Direct Operando Visualization of Metal Support Interactions Induced by Hydrogen Spillover During CO2 Hydrogenation

The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the w...

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Bibliographic Details
Published in:Advanced materials (Weinheim) 2023-12, Vol.35 (51), p.e2306447-n/a
Main Authors: Jenkinson, Kellie, Spadaro, Maria Chiara, Golovanova, Viktoria, Andreu, Teresa, Morante, Joan Ramon, Arbiol, Jordi, Bals, Sara
Format: Article
Language:English
Subjects:
Carbon dioxide
Catalysis
Catalysts
Cerium oxides
CO2 hydrogenation
Design optimization
Electron energy loss spectroscopy
electron microscopy
heterogeneous catalysis
Hydrogenation
in situ
Materials science
Nanoparticles
operando
Oxidation
Shift reaction
Spectrum analysis
Water gas
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Summary:The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure‐activity relationships. In the present work, temperature‐induced morphological and chemical changes in Ni nanoparticle‐decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni‐induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance. Operando electron energy loss spectroscopy in combination with a windowed gas cell and mass spectrometer is used to detect the dynamic formation of Ce3+ active sites within a Ni/CeO2 catalyst during CO2 hydrogenation. The detection of localized active site formation surrounding the Ni nanoparticles highlights the role that interfacial metal–support interactions play in preferencing reaction pathways.
ISSN:0935-9648
1521-4095
DOI:10.1002/adma.202306447