Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation

Debasish Chakraborty , Christian Danvad Damsgaard, Hugo José Lopes Silva, Christian Nagstrup Conradsen, Jakob Lind Olsen, Hudson W. P. de Carvalho, Benjamin Mutz, Thomas Bligaard, Max J Hoffmann, Jan-Dierk Grunwaldt, Felix Studt, Ib Chorkendorff

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

A novel nanoparticulate catalyst of copper (Cu) and ruthenium (Ru) was designed for low-temperature ammonia oxidation at near-stoichiometric mixtures using a bottom-up approach. A synergistic effect of the two metals was found. An optimum CuRu catalyst presents a reaction rate threefold higher than that for Ru and forty-fold higher than that for Cu. X-ray absorption spectroscopy suggests that in the most active catalyst Cu forms one or two monolayer thick patches on Ru and the catalysts are less active once 3D Cu islands form. The good performance of the tuned Cu/Ru catalyst is attributed to changes in the electronic structure, and thus the altered adsorption properties of the surface Cu sites.
Original languageEnglish
JournalAngewandte Chemie International Edition
Volume56
Issue number30
Pages (from-to)8711-8715
Number of pages6
ISSN1433-7851
DOIs
Publication statusPublished - 2017

Keywords

  • X-ray absorption spectroscopy
  • Ammonia oxidation
  • Density functional calculations
  • Heterogeneous catalysis

Cite this

Chakraborty , Debasish ; Damsgaard, Christian Danvad ; Silva, Hugo José Lopes ; Conradsen, Christian Nagstrup ; Olsen, Jakob Lind ; de Carvalho, Hudson W. P. ; Mutz, Benjamin ; Bligaard, Thomas ; Hoffmann, Max J ; Grunwaldt, Jan-Dierk ; Studt, Felix ; Chorkendorff, Ib. / Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation. In: Angewandte Chemie International Edition. 2017 ; Vol. 56, No. 30. pp. 8711-8715.
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title = "Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation",
abstract = "A novel nanoparticulate catalyst of copper (Cu) and ruthenium (Ru) was designed for low-temperature ammonia oxidation at near-stoichiometric mixtures using a bottom-up approach. A synergistic effect of the two metals was found. An optimum CuRu catalyst presents a reaction rate threefold higher than that for Ru and forty-fold higher than that for Cu. X-ray absorption spectroscopy suggests that in the most active catalyst Cu forms one or two monolayer thick patches on Ru and the catalysts are less active once 3D Cu islands form. The good performance of the tuned Cu/Ru catalyst is attributed to changes in the electronic structure, and thus the altered adsorption properties of the surface Cu sites.",
keywords = "X-ray absorption spectroscopy, Ammonia oxidation, Density functional calculations, Heterogeneous catalysis",
author = "Debasish Chakraborty and Damsgaard, {Christian Danvad} and Silva, {Hugo Jos{\'e} Lopes} and Conradsen, {Christian Nagstrup} and Olsen, {Jakob Lind} and {de Carvalho}, {Hudson W. P.} and Benjamin Mutz and Thomas Bligaard and Hoffmann, {Max J} and Jan-Dierk Grunwaldt and Felix Studt and Ib Chorkendorff",
year = "2017",
doi = "10.1002/anie.201703468",
language = "English",
volume = "56",
pages = "8711--8715",
journal = "Angewandte Chemie International Edition",
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Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation. / Chakraborty , Debasish; Damsgaard, Christian Danvad; Silva, Hugo José Lopes; Conradsen, Christian Nagstrup; Olsen, Jakob Lind; de Carvalho, Hudson W. P.; Mutz, Benjamin; Bligaard, Thomas ; Hoffmann, Max J; Grunwaldt, Jan-Dierk; Studt, Felix; Chorkendorff, Ib.

In: Angewandte Chemie International Edition, Vol. 56, No. 30, 2017, p. 8711-8715.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation

AU - Chakraborty , Debasish

AU - Damsgaard, Christian Danvad

AU - Silva, Hugo José Lopes

AU - Conradsen, Christian Nagstrup

AU - Olsen, Jakob Lind

AU - de Carvalho, Hudson W. P.

AU - Mutz, Benjamin

AU - Bligaard, Thomas

AU - Hoffmann, Max J

AU - Grunwaldt, Jan-Dierk

AU - Studt, Felix

AU - Chorkendorff, Ib

PY - 2017

Y1 - 2017

N2 - A novel nanoparticulate catalyst of copper (Cu) and ruthenium (Ru) was designed for low-temperature ammonia oxidation at near-stoichiometric mixtures using a bottom-up approach. A synergistic effect of the two metals was found. An optimum CuRu catalyst presents a reaction rate threefold higher than that for Ru and forty-fold higher than that for Cu. X-ray absorption spectroscopy suggests that in the most active catalyst Cu forms one or two monolayer thick patches on Ru and the catalysts are less active once 3D Cu islands form. The good performance of the tuned Cu/Ru catalyst is attributed to changes in the electronic structure, and thus the altered adsorption properties of the surface Cu sites.

AB - A novel nanoparticulate catalyst of copper (Cu) and ruthenium (Ru) was designed for low-temperature ammonia oxidation at near-stoichiometric mixtures using a bottom-up approach. A synergistic effect of the two metals was found. An optimum CuRu catalyst presents a reaction rate threefold higher than that for Ru and forty-fold higher than that for Cu. X-ray absorption spectroscopy suggests that in the most active catalyst Cu forms one or two monolayer thick patches on Ru and the catalysts are less active once 3D Cu islands form. The good performance of the tuned Cu/Ru catalyst is attributed to changes in the electronic structure, and thus the altered adsorption properties of the surface Cu sites.

KW - X-ray absorption spectroscopy

KW - Ammonia oxidation

KW - Density functional calculations

KW - Heterogeneous catalysis

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DO - 10.1002/anie.201703468

M3 - Journal article

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JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

SN - 1433-7851

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ER -