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

Wenhao Luo; Sankar Meenakshisundaram; Andrew M. Beale; Qian He; Christopher J. Kiely; Pieter C. A. Bruijnincx; Bert M. Weckhuysen

doi:10.1038/ncomms7540

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

Wenhao Luo, Sankar Meenakshisundaram, Andrew M. Beale, Qian He, Christopher J. Kiely, Pieter C. A. Bruijnincx^*, Bert M. Weckhuysen

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into gamma-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, similar to 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 g-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.

Original language	English
Article number	6540
Number of pages	10
Journal	Nature Communications [E]
Volume	6
DOIs	https://doi.org/10.1038/ncomms7540
Publication status	Published - Mar 2015

Funding

We gratefully thank the Smart Mix Program of the Netherlands Ministry of Economic Affairs and the Netherlands Ministry of Education, Culture and Science within the framework of the CatchBio Program. M.S. is grateful to the Research Executive Agency (REA) of the European Commission for awarding a Marie Curie Intra-European Fellowship for Career Development (FP7-PEOPLE-IEF-2010 Grant Agreement No. 275755). C. van de Spek (Utrecht University), Dr J. Gao (Utrecht University) and T.W.G.M. Verhoeven (Eindhoven University of Technology) are acknowledged for the TEM, N<INF>2</INF> physisorption and XPS measurements, respectively.

Keywords

GOLD-PALLADIUM NANOPARTICLES
CO OXIDATION
BIMETALLIC CATALYSTS
TRANSPORTATION FUELS
AU/TIO2 CATALYSTS
IN-SITU
PD
BIOMASS
TEMPERATURE
CONVERSION

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to gamma-valerolactone",

abstract = "The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into gamma-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, similar to 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 g-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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author = "Wenhao Luo and Sankar Meenakshisundaram and Beale, \{Andrew M.\} and Qian He and Kiely, \{Christopher J.\} and Bruijnincx, \{Pieter C. A.\} and Weckhuysen, \{Bert M.\}",

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doi = "10.1038/ncomms7540",

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AU - Luo, Wenhao

AU - Meenakshisundaram, Sankar

AU - Beale, Andrew M.

AU - He, Qian

AU - Kiely, Christopher J.

AU - Bruijnincx, Pieter C. A.

AU - Weckhuysen, Bert M.

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N2 - The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into gamma-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, similar to 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 g-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.

AB - The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into gamma-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, similar to 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 g-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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KW - TRANSPORTATION FUELS

KW - AU/TIO2 CATALYSTS

KW - IN-SITU

KW - PD

KW - BIOMASS

KW - TEMPERATURE

KW - CONVERSION

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ER -

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

Abstract

Funding

Keywords

UN SDGs

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