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  • Ru-promoted perovskites as effective redox catalysts for CO 2 splitting and methane partial oxidation in a cyclic redox scheme
Title: Ru-promoted perovskites as effective redox catalysts for CO 2 splitting and methane partial oxidation in a cyclic redox scheme
The current study reports AxA’1-xByB’1-yO3-𝛿 perovskite redox catalysts (RCs) for CO2-splitting and methane partial oxidation (POx) in a cyclic redox scheme. Strontium (Sr) and iron (Fe) were chosen as A and B site elements with A’ being lanthanum (La), samarium (Sm) or yttrium (Y), and B’ being manganese (Mn), or titanium (Ti) to tailor their equilibrium oxygen partial pressures (P_(O_2 ) s) for CO2-splitting and methane partial oxidation. DFT calculations were performed for predictive optimization of the oxide materials whereas experimental investigation confirmed the DFT predicted redox performance. The redox kinetics of the RCs improved significantly by 1 wt.% ruthenium (Ru) impregnation without affecting their redox thermodynamics. Ru impregnated LaFe0.375Mn0.625O3 (A=0, A’=La, B=Fe, and B’=Mn) was the most promising RC in terms of its superior redox performance (CH4/CO2 conversion >90% and CO selectivity~ 95%) at 800oC. Long-term redox testing over Ru impregnated LaFe0.375Mn0.625O3 indicated stable performance during the first 30 cycles following with a ~25% decrease in the activity during the last 70 cycles. Air treatment was effective to reactivate the redox catalyst. Detailed characterizations revealed the underlying mechanism for redox catalyst deactivation and reactivation. This study not only validated a DFT guided mixed oxide design strategy for CO2 utilization but also provides potentially effective approaches to enhance redox kinetics as well as long-term redox catalyst performance.  more » « less
Award ID(s):
1923468
PAR ID:
10384476
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Nanoscale
ISSN:
2040-3364
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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