Adsorption of Eu3+ and Gd3+ on high-charge micas as inner-sphere complexes

High-charge micas exhibit improved adsorption properties and are a promising alternative clay material for the engineered barrier in deep geological repositories. When combined with Eu3+ cations, they serve as an in situ luminescent probe for tracking the physical–chemical changes occurring in this...

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Detalles Bibliográficos
Autores: Candela de Aroca, Marina Teresa, Martín Rodríguez, Rosa, Díaz Moreno, Sofía, Valiente Barroso, Rafael|||0000-0001-9855-8309, Aguado Menéndez, Fernando|||0000-0003-2912-0228, Perdigón Aller, Ana Carmen|||0000-0003-3865-3405
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universidad de Cantabria (UC)
Repositorio:UCrea Repositorio Abierto de la Universidad de Cantabria
Idioma:inglés
OAI Identifier:oai:repositorio.unican.es:10902/35517
Acceso en línea:https://hdl.handle.net/10902/35517
Access Level:acceso abierto
Palabra clave:High-charge micas
Adsorption
EXAFS
Luminescent cations
Europium
Gadolinium
Descripción
Sumario:High-charge micas exhibit improved adsorption properties and are a promising alternative clay material for the engineered barrier in deep geological repositories. When combined with Eu3+ cations, they serve as an in situ luminescent probe for tracking the physical–chemical changes occurring in this engineered barrier over the long term. Therefore, a better understanding of the local environment of the lanthanide is highly desirable to comprehend the specific behavior of these systems. A combination of different techniques, (X-ray diffraction, thermogravimetry, fluorescence, and X-ray absorption spectroscopy), has allowed the study of the local environment of two luminescent lanthanide cations, Eu3+ and Gd3+, embedded in the galleries of two high-charge micas with different Si/Al tetrahedral ratio. The results show that the hydration state of these cations is primarily influenced by the layer charge of the aluminosilicate, and secondarily by the cation’s hydration enthalpy. High-charge micas doped with trivalent lanthanide cations are more hydrated compared to the original clays with Na+ in the interlayer. Nevertheless, both Eu3+ and Gd3+ are adsorbed as inner-sphere complexes in the galleries of high-charge micas. They are located inside the distorted hexagonal cavity in all cases, coordinated by 3 oxygens from the tetragonal sheet, one fluorine from the octahedral sheet, and by 2–4 oxygens from water molecules, all at distances around 2.4 Å. An additional oxygen atom at a distance of 3.45–3.50 Å, is proposed from an H2O molecule in the second coordination shell.