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The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)

[Image: see text] The effect of alloying Cu and Pd on the reactivity pattern for formic acid and for ethanol has been examined. The electronic structure of the material is strongly affected by the alloying, with the d-band lowered in energy and filled, compared with Pd alone. Hence the reactivity wo...

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Autores principales: Bowker, Michael, Holroyd, Richard, Perkins, Neil
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9511558/
https://www.ncbi.nlm.nih.gov/pubmed/36176315
http://dx.doi.org/10.1021/acs.jpcc.2c04881
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author Bowker, Michael
Holroyd, Richard
Perkins, Neil
author_facet Bowker, Michael
Holroyd, Richard
Perkins, Neil
author_sort Bowker, Michael
collection PubMed
description [Image: see text] The effect of alloying Cu and Pd on the reactivity pattern for formic acid and for ethanol has been examined. The electronic structure of the material is strongly affected by the alloying, with the d-band lowered in energy and filled, compared with Pd alone. Hence the reactivity would be expected to be strongly affected by the alloying. This appears to be the case for formic acid decomposition, whose decomposition temperature in temperature-programmed desorption is shifted by alloying and is between the temperatures for the individual components (at 350 K, compared with 250 and 470 K for Pd and Cu, respectively). However, when a different molecule is chosen as the probe of surface reactivity, namely, ethanol, we come to a very different conclusion. Here the individual reactivity patterns for the two elemental components of the alloy are seen, namely, dehydrogenation on the Cu (to produce acetaldehyde) and decarbonylation on Pd (to methane and CO). There are effects of alloying on destabilizing the former pathway and stabilizing the latter, but the major conclusion from this work is that it is not average electronic structure that dictates reactivity but the individual atomic nature of the surface components. Only monodentate adsorbates truly probe this behavior.
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spelling pubmed-95115582022-09-27 The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110) Bowker, Michael Holroyd, Richard Perkins, Neil J Phys Chem C Nanomater Interfaces [Image: see text] The effect of alloying Cu and Pd on the reactivity pattern for formic acid and for ethanol has been examined. The electronic structure of the material is strongly affected by the alloying, with the d-band lowered in energy and filled, compared with Pd alone. Hence the reactivity would be expected to be strongly affected by the alloying. This appears to be the case for formic acid decomposition, whose decomposition temperature in temperature-programmed desorption is shifted by alloying and is between the temperatures for the individual components (at 350 K, compared with 250 and 470 K for Pd and Cu, respectively). However, when a different molecule is chosen as the probe of surface reactivity, namely, ethanol, we come to a very different conclusion. Here the individual reactivity patterns for the two elemental components of the alloy are seen, namely, dehydrogenation on the Cu (to produce acetaldehyde) and decarbonylation on Pd (to methane and CO). There are effects of alloying on destabilizing the former pathway and stabilizing the latter, but the major conclusion from this work is that it is not average electronic structure that dictates reactivity but the individual atomic nature of the surface components. Only monodentate adsorbates truly probe this behavior. American Chemical Society 2022-09-12 2022-09-22 /pmc/articles/PMC9511558/ /pubmed/36176315 http://dx.doi.org/10.1021/acs.jpcc.2c04881 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Bowker, Michael
Holroyd, Richard
Perkins, Neil
The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title_full The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title_fullStr The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title_full_unstemmed The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title_short The Catalytic Reactivity of Alloys; Ethanol and Formic Acid Decomposition on Cu–Pd(110)
title_sort catalytic reactivity of alloys; ethanol and formic acid decomposition on cu–pd(110)
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9511558/
https://www.ncbi.nlm.nih.gov/pubmed/36176315
http://dx.doi.org/10.1021/acs.jpcc.2c04881
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