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

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...

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Published in:Angewandte Chemie International Edition 2017-07, Vol.56 (30), p.8711-8715
Main Authors: Chakraborty, Debasish, Damsgaard, Christian Danvad, Silva, Hugo, Conradsen, Christian, Olsen, Jakob Lind, Carvalho, Hudson W. P., Mutz, Benjamin, Bligaard, Thomas, Hoffmann, Max J., Grunwaldt, Jan‐Dierk, Studt, Felix, Chorkendorff, Ib
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Adsorption
Ammonia
ammonia oxidation
Catalysts
Copper
density functional calculations
Electronic structure
Heavy metals
heterogeneous catalysis
Low temperature
Nanoparticles
Oxidation
Ruthenium
Spectroscopy
Surface chemistry
Synergistic effect
Temperature effects
X-ray absorption spectroscopy
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Summary: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. Bottoms up! The catalytic activity of the ammonia oxidation reaction can be tuned by a bottom‐up approach that combines theory and experiment. For stoichiometric catalysis, density functional calculations predict an increase in activity when a Cu overlayer is present on Ru. Four‐fold and forty‐fold increases in activity were obtained with synthesized CuRu nanoparticles bearing Cu monolayers compared to pure Ru and Cu, respectively.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201703468