Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nanocatalysts revealed by 3D electron microscopy
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Collins, S., Fernandez-Garcia, S., Calvino, J., & Midgley, P. (2017). Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nanocatalysts revealed by 3D electron microscopy. Scientific Reports, 7 (1. 5406)https://doi.org/10.1038/s41598-017-05671-9
Surface chemical composition, electronic structure, and bonding characteristics determine catalytic activity but are not resolved for individual catalyst particles by conventional spectroscopy. In particular, the nano-scale three-dimensional distribution of aliovalent lanthanide dopants in ceria catalysts and their effect on the surface electronic structure remains unclear. Here, we reveal the surface segregation of dopant cations and oxygen vacancies and observe bonding changes in lanthanum-doped ceria catalyst particle aggregates with sub-nanometer precision using a new model-based spectroscopic tomography approach. These findings refine our understanding of the spatially varying electronic structure and bonding in ceria-based nanoparticle aggregates with aliovalent cation concentrations and identify new strategies for advancing high efficiency doped ceria nano-catalysts.
We thank Alex Eggeman for assistance with computational resources, supported by the Royal Society, for memory-intensive calculations. The research leading to these results has received funding from the European Research Council under the European Union’s Seventh Framework Program (No. FP7/2007–2013)/ERC Grant Agreement No. 291522-3DIMAGE and the European Union’s Seventh Framework Program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483-ESTEEM2).
European Research Council (291522)
EC FP7 CP WITH CSA (312483)
External DOI: https://doi.org/10.1038/s41598-017-05671-9
This record's URL: https://www.repository.cam.ac.uk/handle/1810/266749