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Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold

ABSTRACT: We have examined the role of support oxygen vacancies in the gas phase hydrogenation of furfural over Au/TiO(2) and Au/CeO(2) prepared by deposition–precipitation. Both catalysts exhibited a similar Au particle size distribution (1–6 nm) and mean (2.8–3.2 nm). Excess H(2) consumption durin...

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Autores principales: Li, Maoshuai, Collado, Laura, Cárdenas-Lizana, Fernando, Keane, Mark A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Springer US 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6560467/
https://www.ncbi.nlm.nih.gov/pubmed/31258285
http://dx.doi.org/10.1007/s10562-017-2228-9
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author Li, Maoshuai
Collado, Laura
Cárdenas-Lizana, Fernando
Keane, Mark A.
author_facet Li, Maoshuai
Collado, Laura
Cárdenas-Lizana, Fernando
Keane, Mark A.
author_sort Li, Maoshuai
collection PubMed
description ABSTRACT: We have examined the role of support oxygen vacancies in the gas phase hydrogenation of furfural over Au/TiO(2) and Au/CeO(2) prepared by deposition–precipitation. Both catalysts exhibited a similar Au particle size distribution (1–6 nm) and mean (2.8–3.2 nm). Excess H(2) consumption during TPR is indicative of partial support reduction, which was confirmed by O(2) titration. Gold on CeO(2) with a higher redox potential exhibited a greater oxygen vacancy density. A lower furfural turnover frequency (TOF) was recorded over Au/CeO(2) than Au/TiO(2) and is linked to suppressed H(2) chemisorption capacity and strong –C=O interaction at oxygen vacancies that inhibited activity. Gold on non-reducible Al(2)O(3) as benchmark exhibited greater H(2) uptake and delivered the highest furfural TOF. Full selectivity to the target furfuryl alcohol was achieved over Au/TiO(2) and Au/Al(2)O(3) at 413 K and over Au/CeO(2) at 473 K with hydrogenolysis to 2-methylfuran at higher reaction temperature (523 K). A surface reaction mechanism is proposed to account for the activity/selectivity response. GRAPHICAL ABSTRACT: [Image: see text]
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spelling pubmed-65604672019-06-26 Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold Li, Maoshuai Collado, Laura Cárdenas-Lizana, Fernando Keane, Mark A. Catal Letters Article ABSTRACT: We have examined the role of support oxygen vacancies in the gas phase hydrogenation of furfural over Au/TiO(2) and Au/CeO(2) prepared by deposition–precipitation. Both catalysts exhibited a similar Au particle size distribution (1–6 nm) and mean (2.8–3.2 nm). Excess H(2) consumption during TPR is indicative of partial support reduction, which was confirmed by O(2) titration. Gold on CeO(2) with a higher redox potential exhibited a greater oxygen vacancy density. A lower furfural turnover frequency (TOF) was recorded over Au/CeO(2) than Au/TiO(2) and is linked to suppressed H(2) chemisorption capacity and strong –C=O interaction at oxygen vacancies that inhibited activity. Gold on non-reducible Al(2)O(3) as benchmark exhibited greater H(2) uptake and delivered the highest furfural TOF. Full selectivity to the target furfuryl alcohol was achieved over Au/TiO(2) and Au/Al(2)O(3) at 413 K and over Au/CeO(2) at 473 K with hydrogenolysis to 2-methylfuran at higher reaction temperature (523 K). A surface reaction mechanism is proposed to account for the activity/selectivity response. GRAPHICAL ABSTRACT: [Image: see text] Springer US 2017-10-23 2018 /pmc/articles/PMC6560467/ /pubmed/31258285 http://dx.doi.org/10.1007/s10562-017-2228-9 Text en © The Author(s) 2017 Open AccessThis article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.
spellingShingle Article
Li, Maoshuai
Collado, Laura
Cárdenas-Lizana, Fernando
Keane, Mark A.
Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title_full Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title_fullStr Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title_full_unstemmed Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title_short Role of Support Oxygen Vacancies in the Gas Phase Hydrogenation of Furfural over Gold
title_sort role of support oxygen vacancies in the gas phase hydrogenation of furfural over gold
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6560467/
https://www.ncbi.nlm.nih.gov/pubmed/31258285
http://dx.doi.org/10.1007/s10562-017-2228-9
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