Mechanistic in situ insights into the formation, structural and catalytic aspects of the La2NiO4 intermediate phase in the dry reforming of methane over Ni-based perovskite catalysts
Autor: | Nicolas Bonmassar, Marc Heggen, Aligholi Niaei, Andrew Doran, Simon Penner, Albert Gili, Parastoo Delir Kheyrollahi Nezhad, Ali Farzi, Yuanxu Gao, Bernhard Klötzer, Maged F. Bekheet, Sabine Schwarz, Johannes Bernardi, Franz Kamutzki, Lukas Schlicker, Aleksander Gurlo |
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Rok vydání: | 2021 |
Předmět: |
Carbon dioxide reforming
Hydrogen 010405 organic chemistry Chemistry Process Chemistry and Technology chemistry.chemical_element Chemical Engineering 010402 general chemistry 01 natural sciences Decomposition Physical Chemistry Catalysis Methane 0104 chemical sciences chemistry.chemical_compound Chemical engineering Phase (matter) ddc:540 Crystallite Perovskite (structure) Physical Chemistry (incl. Structural) |
Zdroj: | Applied catalysis / A 612, 117984-(2021). doi:10.1016/j.apcata.2020.117984 |
Popis: | Parastoo Delir Kheyrollahi Nezhad; Maged Behkeet; Nicolas Bonmassar; Lukas Schlicker; Albert Gili; Franz Kamutzki; Andrew Doran; Yuanxu Gao; Marc Heggen; Sabine Schwarz; Johannes Bernardi; Bernhard Klötzer; Aligholi Niaei; Ali Farzi; and Simon Penner “Mechanistic In Situ Insights into the Formation, Structural and Catalytic Aspects of the La2NiO4 Intermediate Phase in the Dry Reforming of Methane over Ni-based Perovskite Catalysts”, Applied Catalysis A, Volume 612, (2021), 117984, https://doi.org/10.1016/j.apcata.2020.117984Abstract:We focus on the stability and bulk/surface structural properties of the Ruddlesden-Popper phase La2NiO4 and their consequences for dry reforming of methane (DRM) activity. Fuelled by the appearance as a crucial intermediate during in situ decomposition of highly DRM-active LaNiO3 perovskite structures, we show that La2NiO4 can be equally in situ decomposed into a Ni/La2O3 phase offering CO2 capture and release necessary for DRM activity, albeit at much higher temperatures compared to LaNiO3. Decomposition in hydrogen also leads to an active Ni/La2O3 phase. In situ X-ray diffraction during DRM operation reveals considerable coking and encapsulation of exsolved Ni, yielding much smaller Ni crystallites compared to on LaNiO3, where coking is virtually absent. Generalizing the importance of intermediate Ruddlesden-Popper phases, the in situ decomposition of La-based perovskite structures yields several obstacles due to the high stability of both the parent perovskite and the Ruddlesden-Popper structures and the occurrence of parasitic structures. |
Databáze: | OpenAIRE |
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