Advanced

Pd-LaFeO3 Catalysts in Aqueous Ethanol : Pd Reduction, Leaching, and Structural Transformations in the Presence of a Base

Checchia, Stefano LU ; Mulligan, Christopher J. ; Emerich, Hermann ; Alxneit, Ivo ; Krumeich, Frank ; Di Michiel, Marco ; Thompson, Paul B.J. ; Hii, King Kuok Mimi ; Ferri, Davide and Newton, Mark A. (2020) In ACS Catalysis 10(6). p.3933-3944
Abstract

The reactive behavior of three catalysts based on Pd-loaded LaFeO3 was investigated in terms of the reducibility of Pd and its propensity to leaching into the liquid phase in flowing solutions prototypical of C-C coupling catalysis in a continuous flow reactor cell. In situ quick extended X-ray absorption fine structure spectroscopy showed that Pd remains stable and nonreducible in the flowing ethanol/water solvent mixture under heating to 353 K. However, ex situ transmission electron microscopy, high-energy X-ray diffraction, and fluorescence yield Fe K-edge X-ray absorption near-edge structure show that the addition of a significant amount of base (K2CO3, 0.1 M) results in the structural degradation of... (More)

The reactive behavior of three catalysts based on Pd-loaded LaFeO3 was investigated in terms of the reducibility of Pd and its propensity to leaching into the liquid phase in flowing solutions prototypical of C-C coupling catalysis in a continuous flow reactor cell. In situ quick extended X-ray absorption fine structure spectroscopy showed that Pd remains stable and nonreducible in the flowing ethanol/water solvent mixture under heating to 353 K. However, ex situ transmission electron microscopy, high-energy X-ray diffraction, and fluorescence yield Fe K-edge X-ray absorption near-edge structure show that the addition of a significant amount of base (K2CO3, 0.1 M) results in the structural degradation of the perovskite support as well as the mobilization of Pd along the sample bed that is dependent on the structure and crystallite size of the perovskite. The results are discussed in terms of the use of perovskite-type oxides in various areas of research where they are placed in contact with liquid phases of variable temperature and elevated pH.

(Less)
Please use this url to cite or link to this publication:
author
; ; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
basic condition, leaching, pair distribution function, palladium catalysis, Suzuki coupling, X-ray absorption spectroscopy, X-ray diffraction
in
ACS Catalysis
volume
10
issue
6
pages
12 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85082879853
ISSN
2155-5435
DOI
10.1021/acscatal.9b04869
language
English
LU publication?
yes
id
f16df761-bfe5-4d73-a78e-1debcc15623f
date added to LUP
2020-04-20 17:14:30
date last changed
2020-04-22 05:55:08
@article{f16df761-bfe5-4d73-a78e-1debcc15623f,
  abstract     = {<p>The reactive behavior of three catalysts based on Pd-loaded LaFeO<sub>3</sub> was investigated in terms of the reducibility of Pd and its propensity to leaching into the liquid phase in flowing solutions prototypical of C-C coupling catalysis in a continuous flow reactor cell. In situ quick extended X-ray absorption fine structure spectroscopy showed that Pd remains stable and nonreducible in the flowing ethanol/water solvent mixture under heating to 353 K. However, ex situ transmission electron microscopy, high-energy X-ray diffraction, and fluorescence yield Fe K-edge X-ray absorption near-edge structure show that the addition of a significant amount of base (K<sub>2</sub>CO<sub>3</sub>, 0.1 M) results in the structural degradation of the perovskite support as well as the mobilization of Pd along the sample bed that is dependent on the structure and crystallite size of the perovskite. The results are discussed in terms of the use of perovskite-type oxides in various areas of research where they are placed in contact with liquid phases of variable temperature and elevated pH.</p>},
  author       = {Checchia, Stefano and Mulligan, Christopher J. and Emerich, Hermann and Alxneit, Ivo and Krumeich, Frank and Di Michiel, Marco and Thompson, Paul B.J. and Hii, King Kuok Mimi and Ferri, Davide and Newton, Mark A.},
  issn         = {2155-5435},
  language     = {eng},
  month        = {03},
  number       = {6},
  pages        = {3933--3944},
  publisher    = {The American Chemical Society (ACS)},
  series       = {ACS Catalysis},
  title        = {Pd-LaFeO<sub>3</sub> Catalysts in Aqueous Ethanol : Pd Reduction, Leaching, and Structural Transformations in the Presence of a Base},
  url          = {http://dx.doi.org/10.1021/acscatal.9b04869},
  doi          = {10.1021/acscatal.9b04869},
  volume       = {10},
  year         = {2020},
}