Effect of oxygen functionalities on the hydrous hydrazine decomposition over carbonaceous materials

Bellomi, Silvio, Barlocco, Ilaria, Tumiati, Simone, Fumagalli, Patrizia, Dimitratos, Nikolaos, Roldan, Alberto ORCID: https://orcid.org/0000-0003-0353-9004 and Villa, Alberto 2023. Effect of oxygen functionalities on the hydrous hydrazine decomposition over carbonaceous materials. Dalton Transactions 52 (43) , pp. 15871-15877. 10.1039/D3DT02310A

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Abstract

Metal-free heterogeneous catalysis is promising in the context of H2 generation. Therefore, establishing structure-activity relationships is a crucial issue to improve the development of more efficient catalysts. Herein, to evaluate the reactivity of the oxygen functionalities in carbonaceous materials, functionalized commercial pyrolytically stripped carbon nanofibers (CNFs) were used as catalysts in the liquid-phase hydrous hydrazine decomposition process and compared its activity to the one of pristine CNF material. Different oxygenated groups were inserted by treating CNFs with hydrogen peroxide for 1h (O1-H2O2) and HNO3 for 1h (O1-HNO3) and 6h (O6-HNO3). An increase in activity was observed as a function of the oxidizing agent strength (HNO3 > H2O2) and the functionalization time (6h > 1h). A thorough characterization of the catalysts demonstrated that the activity could be directly correlated with the oxygen content (O6-HNO3 > O1-HNO3 > O1-H2O2 > CNFs) and pointed out the active sites for the reaction at carbon-oxygen double bond groups (C=O and COOH). Systematic DFT calculations supported rationalizing the experimental kinetic trends with respect to each oxygen group (C=O, C-O-C, C-OH and COOH).

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Royal Society of Chemistry
ISSN:	1477-9226
Date of First Compliant Deposit:	4 October 2023
Date of Acceptance:	17 September 2023
Last Modified:	29 Nov 2023 15:36
URI:	https://orca.cardiff.ac.uk/id/eprint/162939

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