Angewandte Chemie - International Edition
Angewandte Chemie - International Edition
4 years ago

New Insights into the Activation and Deactivation of Au/CeZrO4 in the Low-Temperature Water-Gas Shift Reaction

Liwei Niu, David Morgan, Xi Liu, Stanislaw Golunski, Christopher Kiely, Graham John Hutchings, Yongwang Li, Hans Niemantsverdriet, Simon Freakley, Qian He, Ewa Nowicka, Sultan Althahban, James Carter
Gold on ceria-zirconia is an active catalyst for the low-temperature water-gas shift reaction (LTS), a key stage of upgrading H2 reformate streams for fuel cells. However, this catalyst rapidly deactivates and the mechanism remains unclear. Using stop-start scanning transmission electron microscopy (STEM) to follow the exact same area of the sample at different stages of the LTS reaction, as well as complementary X-ray photoelectron spectroscopy, we observed the activation and deactivation of the catalyst at various stages. During the heating of the catalyst to reaction temperature, we observed the formation of small Au nanoparticles (1-2 nm) from sub-nm Au species. These nanoparticles then agglomerated further over 48 h on-stream, most rapidly in the first 5 h when the highest rate of deactivation was observed. These findings suggest that the primary deactivation process consists of the loss of active sites through the agglomeration and possible dewetting of Au nanoparticles.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201709708

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