediate, whereby a catalytic amount of base was found to be sufficient to mediate its formation from CO and the alcohol in situ. Selectivity for methanol formation reached >99% with no accumulation of the formate ester. The reaction was demonstrated to work with methanol as the alcohol component, resulting in a reactive system that allows catalytic "breeding" of methanol without any coreagents.

SUBMITTER: Kaithal A 

PROVIDER: S-EPMC8395606 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts.

Kaithal Akash A   Werlé Christophe C   Leitner Walter W  

JACS Au 20210125 2


Alcohol-assisted hydrogenation of carbon monoxide (CO) to methanol was achieved using homogeneous molecular complexes. The molecular manganese complex [Mn(CO)<sub>2</sub>Br[HN(C<sub>2</sub>H<sub>4</sub>P <sup><i>i</i></sup> Pr<sub>2</sub>)<sub>2</sub>]] ([HN(C<sub>2</sub>H<sub>4</sub>P <sup><i>i</i></sup> Pr<sub>2</sub>)<sub>2</sub>] = MACHO- <sup><i>i</i></sup> Pr) revealed the best performance, reaching up to turnover number = 4023 and turnover frequency 857 h<sup>-1</sup> in EtOH/toluene as s  ...[more]

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