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High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone

The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into γ-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, selec...

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Autores principales: Luo, Wenhao, Sankar, Meenakshisundaram, Beale, Andrew M., He, Qian, Kiely, Christopher J., Bruijnincx, Pieter C. A., Weckhuysen, Bert M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4382690/
https://www.ncbi.nlm.nih.gov/pubmed/25779385
http://dx.doi.org/10.1038/ncomms7540
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author Luo, Wenhao
Sankar, Meenakshisundaram
Beale, Andrew M.
He, Qian
Kiely, Christopher J.
Bruijnincx, Pieter C. A.
Weckhuysen, Bert M.
author_facet Luo, Wenhao
Sankar, Meenakshisundaram
Beale, Andrew M.
He, Qian
Kiely, Christopher J.
Bruijnincx, Pieter C. A.
Weckhuysen, Bert M.
author_sort Luo, Wenhao
collection PubMed
description The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into γ-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, selective and stable supported metal catalysts for this reaction and on the beneficial effects of metal nano-alloying. Bimetallic random alloys of gold-palladium and ruthenium-palladium supported on titanium dioxide are prepared with a modified metal impregnation method. Gold-palladium/titanium dioxide shows a marked,~27-fold increase in activity (that is, turnover frequency of 0.1 s(−1)) compared with its monometallic counterparts. Although ruthenium-palladium/titanium dioxide is not only exceptionally active (that is, turnover frequency of 0.6 s(−1)), it shows excellent, sustained selectivity to γ-valerolactone (99%). The dilution and isolation of ruthenium by palladium is thought to be responsible for this superior catalytic performance. Alloying, furthermore, greatly improves the stability of both supported nano-alloy catalysts.
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spelling pubmed-43826902015-04-07 High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone Luo, Wenhao Sankar, Meenakshisundaram Beale, Andrew M. He, Qian Kiely, Christopher J. Bruijnincx, Pieter C. A. Weckhuysen, Bert M. Nat Commun Article The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into γ-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, selective and stable supported metal catalysts for this reaction and on the beneficial effects of metal nano-alloying. Bimetallic random alloys of gold-palladium and ruthenium-palladium supported on titanium dioxide are prepared with a modified metal impregnation method. Gold-palladium/titanium dioxide shows a marked,~27-fold increase in activity (that is, turnover frequency of 0.1 s(−1)) compared with its monometallic counterparts. Although ruthenium-palladium/titanium dioxide is not only exceptionally active (that is, turnover frequency of 0.6 s(−1)), it shows excellent, sustained selectivity to γ-valerolactone (99%). The dilution and isolation of ruthenium by palladium is thought to be responsible for this superior catalytic performance. Alloying, furthermore, greatly improves the stability of both supported nano-alloy catalysts. Nature Pub. Group 2015-03-17 /pmc/articles/PMC4382690/ /pubmed/25779385 http://dx.doi.org/10.1038/ncomms7540 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Luo, Wenhao
Sankar, Meenakshisundaram
Beale, Andrew M.
He, Qian
Kiely, Christopher J.
Bruijnincx, Pieter C. A.
Weckhuysen, Bert M.
High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title_full High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title_fullStr High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title_full_unstemmed High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title_short High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
title_sort high performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4382690/
https://www.ncbi.nlm.nih.gov/pubmed/25779385
http://dx.doi.org/10.1038/ncomms7540
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