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Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

AutorNavascués, Paula; Obrero-Pérez, Jose M.; Cotrino, José ; González-Elipe, Agustín R.; Gómez-Ramírez, Ana
Fecha de publicación4-ene-2019
EditorMultidisciplinary Digital Publishing Institute
CitaciónCatalysts 9 (1): 45 (2019)
ResumenDielectric 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 D<sub>2</sub>O instead of H<sub>2</sub>O as reactant, and for the ammonia synthesis, using NH<sub>3</sub>/D<sub>2</sub>/N<sub>2</sub> 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, CD<sub>x</sub>H<sub>y</sub> for methane, or ND<sub>x</sub>H<sub>y</sub> 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.
Identificadoresdoi: 10.3390/catal9010045
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