Journal
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 47, Issue 67, Pages 28978-28992Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2022.06.228
Keywords
Hydrogen storage; Metal oxides; Nanocatalysis; X-ray diffraction
Categories
Funding
- FCTeFundacao para a Ciencia e a Tecnologia [57/2016, POCI-01-0247-FEDER-039926, POCI-01-0145-FEDER-032241, UIDB/00481/2020, UIDB/50011/2020, LA/P/0006/2020, PTDC/CTM-CTM/32241/2017, CASOLEM (028917)]
- European Regional Development Fund [CENTRO-01-0145-FEDER-022083]
- FCT [CEECIND/04158/2017]
- CentroPortugal Regional Operational Programme Centro 2020
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This study provides insights into the active catalytic species in ceria additive loaded hydrogen storage system, MgH2, through mechanical milling and cycling tests. In-situ X-ray diffraction and Raman spectroscopy studies confirm the interaction between MgH2 and CeO2, with evidence of reduced cerium oxides throughout the interactions. The CeHx/CeOx interfaces play a key role in suppressing the formation of MgO rock salt.
In continuation with the results explored in our recent previous study (https://doi.org/10. 1016/j.apsusc.2021.150062), the current work sheds more light regarding the active in situ catalytic species in ceria additive loaded hydrogen storage system, MgH2. For this study, two samples, MgH2+0.167CeO(2) and MgH2+0.5CeO(2) were processed through mechanical milling (5 h/200 rpm) and tests were conducted at various stages of hydrogenation/dehy-drogenation cycles (cycles: 1, 5 and 10). Evidence for mild chemical interaction between MgH2 and CeO2 is observed at the time of mechanical milling, whereas strong redox type interaction is witnessed in the cycle tested samples. In-situ X ray diffraction study con-firms that the thermally activated interaction between MgH2 and CeO2 does not produce MgO. In situ Raman spectra provide crucial evidence that reduced cerium oxides exist at all stages of interactions in the MgH2/CeO2 hydrogen storage system. Detailed advanced electron microscopic observations concur well with the in-situ X ray diffraction and Raman spectroscopy studies. Although Gibbs free energy calculations reveal the possible existence of cerium hydrides, owing to the structural similarities between CeHx and CeOx phases, the chemical identity of the most abundant catalytic product remains debatable. Regarding the catalytic mechanism, suppression of MgO rock salt formation is identified to be a key step where the role of CeHx/CeOx interfaces gains more importance. (c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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