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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...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Springer US
2017
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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] |
format | Online Article Text |
id | pubmed-6560467 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Springer US |
record_format | MEDLINE/PubMed |
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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