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Tuning the magnetic properties of Sn(1−x−y)Ce(4+x)Ce(3+y)O(2) nanoparticles: an experimental and theoretical approach

During the last decade, there was a substantial increase in the research on metal-doped oxide semiconductor nanoparticles due to advances in the engineering of nanomaterials and their potential application in spintronics, biomedicine and photocatalysis fields. In this regard, doping a nanomaterial i...

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Detalles Bibliográficos
Autores principales: Aragón, F. F. H., Villegas-Lelovsky, L., Cabral, L., Lima, M. P., Mesquita, A., Coaquira, J. A. H.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: RSC 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9419532/
https://www.ncbi.nlm.nih.gov/pubmed/36132869
http://dx.doi.org/10.1039/d0na00700e
Descripción
Sumario:During the last decade, there was a substantial increase in the research on metal-doped oxide semiconductor nanoparticles due to advances in the engineering of nanomaterials and their potential application in spintronics, biomedicine and photocatalysis fields. In this regard, doping a nanomaterial is a powerful tool to tune its physicochemical properties. The aim of this work is to shine a new light on the role of the neighbouring elements on the oxidation state of the Ce-impurity, from both experimental and theoretical points of view. Herein, we present an accurate study of the mechanisms involved in the oxidation states of the Ce-ions during the doping process of SnO(2) nanoparticles (NPs) prepared by the polymeric precursor method. X-ray diffraction measurements have displayed the tetragonal rutile-type SnO(2) phase in all samples. However, the Bragg’s peak (111) and (220) located at 2θ ∼29° and ∼47° evidence the formation of a secondary CeO(2) phase for samples with Ce content up to 10%. X-ray absorption near-edge structure (XANES) measurements, at Ce L3 edge, were performed on the NPs as a function of Ce content. The results show, on one side, the coexistence of Ce(3+) and Ce(4+) states in all samples; and on the other side, a clear reduction in the Ce(3+) population driven by the increase of Ce content. It is shown that this is induced by the neighboring cation, and confirmed by magnetic measurements. The monotonic damping of the Ce(3+)/Ce(4+) ratio experimentally, was connected with theoretical calculations via density functional theory by simulating a variety of point defects composed of Ce impurities and surrounding oxygen vacancies. We found that the number of oxygen vacancies around the Ce-ions is the main ingredient to change the Ce oxidation state, and hence the magnetic properties of Ce-doped SnO(2) NPs. The presented results pave the way for handling the magnetic properties of oxides through the control of the oxidation state of impurities.