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Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface

Monitoring reaction paths is not only a fundamental scientific issue but also helps us to understand and optimize the catalytic process. Infrared (IR) and Raman spectroscopies are powerful tools for detecting particular molecules or intermediate products as a result of their ability to provide the m...

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Autores principales: Hu, Wei, Cao, Xinrui
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6017320/
https://www.ncbi.nlm.nih.gov/pubmed/29320428
http://dx.doi.org/10.3390/molecules23010126
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author Hu, Wei
Cao, Xinrui
author_facet Hu, Wei
Cao, Xinrui
author_sort Hu, Wei
collection PubMed
description Monitoring reaction paths is not only a fundamental scientific issue but also helps us to understand and optimize the catalytic process. Infrared (IR) and Raman spectroscopies are powerful tools for detecting particular molecules or intermediate products as a result of their ability to provide the molecular “finger-print”. However, theoretical modeling for the vibrational spectra of molecular adsorbates on metallic surfaces is a long-standing challenge, because accurate descriptions of the electronic structure for both the metallic substrates and adsorbates are required. In the present work, we applied a quasi-analytical IR and Raman simulation method to monitor the dehydrogenation of propane towards propylene on a Pd-doped Cu(111) surface in real-time. Different Pd ensembles were used to construct the single-atom catalyst (SAC). We found that the number of sublayer Pd atoms could only affect the intensity of the peak rather than the peak position on the vibrational spectra. However, with the dehydrogenation reaction proceeding, both IR and Raman spectra were changed greatly, which indicates that every reaction step can be distinguished from the point of view of vibrational spectroscopies. Additionally, we found that the catalytic process, which starts from different initial states, shows different spectral profiles. The present results suggest that the vibrational spectroscopies obtained by the high-precision simulations pave the way for identifying different catalytic reaction paths.
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spelling pubmed-60173202018-11-13 Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface Hu, Wei Cao, Xinrui Molecules Article Monitoring reaction paths is not only a fundamental scientific issue but also helps us to understand and optimize the catalytic process. Infrared (IR) and Raman spectroscopies are powerful tools for detecting particular molecules or intermediate products as a result of their ability to provide the molecular “finger-print”. However, theoretical modeling for the vibrational spectra of molecular adsorbates on metallic surfaces is a long-standing challenge, because accurate descriptions of the electronic structure for both the metallic substrates and adsorbates are required. In the present work, we applied a quasi-analytical IR and Raman simulation method to monitor the dehydrogenation of propane towards propylene on a Pd-doped Cu(111) surface in real-time. Different Pd ensembles were used to construct the single-atom catalyst (SAC). We found that the number of sublayer Pd atoms could only affect the intensity of the peak rather than the peak position on the vibrational spectra. However, with the dehydrogenation reaction proceeding, both IR and Raman spectra were changed greatly, which indicates that every reaction step can be distinguished from the point of view of vibrational spectroscopies. Additionally, we found that the catalytic process, which starts from different initial states, shows different spectral profiles. The present results suggest that the vibrational spectroscopies obtained by the high-precision simulations pave the way for identifying different catalytic reaction paths. MDPI 2018-01-10 /pmc/articles/PMC6017320/ /pubmed/29320428 http://dx.doi.org/10.3390/molecules23010126 Text en © 2018 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Hu, Wei
Cao, Xinrui
Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title_full Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title_fullStr Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title_full_unstemmed Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title_short Monitoring Reaction Paths Using Vibrational Spectroscopies: The Case of the Dehydrogenation of Propane toward Propylene on Pd-Doped Cu(111) Surface
title_sort monitoring reaction paths using vibrational spectroscopies: the case of the dehydrogenation of propane toward propylene on pd-doped cu(111) surface
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6017320/
https://www.ncbi.nlm.nih.gov/pubmed/29320428
http://dx.doi.org/10.3390/molecules23010126
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