Ethanol Upgrading to n -Butanol Using Transition-Metal-Incorporated Poly(triazine)imide Frameworks.

Autor: Cypher SM; Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States., Pauly M; Department of Chemistry, North Carolina State University, Raleigh, North Carolina 27695, United States., Castro LG; Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States., Donley CL; Chapel Hill Analytical and Nanofabrication Laboratory, Department of Chemistry, University of North Carolina, Chapel Hill, North Carolina 27599, United States., Maggard PA; Department of Chemistry, North Carolina State University, Raleigh, North Carolina 27695, United States., Goldberg KI; Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2023 Aug 02; Vol. 15 (30), pp. 36384-36393. Date of Electronic Publication: 2023 Jul 24.
DOI: 10.1021/acsami.3c07396
Abstrakt: 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*)IrCl 2 ] 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*)IrCl 2 ] 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.
Databáze: MEDLINE
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