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Enhanced stability of sub-nanometric Iridium decorated graphitic carbon nitride for H2 production upon hydrous hydrazine decomposition

Bellomi, Silvio, Barlocco, Ilaria, Chen, Xiaowei, Delgado, Juan J., Arrigo, Rosa, Dimitratos, Nikolaos, Roldan, Alberto ORCID: and Villa, Alberto 2023. Enhanced stability of sub-nanometric Iridium decorated graphitic carbon nitride for H2 production upon hydrous hydrazine decomposition. Physical Chemistry Chemical Physics 25 (2) , pp. 1081-1095. 10.1039/D2CP04387D

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Stabilizing metal nanoparticles is vital for large scale implementations of supported metal catalysts, particularly in view for a sustainable transition to clean energy, e.g., H2 production. In this work, iridium sub-nanometric particles were deposited on commercial graphite and on graphitic carbon nitride by a wet impregnation method to investigate the metal-support interaction during the hydrous hydrazine decomposition reaction. To establish a structure-activity relationship, samples were characterized by transmission electron microscopy and x-ray photoelectron spectroscopy. The catalytic performance of the synthesized materials were evaluated under mild reaction conditions, i.e. 323 K and ambient pressure. The results showed that graphitic carbon nitride enhances the stability of Ir nanoparticles compared to graphite, while maintaining a remarkable activity and selectivity. Simulation techniques including Genetic Algorithm geometry screening and electronic structure analyses were employed to provide valuable atomic level understanding on the metal-support interactions. N anchoring sites of GCN were found to minimise the thermodynamic driving force of cohalescence, thus improving the catalysts stability, as well as to lead charge redistributions in the cluster improving the resistance to poisoning by decomposition intermediates.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Royal Society of Chemistry
ISSN: 1463-9076
Funders: Ministry of Science, Innovation and Universities of Spain
Date of First Compliant Deposit: 8 December 2022
Date of Acceptance: 29 November 2022
Last Modified: 30 Jun 2023 06:49

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