Reactions of cationic iron clusters with ammonia, models of nitrogen hydrogenation and dehydrogenation

Dalton Transactions : an International Journal of Inorganic Chemistry
Kjell O Fossan, Einar Uggerud

Abstract

The gas phase reactivities of small cationic iron clusters, Fen+ (n = 1-20), towards ammonia were investigated using Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry. Sequential addition of ammonia molecules to the clusters was observed to be the dominating process for n > 4. In the case of n = 4 we observed addition of ammonia accompanied by dehydrogenation. This reaction was modelled using hybrid density functional theory. Clusters with n < 4 do not react with ammonia. Clusters Fen+ (n = 1-20) react with neither N2 nor H2 at around 10(-8) mbar. When dinitrogen was seeded into the expanding helium, mixed clusters of the type FenNm+ were observed. These ions react with H2, either by addition, or by substitution of N2. The clusters with m = 1 were isolated in separate experiments and reacted with H2, which showed that mixed clusters with n = 5-13 add up to 5 molecules of dihydrogen in successive slow reactions.

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Citations

Jun 9, 2016·The Journal of Physical Chemistry Letters·Denis M KiawiJoost M Bakker
Jan 15, 2009·The Journal of Chemical Physics·Xun-Lei DingSheng-Gui He
Mar 11, 2021·The Journal of Physical Chemistry. a·Lijun GengZhixun Luo
Nov 26, 2010·The Journal of Physical Chemistry. a·Shinichi HirabayashiTamotsu Kondow
Jun 24, 2020·The Journal of Physical Chemistry. a·Lijun GengZhixun Luo
Nov 10, 2006·The Journal of Physical Chemistry. a·Sandro ChiodoJesus M Ugalde

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