Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

Liu L.; Meira D.M.; Concepcion P.; Puga A.V.; Arenal R.; Corma A.

doi:10.1021/acscatal.9b04214

Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

Liu L. ; Meira D.M. ; Arenal R. (Universidad de Zaragoza) ; Concepcion P. ; Puga A.V. ; Corma A.

Resumen: Identification of active sites in heterogeneous metal catalysts is critical for understanding the reaction mechanism at the molecular level and for designing more efficient catalysts. Because of their structural flexibility, subnanometric metal catalysts, including single atoms and clusters with a few atoms, can exhibit dynamic structural evolution when interacting with substrate molecules, making it difficult to determine the catalytically active sites. In this work, Pt catalysts containing selected types of Pt entities (from single atoms to clusters and nanoparticles) have been prepared, and their evolution has been followed, while they were reacting in a variety of heterogeneous catalytic reactions, including selective hydrogenation reactions, CO oxidation, dehydrogenation of propane, and photocatalytic H2 evolution reaction. By in situ X-ray absorption spectroscopy, in situ IR spectroscopy, and high-resolution electron microscopy techniques, we will show that some characterization techniques carried out in an inadequate way can introduce confusion on the interpretation of coordination environment of highly dispersed Pt species. Finally, the combination of catalytic reactivity and in situ characterization techniques shows that, depending on the catalyst-reactant interaction and metal-support interaction, singly dispersed metal atoms can rapidly evolve into metal clusters or nanoparticles, being the working active sites for those abovementioned heterogeneous reactions.
Idioma: Inglés
DOI: 10.1021/acscatal.9b04214
Año: 2019
Publicado en: ACS CATALYSIS 9, 12 (2019), 10626-10639
ISSN: 2155-5435
Factor impacto JCR: 12.35 (2019)
Categ. JCR: CHEMISTRY, PHYSICAL rank: 12 / 159 = 0.075 (2019) - Q1 - T1
Factor impacto SCIMAGO: 4.633 - Chemistry (miscellaneous) (Q1) - Catalysis (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA/E13-17R
Financiación: info:eu-repo/grantAgreement/EC/H2020/671093/EU/MATching zeolite SYNthesis with CATalytic activity/SynCatMatch
Financiación: info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ESTEEM3
Financiación: info:eu-repo/grantAgreement/ES/MINECO-AEI-FEDER/MAT2016-79776-P
Financiación: info:eu-repo/grantAgreement/ES/MINECO/SEV-2016-0683
Tipo y forma: Article (Published version)
Área (Departamento): Área Física Materia Condensada (Dpto. Física Materia Condensa.)

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Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?