Ru-promoted perovskites as effective redox catalysts for CO2 splitting and methane partial oxidation in a cyclic redox scheme

Iftikhar, Sherafghan; Martin, William; Wang, Xijun; Liu, Junchen; Gao, Yunfei; Li, Fanxing

doi:10.1039/d2nr04437d

Title: Ru-promoted perovskites as effective redox catalysts for CO2 splitting and methane partial oxidation in a cyclic redox scheme

Journal Article · Mon Nov 14 00:00:00 EST 2022 · Nanoscale

DOI:https://doi.org/10.1039/d2nr04437d· OSTI ID:1899044

Iftikhar, Sherafghan ^[1]; Martin, William ^[1]; Wang, Xijun ^[1]; Liu, Junchen ^[1]; Gao, Yunfei ^[2]; Li, Fanxing ^[1]

North Carolina State Univ., Raleigh, NC (United States)
North Carolina State Univ., Raleigh, NC (United States); East China Univ. of Science and Technology, Shanghai (China)

The current study reports AxA’1-xByB’1-yO3- 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=Mn, and B’=0) 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. Furthermore, 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.

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Research Organization:: North Carolina State University, Raleigh, NC (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE), Office of Clean Energy Systems (FE-22); National Science Foundation (NSF); USDOE

Grant/Contract Number:: FE0031703; CBET1923468; Award DE-FE0031703

OSTI ID:: 1899044

Alternate ID(s):: OSTI ID: 1900547

Journal Information:: Nanoscale, Vol. 14, Issue 48; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2
Utilization
Syngas
Partial Oxidation
DFT
Ruthenium

Title: Ru-promoted perovskites as effective redox catalysts for CO2 splitting and methane partial oxidation in a cyclic redox scheme

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