Issue 43, 2023

Effects of oxygen functionalities on hydrous hydrazine decomposition over carbonaceous materials

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[double bond, length as m-dash]O and COOH). Systematic DFT calculations supported rationalization of the experimental kinetic trends with respect to each oxygen group (C[double bond, length as m-dash]O, C–O–C, C–OH and COOH).

Graphical abstract: Effects of oxygen functionalities on hydrous hydrazine decomposition over carbonaceous materials

Supplementary files

Article information

Article type
Paper
Submitted
20 Jul 2023
Accepted
17 Sep 2023
First published
26 Sep 2023
This article is Open Access
Creative Commons BY-NC license

Dalton Trans., 2023,52, 15871-15877

Effects of oxygen functionalities on hydrous hydrazine decomposition over carbonaceous materials

S. Bellomi, I. Barlocco, S. Tumiati, P. Fumagalli, N. Dimitratos, A. Roldan and A. Villa, Dalton Trans., 2023, 52, 15871 DOI: 10.1039/D3DT02310A

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