Low-Temperature Catalytic NO Reduction with CO by Subnanometric Pt Clusters

[EN] The catalytic subnanometric metal clusters with a few atoms can be regarded as an intermediate state between single atoms and metal nanoparticles (>1 nm). Their molecule-like electronic structures and flexible geometric structures bring rich chemistry and also a different catalytic behav...

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Detalles Bibliográficos
Autores: Fernández-Villanueva, Estefanía, Liu, Lichen, Arenal, Raul, Boronat Zaragoza, Mercedes|||0000-0002-6211-5888, Concepción Heydorn, Patricia|||0000-0003-2058-3103, Corma Canós, Avelino|||0000-0002-2232-3527
Tipo de recurso: artículo
Fecha de publicación:2019
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:10251/150654
Acceso en línea:https://riunet.upv.es/handle/10251/150654
Access Level:acceso abierto
Palabra clave:Single atoms
Subnanometric metal clusters
Platinum
CO plus NO
Operando IR
DFT calculations
QUIMICA ORGANICA
Descripción
Sumario:[EN] The catalytic subnanometric metal clusters with a few atoms can be regarded as an intermediate state between single atoms and metal nanoparticles (>1 nm). Their molecule-like electronic structures and flexible geometric structures bring rich chemistry and also a different catalytic behavior, in comparison with the single-atom or nanoparticulate counterparts. In this work, by combination of operando IR spectroscopy techniques and electronic structure calculations, we will show a comparative study on Pt catalysts for CO + NO reaction at a very low temperature range (140-200 K). It has been found that single Pt atoms immobilized on MCM-22 zeolite are not stable under reaction conditions and agglomerate into Pt nanoclusters and particles, which are the working active sites for CO + NO reaction. In the case of the catalyst containing Pt nanoparticles (similar to 2 nm), the oxidation of CO to CO2 occurs in a much lower extension, and Pt nanoparticles become poisoned under reaction conditions because of a strong interaction with CO and NO. Therefore, only subnanometric Pt clusters allow NO dissociation at a low temperature and CO oxidation to occur well on the surface, while CO interaction is weak enough to avoid catalyst poisoning, resulting in a good balance to achieve enhanced catalytic performance.