Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy

Abstract 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...

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Autores principales:	Sean M. Collins, Susana Fernandez-Garcia, José J. Calvino, Paul A. Midgley
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/32fb9a2e6937421198f202f96570e978
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spelling	oai:doaj.org-article:32fb9a2e6937421198f202f96570e9782021-12-02T16:06:58ZSub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy10.1038/s41598-017-05671-92045-2322https://doaj.org/article/32fb9a2e6937421198f202f96570e9782017-07-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-05671-9https://doaj.org/toc/2045-2322Abstract 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.Sean M. CollinsSusana Fernandez-GarciaJosé J. CalvinoPaul A. MidgleyNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-9 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Sean M. Collins Susana Fernandez-Garcia José J. Calvino Paul A. Midgley Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
description	Abstract 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.
format	article
author	Sean M. Collins Susana Fernandez-Garcia José J. Calvino Paul A. Midgley
author_facet	Sean M. Collins Susana Fernandez-Garcia José J. Calvino Paul A. Midgley
author_sort	Sean M. Collins
title	Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
title_short	Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
title_full	Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
title_fullStr	Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
title_full_unstemmed	Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy
title_sort	sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3d electron microscopy
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/32fb9a2e6937421198f202f96570e978
work_keys_str_mv	AT seanmcollins subnanometersurfacechemistryandorbitalhybridizationinlanthanumdopedceriananocatalystsrevealedby3delectronmicroscopy AT susanafernandezgarcia subnanometersurfacechemistryandorbitalhybridizationinlanthanumdopedceriananocatalystsrevealedby3delectronmicroscopy AT josejcalvino subnanometersurfacechemistryandorbitalhybridizationinlanthanumdopedceriananocatalystsrevealedby3delectronmicroscopy AT paulamidgley subnanometersurfacechemistryandorbitalhybridizationinlanthanumdopedceriananocatalystsrevealedby3delectronmicroscopy
_version_	1718384767882231808

Sub-nanometer surface chemistry and orbital hybridization in lanthanum-doped ceria nano-catalysts revealed by 3D electron microscopy

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