Bellomi, Silvio, Cano-Blanco, Daniel C., Barlocco, Ilaria, Delgado, Juan J., Chen, Xiaowei, Prati, Laura, Ferri, Davide, Dimitratos, Nikolaos, Roldan, Alberto ![]() Item availability restricted. |
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Abstract
Understanding the structure of a functional catalyst is crucial to disclosing the complexity of heterogeneous processes and improving their efficiency. Herein, coprecipitated cobalt–ceria (CoCeOx) oxides doped with Ir (IrCoCeOx) were synthesized and used to assess the performances of metal/oxide interfaces in the N2H4·H2O decomposition performed in aqueous NaOH. Kinetic experiments in batch showed that CoO is the active phase of CoCeOx and that the copresence of Ir and Co (IrCoCeOx) enhanced H2 productivity. A comprehensive characterization (X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy, and in situ diffuse reflectance infrared Fourier transform spectroscopy) combined with robust computational modeling based on the density functional theory was employed to attribute the IrCoCeOx performance enhancement to the Ir/CoO metal/oxide interface, the active site of the reaction. On these sites, the improved H2 productivity in the presence of aqueous NaOH was studied operando through modulated excitation-attenuated total reflectance infrared coupled with phase sensitive detection. The formation of surface Co-hydroxyl and -imido groups at the Ir/CoO interface induced the preferential breakage of the N–H bond of N2H4·H2O, favoring the production of H2.
Item Type: | Article |
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Date Type: | Publication |
Status: | Published |
Schools: | Cardiff Catalysis Institute (CCI) Chemistry |
Publisher: | American Chemical Society |
ISSN: | 1944-8244 |
Date of First Compliant Deposit: | 13 November 2024 |
Date of Acceptance: | 23 September 2024 |
Last Modified: | 13 Nov 2024 10:15 |
URI: | https://orca.cardiff.ac.uk/id/eprint/173119 |
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