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  Visualizing the importance of oxide-metal phase transitions in the production of synthesis gas over Ni catalysts

Sandoval Diaz, L., Plodinec, M., Ivanov, D., Poitel, S., Hammud, A., Nerl, H., et al. (2020). Visualizing the importance of oxide-metal phase transitions in the production of synthesis gas over Ni catalysts. Journal of Energy Chemistry, 50, 178-186. doi:10.1016/j.jechem.2020.03.013.

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1-s2.0-S2095495620301285-main.pdf (Publisher version), 4MB
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 Creators:
Sandoval Diaz, Luis1, Author              
Plodinec, Milivoj1, Author              
Ivanov, Danail1, Author              
Poitel, Stéphane2, Author
Hammud, Adnan1, Author              
Nerl, Hannah1, Author              
Schlögl, Robert1, 3, Author              
Lunkenbein, Thomas1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Electron Spectrometry and Microscopy Laboratory, School of Basic Sciences, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland, ou_persistent22              
3Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, 45470 Mühlheim a.d. Ruhr, Germany, ou_persistent22              

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 Abstract: Synthesis gas, composed of H2 and CO, is an important fuel which serves as feedstock for industrially relevant processes, such as methanol or ammonia synthesis. The efficiency of these reactions depends on the H2: CO ratio, which can be controlled by a careful choice of reactants and catalyst surface chemistry. Here, using a combination of environmental scanning electron microscopy (ESEM) and online mass spectrometry, direct visualization of the surface chemistry of a Ni catalyst during the production of synthesis gas was achieved for the first time. The insertion of a homebuilt quartz tube reactor in the modified ESEM chamber was key to success of the setup. The nature of chemical dynamics was revealed in the form of reversible oxide-metal phase transitions and surface transformations which occurred on the performing catalyst. The oxide-metal phase transitions were found to control the production of synthesis gas in the temperature regime between 700 and 900 °C in an atmosphere relevant for dry reforming of methane (DRM, CO2: CH4 =0.75). This was confirmed using high resolution transmission electron microscopy imaging, electron energy loss spectroscopy, thermal analysis, and C18O2 labelled experiments. Our dedicated operando approach of simultaneously studying the surface processes of a catalyst and its activity allowed to uncover how phase transitions can steer catalytic reactions.

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Language(s): eng - English
 Dates: 2020-02-282019-12-202020-03-042020-03-132020-11
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.jechem.2020.03.013
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Title: Journal of Energy Chemistry
  Abbreviation : J. Energy Chem.
Source Genre: Journal
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Publ. Info: Amsterdam, The Netherlands : Elsevier BV
Pages: 9 Volume / Issue: 50 Sequence Number: - Start / End Page: 178 - 186 Identifier: ISSN: 20954956
CoNE: https://pure.mpg.de/cone/journals/resource/20954956