Catalytic Conversion of Ethanol to <i>n</i>‑Butanol Using Ruthenium P–N Ligand Complexes
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Abstract
We report several ruthenium catalysts
incorporating mixed donor
phosphine-amine ligands for the upgrade of ethanol to the advanced
biofuel <i>n</i>-butanol, which show high selectivity (≥90%)
at good (up to 31%) conversion. In situ formation of catalysts from
mixtures of [RuCl<sub>2</sub>(η<sup>6</sup>-<i>p</i>-cymene)]<sub>2</sub> and 2-(diphenylphosphino)ethylamine (<b>1</b>) shows enhanced activity at initial water concentrations
higher than those of our previously reported diphosphine systems.
Preliminary mechanistic studies (electrospray ionization mass spectrometry
and nuclear magnetic resonance spectroscopy) suggest the possibility
of ligand-assisted proton transfer in some derivatives