Mostra el registre d'ítem simple
New insights into the dynamics that control the activity of ceria-zirconia solid solutions in thermochemical water splitting cycles
dc.contributor.author | Pappacena, Alfonsina |
dc.contributor.author | Rancan, M. |
dc.contributor.author | Armelao, Lidia |
dc.contributor.author | Llorca Piqué, Jordi |
dc.contributor.author | Ge, W. |
dc.contributor.author | Ye, B. |
dc.contributor.author | Lucotti, A. |
dc.contributor.author | Trovarelli, Alessandro |
dc.contributor.author | Boaro, Marta |
dc.contributor.other | Universitat Politècnica de Catalunya. Departament d'Enginyeria Química |
dc.date.accessioned | 2017-09-15T12:43:11Z |
dc.date.available | 2018-08-02T00:30:24Z |
dc.date.issued | 2017-08-24 |
dc.identifier.citation | Pappacena, A., Rancan, M., Armelao, L., Llorca, J., Ge, W., Ye, B., Lucotti, A., Trovarelli, A., Boaro, M. New insights into the dynamics that control the activity of ceria-zirconia solid solutions in thermochemical water splitting cycles. "Journal of Physical Chemistry C", 24 Agost 2017, vol. 121, núm. 33, p. 17746-17755. |
dc.identifier.issn | 1932-7455 |
dc.identifier.uri | http://hdl.handle.net/2117/107660 |
dc.description.abstract | The reactivity of a ceria-rich Ce0.85Zr0.15O2 solid solution toward the thermochemical water splitting process (TWS) was studied over repeated H2/H2O redox cycles. The structural and surface modifications after treatment at high temperature under air or N2 atmospheres were characterized by high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and positron annihilation lifetime spectroscopy (PALS). Samples treated under nitrogen resulted more active due to phase segregation with formation of a zirconyl oxynitride phase in catalytic amount. Insertion of N3- into the structure contributes to an increase in the numbers of oxygen vacancies that preferably arrange in large clusters, and to the stabilization of Ce3+ centers on the surface. In comparison, treatment under air resulted in a different arrangement of defects with less Ce3+ and smaller and more numerous vacancy clusters. This affects charge transfer and H-coupling processes, which play an important role in boosting the rate of H2 production. The behavior is found to be only slightly dependent on the starting ceria-zirconia composition, and it is related to the development of a similar surface heterostructure configuration, characterized by the presence of at least a ceria-rich solid solution and a (cerium-doped) zirconyl oxynitride phase, which is supposed to act as a promoter for TWS reaction. The above findings confirm the importance of a multiphase structure in the design of ceria-zirconia oxides for water splitting reaction and allow a step forward to find an optimal composition. Moreover, the results indicate that doping with nitrogen might be a novel approach for the design of robust, thermally resistant, and redox active materials. |
dc.format.extent | 10 p. |
dc.language.iso | eng |
dc.subject | Àrees temàtiques de la UPC::Enginyeria química |
dc.subject.lcsh | Cerium oxides |
dc.subject.lcsh | Hydrogen industry |
dc.title | New insights into the dynamics that control the activity of ceria-zirconia solid solutions in thermochemical water splitting cycles |
dc.type | Article |
dc.subject.lemac | Òxids |
dc.contributor.group | Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia |
dc.identifier.doi | 10.1021/acs.jpcc.7b06043 |
dc.relation.publisherversion | http://pubs.acs.org/doi/abs/10.1021/acs.jpcc.7b06043 |
dc.rights.access | Open Access |
local.identifier.drac | 21478751 |
dc.description.version | Postprint (author's final draft) |
local.citation.author | Pappacena, A.; Rancan, M.; Armelao, L.; Llorca, J.; Ge, W.; Ye, B.; Lucotti, A.; Trovarelli, A.; Boaro, M. |
local.citation.publicationName | Journal of Physical Chemistry C |
local.citation.volume | 121 |
local.citation.number | 33 |
local.citation.startingPage | 17746 |
local.citation.endingPage | 17755 |
Fitxers d'aquest items
Aquest ítem apareix a les col·leccions següents
-
Articles de revista [244]
-
Articles de revista [2.227]