Restructuring of supported Pd by green solvents: an operando Quick EXAFS (QEXAFS) study and implications for the derivation of structure-function relationships in Pd catalysis

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Title: Restructuring of supported Pd by green solvents: an operando Quick EXAFS (QEXAFS) study and implications for the derivation of structure-function relationships in Pd catalysis
Authors: Newton, MA
Brazier, JB
Barreiro, EM
Emerich, H
Adrio, LA
Mulligan, C
Hellgardt, K
Hii, KM
Item Type: Journal Article
Abstract: Transmission electron microscopy (TEM) is commonly used as an ex-situ technique to determine structural changes by comparing images of catalyst particles before and after a reaction. This requires the use of an alcoholic solvent to disperse the particles on a grid. In this work, we will show that Pd catalysts can be transformed during the procedure, by using EXAFS to determine the structure of Pd catalysts in different environments (as dry or wet samples). Supported palladium nanoparticles exposed to aqueous ethanolic solution (50% w/v) are transformed to a common, reduced, and hydrogen-contaminated state, irrespective of their initial habit or support. Catalysts comprised of nanosize PdO are reduced at ca. 350 K, whereas samples comprised of very small (ca. ≤ 10 atoms) Pd particles react with the solvent at just above room temperature and agglomerating with considerable loss of dispersion. As such any potential benefits to catalysis sought through the synthesis of very highly dispersed metallic Pd supported upon a range of inorganic dispersants will be rapidly erased through the action of such solvents.
Issue Date: 14-Nov-2016
Date of Acceptance: 14-Nov-2016
URI: http://hdl.handle.net/10044/1/42652
DOI: https://dx.doi.org/10.1039/C6CY02073A
ISSN: 2044-4753
Publisher: Royal Society of Chemistry
Start Page: 8525
End Page: 8531
Journal / Book Title: Catalysis Science & Technology
Volume: 6
Copyright Statement: © The Royal Society of Chemistry 2016. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (https://creativecommons.org/licenses/by/3.0/)
Sponsor/Funder: Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (E
Funder's Grant Number: EP/G070172/1
EP/L003279/1
Keywords: Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
X-RAY-ABSORPTION
SELECTION GUIDES
LIGAND-FREE
NANOPARTICLES
PALLADIUM
HYDROGEN
OXIDATION
ALCOHOLS
ETHYLENE
CLUSTERS
Publication Status: Published
Appears in Collections:Faculty of Engineering
Chemistry
Catalysis and Advanced Materials
Chemical Engineering
Faculty of Natural Sciences



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