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Catalysts 2019, 9(1), 45; https://doi.org/10.3390/catal9010045

Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

1
Laboratory of Nanotechnology on Surfaces, Instituto de Ciencia de los Materiales de Sevilla (CSIC-Universidad de Sevilla), Avda. Américo Vespucio 49, 41092 Sevilla, Spain
2
Departamento de Física Atómica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes, 41012 Sevilla, Spain
*
Author to whom correspondence should be addressed.
Received: 27 November 2018 / Revised: 26 December 2018 / Accepted: 28 December 2018 / Published: 4 January 2019
(This article belongs to the Special Issue Plasma Catalysis)
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Abstract

Dielectric barrier discharge (DBD) plasmas and plasma catalysis are becoming an alternative procedure to activate various gas phase reactions. A low-temperature and normal operating pressure are the main advantages of these processes, but a limited energy efficiency and little selectivity control hinder their practical implementation. In this work, we propose the use of isotope labelling to retrieve information about the intermediate reactions that may intervene during the DBD processes contributing to a decrease in their energy efficiency. The results are shown for the wet reforming reaction of methane, using D2O instead of H2O as reactant, and for the ammonia synthesis, using NH3/D2/N2 mixtures. In the two cases, it was found that a significant amount of outlet gas molecules, either reactants or products, have deuterium in their structure (e.g., HD for hydrogen, CDxHy for methane, or NDxHy for ammonia). From the analysis of the evolution of the labelled molecules as a function of power, useful information has been obtained about the exchange events of H by D atoms (or vice versa) between the plasma intermediate species. An evaluation of the number of these events revealed a significant progression with the plasma power, a tendency that is recognized to be detrimental for the energy efficiency of reactant to product transformation. The labelling technique is proposed as a useful approach for the analysis of plasma reaction mechanisms. View Full-Text
Keywords: dielectric barrier discharge (DBD); isotope labelling; methane reforming; ammonia synthesis; plasma catalysis dielectric barrier discharge (DBD); isotope labelling; methane reforming; ammonia synthesis; plasma catalysis
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Navascués, P.; Obrero-Pérez, J.M.; Cotrino, J.; González-Elipe, A.R.; Gómez-Ramírez, A. Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes. Catalysts 2019, 9, 45.

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