Confined Pt-1(1+) Water Clusters in a MOF Catalyze the Low-Temperature Water-Gas Shift Reaction with both CO2 Oxygen Atoms Coming from Water

[EN] The synthesis and reactivity of single metal atoms in a low-valence state bound to just water, rather than to organic ligands or surfaces, is a major experimental challenge. Herein, we show a gram-scale wet synthesis of Pt-1(1+) stabilized in a confined space by a crystallographically well-defi...

Descripción completa

Detalles Bibliográficos
Autores: Rivero-Crespo, Miguel Ángel, Mon, Marta, Ferrando-Soria, Jesus, Lopes, Christian W., Hernandez-Garrido, Juan carlos, López-Haro, Miguel, Calvino, Jose J., Ramos-Fernandez, Enrique V., Armentano, Donatella, Pardo, Emilio, Boronat Zaragoza, Mercedes|||0000-0002-6211-5888, Leyva Perez, Antonio|||0000-0003-1063-5811, Corma Canós, Avelino|||0000-0002-2232-3527
Tipo de recurso: artículo
Fecha de publicación:2018
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/190347
Acceso en línea:https://riunet.upv.es/handle/10251/190347
Access Level:acceso abierto
Palabra clave:Metal-organic frameworks (MOFs)
Platinum
Single-atom catalyst
Water clusters
Water-gas shift reaction
Descripción
Sumario:[EN] The synthesis and reactivity of single metal atoms in a low-valence state bound to just water, rather than to organic ligands or surfaces, is a major experimental challenge. Herein, we show a gram-scale wet synthesis of Pt-1(1+) stabilized in a confined space by a crystallographically well-defined first water sphere, and with a second coordination sphere linked to a metal-organic framework (MOF) through electrostatic and H-bonding interactions. The role of the water cluster is not only isolating and stabilizing the Pt atoms, but also regulating the charge of the metal and the adsorption of reactants. This is shown for the low-temperature water-gas shift reaction (WGSR: CO + H2O CO2 + H-2), where both metal coordinated and H-bonded water molecules trigger a double water attack mechanism to CO and give CO2 with both oxygen atoms coming from water. The stabilized Pt1+ single sites allow performing the WGSR at temperatures as low as 50 degrees C.