Enhanced CO2 methanation activity over La2-xCexNiO4 perovskite-derived catalysts: Understanding the structure-performance relationships

[Display omitted] •La2−xCexNiO4 perovskite-derived catalysts were proved to be active for methanation.•CO2 conversion and CH4 selectivity reached to 78.9% and 99.3% over r-La0.5Ce1.5NiO4 at 350 °C.•r-La0.5Ce1.5NiO4 with large Ni(111) plane and abundant oxygen vacancies exhibited great stability and...

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Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2021-12, Vol.426, p.131760, Article 131760
Main Authors: Ren, Jie, Mebrahtu, Chalachew, van Koppen, Luke, Martinovic, Ferenc, Hofmann, Jan P., Hensen, Emiel J.M., Palkovits, Regina
Format: Article
Language:English
Subjects:
Basicity
CO2 methanation
Oxygen vacancy
perovskite-derived catalysts
Structure-performance relationships
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Summary:[Display omitted] •La2−xCexNiO4 perovskite-derived catalysts were proved to be active for methanation.•CO2 conversion and CH4 selectivity reached to 78.9% and 99.3% over r-La0.5Ce1.5NiO4 at 350 °C.•r-La0.5Ce1.5NiO4 with large Ni(111) plane and abundant oxygen vacancies exhibited great stability and regenerability.•CO2 methanation pathway over r-La0.5Ce1.5NiO4 follows CO hydrogenation route. The design of advanced catalysts for CO2 methanation remains as a research challenge. Besides, the effects of feed composition on the activity and stability of existed catalysts are not well addressed yet. In this work, novel A2BO4-type catalysts derived from La2−xCexNiO4 perovskites are reported for CO2 methanation. The reduced La0.5Ce1.5NiO4 (r-La0.5Ce1.5NiO4) sample with tailored oxygen vacancies, higher reducibility, better Ni dispersion, and exposed Ni(111) crystal plane exhibited the highest CO2 conversion of 78.9% and 99.3% CH4 selectivity at 350 °C, which can also endure different H2/CO2 ratios and even up to 50 %v/v steam. Interestingly, the activity and structure of spent r-La0.5Ce1.5NiO4 can be fully recovered after 100 h TOS under 10 %v/v steam. In-situ DRIFTS experiments confirmed CO2 methanation over the r-La0.5Ce1.5NiO4 to proceed via CO route. The present work suggests that both basicity and the presence of oxygen vacancy facilitate superior catalytic activity and stability during CO2 methanation.
ISSN:1385-8947
1873-3212
DOI:10.1016/j.cej.2021.131760