Zeinalipour-Yazdi, Constantinos D. ORCID: 0000-0002-8388-1549 and Catlow, C. Richard A. (2017) A computational study of the heterogeneous synthesis of hydrazine on Co3Mo3N. Catalysis Letters, 147 (7). pp. 1820-1826. ISSN 1011-372X (doi:https://doi.org/10.1007/s10562-017-2080-y)

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Abstract

Periodic and molecular density functional theory calculations have been applied to elucidate the associative mechanism for hydrazine and ammonia synthesis in the gas phase and hydrazine formation on Co3Mo3N. We find that there are two activation barriers for the associative gas phase mechanism with barriers of 730 and 658 kJ/mol, corresponding to a hydrogenation step from N2 to NNH2 and H2NNH2 to H3NNH3, respectively. The second step of the mechanism is barrierless and an important intermediate, NNH2, can also readily form on Co3Mo3N surfaces via the Eley–Rideal chemisorption of H2 on a pre-adsorbed N2 at nitrogen vacancies. Based on this intermediate a new heterogeneous mechanism for hydrazine synthesis is studied. The highest relative barrier for this heterogeneous catalysed process is 213 kJ/mol for Co3Mo3N containing nitrogen vacancies, clearly pointing towards a low-energy process for the synthesis of hydrazine via a heterogeneous catalysis route.

Item Type:	Article
Additional Information:	© The Author(s) 2017. Open Access. This article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.
Uncontrolled Keywords:	Low-T Mechanisms of Ammonia Synthesis on Co3Mo3N
Subjects:	G Geography. Anthropology. Recreation > GE Environmental Sciences Q Science > QD Chemistry
Faculty / School / Research Centre / Research Group:	Faculty of Engineering & Science Faculty of Engineering & Science > School of Science (SCI)
Last Modified:	30 Sep 2018 01:09
URI:	http://gala.gre.ac.uk/id/eprint/21487

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