Catalytic Conversion of Ethanol to n-Butanol Using Ruthenium P-N Ligand Complexes

Richard L. Wingad; Paul J. Gates; Steven T.G. Street; Duncan F. Wass

doi:10.1021/acscatal.5b01327

Catalytic Conversion of Ethanol to n-Butanol Using Ruthenium P-N Ligand Complexes

Richard L. Wingad
, Paul J. Gates
, Steven T.G. Street
, Duncan F. Wass^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

We report several ruthenium catalysts incorporating mixed donor phosphine-amine ligands for the upgrade of ethanol to the advanced biofuel n-butanol, which show high selectivity (≥90%) at good (up to 31%) conversion. In situ formation of catalysts from mixtures of [RuCl₂(η⁶-p-cymene)]₂ and 2-(diphenylphosphino)ethylamine (1) 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.

Original language	English
Pages (from-to)	5822-5826
Number of pages	5
Journal	ACS Catalysis
Volume	5
Issue number	10
DOIs	https://doi.org/10.1021/acscatal.5b01327
Publication status	Published - 2 Oct 2015

Bibliographical note

Publisher Copyright:
© 2015 American Chemical Society.

Keywords

biofuels
butanol
ethanol upgrading
Guerbet catalysis
ruthenium

ASJC Scopus subject areas

Catalysis
General Chemistry

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10.1021/acscatal.5b01327

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title = "Catalytic Conversion of Ethanol to n-Butanol Using Ruthenium P-N Ligand Complexes",

abstract = "We report several ruthenium catalysts incorporating mixed donor phosphine-amine ligands for the upgrade of ethanol to the advanced biofuel n-butanol, which show high selectivity (≥90\%) at good (up to 31\%) conversion. In situ formation of catalysts from mixtures of [RuCl2(η6-p-cymene)]2 and 2-(diphenylphosphino)ethylamine (1) 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.",

keywords = "biofuels, butanol, ethanol upgrading, Guerbet catalysis, ruthenium",

author = "Wingad, \{Richard L.\} and Gates, \{Paul J.\} and Street, \{Steven T.G.\} and Wass, \{Duncan F.\}",

note = "Publisher Copyright: {\textcopyright} 2015 American Chemical Society.",

year = "2015",

month = oct,

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doi = "10.1021/acscatal.5b01327",

language = "English",

volume = "5",

pages = "5822--5826",

journal = "ACS Catalysis",

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publisher = "American Chemical Society",

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T1 - Catalytic Conversion of Ethanol to n-Butanol Using Ruthenium P-N Ligand Complexes

AU - Wingad, Richard L.

AU - Gates, Paul J.

AU - Street, Steven T.G.

AU - Wass, Duncan F.

PY - 2015/10/2

Y1 - 2015/10/2

N2 - We report several ruthenium catalysts incorporating mixed donor phosphine-amine ligands for the upgrade of ethanol to the advanced biofuel n-butanol, which show high selectivity (≥90%) at good (up to 31%) conversion. In situ formation of catalysts from mixtures of [RuCl2(η6-p-cymene)]2 and 2-(diphenylphosphino)ethylamine (1) 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.

AB - We report several ruthenium catalysts incorporating mixed donor phosphine-amine ligands for the upgrade of ethanol to the advanced biofuel n-butanol, which show high selectivity (≥90%) at good (up to 31%) conversion. In situ formation of catalysts from mixtures of [RuCl2(η6-p-cymene)]2 and 2-(diphenylphosphino)ethylamine (1) 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.

KW - biofuels

KW - butanol

KW - ethanol upgrading

KW - Guerbet catalysis

KW - ruthenium

UR - https://www.scopus.com/pages/publications/84942921405

U2 - 10.1021/acscatal.5b01327

DO - 10.1021/acscatal.5b01327

M3 - Article

AN - SCOPUS:84942921405

SN - 2155-5435

VL - 5

SP - 5822

EP - 5826

JO - ACS Catalysis

JF - ACS Catalysis

IS - 10

ER -

Catalytic Conversion of Ethanol to n-Butanol Using Ruthenium P-N Ligand Complexes

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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