Inducing Reactivity by Cluster Strain in Titanium Frameworks

[EN] Despite their potential to control charge separation and redox activity, deliberate strategies to distort metal-oxo clusters in molecular frameworks remain limited. Here we present a proof-of-concept for cluster strain engineering using the titanium-organic framework MUV-10 as a model. Replacin...

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Detalles Bibliográficos
Autores: Gomez-Oliveira, Eloy P., Castells-Gil, Javier, Gandara, Felipe, Almora-Barrios, Neyvis, Tatay, Sergio, Padial, Natalia M., Marti-Gastaldo, Carlos, Fernandes-de Almeida, Vitor, Garcia-Baldovi, Hermenegildo, Navalón Oltra, Sergio|||0000-0001-8423-0759
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:dnet:riunet______::737d93ec36032cd5d13a068809b44d1e
Acceso en línea:https://riunet.upv.es/handle/10251/233404
Access Level:acceso abierto
Palabra clave:Metal-organic frameworks
Cluster strain engineering
Titanium-oxo clusters
Goldschmidt tolerance factor
Photocatalytic CO2 methanation
Redox activity
Descripción
Sumario:[EN] Despite their potential to control charge separation and redox activity, deliberate strategies to distort metal-oxo clusters in molecular frameworks remain limited. Here we present a proof-of-concept for cluster strain engineering using the titanium-organic framework MUV-10 as a model. Replacing Ca2+ with larger alkaline-earth cations (Sr2+, Ba2+) induces predictable distortions of Ti2M2 clusters and a cubic-to-tetragonal cell transformation while preserving the overall connectivity. This local strain alters Ti-O coordination geometry, enhances ligand-to-metal charge transfer, and promotes the photogeneration of Ti3+ sites, as validated by photocatalytic CO2 methanation under standardized conditions. Importantly, the extent of distortion follows the trend anticipated from the Goldschmidt tolerance factor, a classical descriptor from perovskite chemistry, that we repurpose here to rationalize strain in reticular frameworks. Taken together, these findings establish a conceptual link between oxide catalysis and reticular chemistry, highlighting cluster strain as a potential structural switch to modulate redox reactivity in molecular solids.