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Effects of oxygen functionalities on hydrous hydrazine decomposition over carbonaceous materials.

Authors :
Bellomi, Silvio
Barlocco, Ilaria
Tumiati, Simone
Fumagalli, Patrizia
Dimitratos, Nikolaos
Roldan, Alberto
Villa, Alberto
Source :
Dalton Transactions: An International Journal of Inorganic Chemistry. 11/21/2023, Vol. 52 Issue 43, p15871-15877. 7p.
Publication Year :
2023

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, commercial functionalized pyrolytically stripped carbon nanofibers (CNFs) were used as catalysts in the liquid-phase hydrous hydrazine decomposition process and its activity was compared to that of a pristine CNF material. Different oxygenated groups were inserted by treating CNFs with hydrogen peroxide for 1 h (O1-H2O2) and HNO3 for 1 h (O1-HNO3) and 6 h (O6-HNO3). An increase in activity was observed as a function of the oxidizing agent strength (HNO3 > H2O2) and the functionalization time (6 h > 1 h). 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 rationalization of the experimental kinetic trends with respect to each oxygen group (C=O, C–O–C, C–OH and COOH). [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
14779226
Volume :
52
Issue :
43
Database :
Academic Search Index
Journal :
Dalton Transactions: An International Journal of Inorganic Chemistry
Publication Type :
Academic Journal
Accession number :
173476149
Full Text :
https://doi.org/10.1039/d3dt02310a