Methanation of CO2: Structural response of a Ni-based catalyst under fluctuating reaction conditions unraveled by operando spectroscopy (English)

In: Journal of catalysis   ;  327 ;  2015
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Display Omitted * Maximum CO2 conversion of 81% at 400°C obtaining 80% CH4. * Operando XAS study during methanation of CO2 under changing reaction conditions. * Significant changes in the structure of the Ni particles under reaction conditions. * Deactivation of the catalyst in the second methanation cycle after H2 dropout. * Partial oxidation of Ni particles leads to lower catalytic methanation performance. The methanation of CO2 as a relevant strategy for energy storage has been studied by operando X-ray absorption spectroscopy under dynamic H2/CO2 and CO2 reaction atmospheres. A typical CO2 conversion of 81% was reached at 400°C with a 23wt.-% Ni/CaO-Al2O3 catalyst, yielding 80% of CH4. The operando XAS experiment under working conditions revealed pronounced structural changes, e.g., a fast bulk oxidation of the Ni particles after removal of H2 from the H2/CO2 (4:1) gas stream. A lower performance of the catalyst was observed in the subsequent methanation cycle due to the presence of a residual oxidized fraction of Ni.

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| 2015