Ammonia Decomposition Enhancement by Cs-Promoted Fe/Al2O3 Catalysts

• Published in: Catalysis letters Vol. 150; no. 12; pp. 3369 - 3376
• Main Authors: Parker, Luke A., Carter, James H., Dummer, Nicholas F., Richards, Nia, Morgan, David J., Golunski, Stanislaw E., Hutchings, Graham J.
• Format: Journal Article
• Language: English
• Published: New York Springer US 01.12.2020
• Subjects: Catalysis; Chemistry; Chemistry and Materials Science; Industrial Chemistry/Chemical Engineering; Organometallic Chemistry; Physical Chemistry; Hydrogen energy; Fe/Al; Ammonia decomposition; Cs-promotion; O
• ISSN: 1011-372X; 1572-879X
• DOI: 10.1007/s10562-020-03247-3

A range of Cs-doped Fe/Al 2 O 3 catalysts were prepared for the ammonia decomposition reaction. Through time on-line studies it was shown that at all loadings of Cs investigated the activity of the Fe/Al 2 O 3 catalysts was enhanced, with the optimum Cs:Fe being ca. 1. Initially, the rate of NH 3 decomposition was low, typically < 10% equilibrium conversion (99.7%@500°C) recorded after 1 h. All catalysts exhibited an induction period (typically ca. 10 h) with the conversion reaching a high of 67% equilibrium conversion for Cs:Fe = 0.5 and 1. The highest rate of decomposition observed was attributed to the balance between increasing the concentration of Cs without blocking the active site. Analysis of H 2 -TPR and XPS measurements indicated that Cs acts as an electronic promoter. Previously, Cs has been shown to act as a promoter for Ru, where Cs alters the electron density of the active site, thereby facilitating the recombination of N 2 which is considered the rate determining step. In addition, XRD and N 2 adsorption measurements suggest that with higher Cs loadings deactivation of the catalytic activity is due to a layer of CsOH that forms on the surface and blocks active sites. Graphic Abstract