Catalysis of ceria incorporated magnesium hydride: a follow up study

• Autor(a) principal: Pukazhselvan, D.
• Data de Publicação: 2022
• Outros Autores: Çaha, Ihsan, Jakka, Suresh Kumar, Graça, Vanessa C.D., Holz, Laura I.V., Soares, M.J., Kovalevsky, A.V, Deepak, Francis Leonard, Fagg, Duncan Paul
• Tipo de documento: Artigo
• Idioma: eng
• Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
• Texto Completo: http://hdl.handle.net/10773/35842

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+0.167CeO2 and MgH2+0.5CeO2 were processed through mechanical milling (5 h/200 rpm) and tests were conducted at various stages of hydrogenation/dehydrogenation 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 confirms 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.