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Published on: June 23, 2023
Ethanol Upgrading to n-Butanol Using Transition-Metal-Incorporated Poly(triazine)imide Frameworks
Sabrine M Cypher1, Magnus Pauly2, Leslie G Castro1
1Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.
Abstract:
The upgrading of ethanol to n-butanol was performed using a molecular catalyst integrated into a carbon nitride support, one of the first examples of a supported molecular catalyst performing the Guerbet process. Initial studies using crystalline poly(triazine)imide (PTI) with lithium or transition-metal cations imbedded in the support together with a base as the catalyst system did not produce any significant amounts of n-butanol. However, when using the catalyst material formed by treatment of PTI-LiCl with [(Cp*)IrCl2]2 (Cp* = pentamethylcyclopentadienyl) along with sodium hydroxide, a 59% selectivity for butanol (13% yield) was obtained at 145 °C. This PTI-(Cp*)Ir material exhibited distinct UV-vis absorption features and powder X-ray diffractions which differ from those of the parent PTI-LiCl and [(Cp*)IrCl2]2. The PTI-(Cp*)Ir material was found to have a metal loading of 27% iridium per empirical unit of the framework. Along with the formation of n-butanol from the Guerbet reaction, the presence of higher chain alcohols was also observed.
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