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Journal Article

Metastable nickel-oxygen species modulate rate oscillations during dry reforming of methane

MPS-Authors
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Sandoval Diaz,  Luis       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons215315

Cruz,  Daniel       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons295443

Vuijk,  Maurits       
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons295446

Ducci,  Gianmarco       
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21590

Hävecker,  Michael       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons291560

Jiang,  Wulyu       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons200441

Plodinec,  Milivoj       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons188971

Hammud,  Adnan       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons188969

Ivanov,  Danail
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons230432

Götsch,  Thomas       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22000

Reuter,  Karsten       
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons260321

Scheurer,  Christoph
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21743

Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons41515

Lunkenbein,  Thomas       
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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s41929-023-01090-4.pdf
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Citation

Sandoval Diaz, L., Cruz, D., Vuijk, M., Ducci, G., Hävecker, M., Jiang, W., et al. (2024). Metastable nickel-oxygen species modulate rate oscillations during dry reforming of methane. Nature Catalysis, 7, 161-171. doi:10.1038/s41929-023-01090-4.


Cite as: https://hdl.handle.net/21.11116/0000-000E-4CFC-2
Abstract
When a heterogeneous catalyst is active, it forms metastable structures that constantly transform into each other. These structures contribute differently to the catalytic function. Here we show the role of different metastable oxygen species on a Ni catalyst during dry reforming of methane by combining environmental scanning electron microscopy, near ambient pressure X-ray photoelectron spectroscopy, on-line product detection and computer vision. We highlight the critical role of dissociative CO2 adsorption in regulating the oxygen content of the catalyst and in CH4 activation. We also discover rate oscillations during dry reforming of methane resulting from the sequential transformation of metastable oxygen species that exhibit different catalytic properties: atomic surface oxygen, subsurface oxygen and bulk NiOx. The imaging approach allowed the localization of fluctuating surface regions that correlated directly with catalytic activity. The study highlights the importance of metastability and operando analytics in catalysis science and provides impetus towards the design of catalytic systems.