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.
Bibliographical noteFunding Information:
We thank JARA-Energy (Seed Fund - JARA-ENERGY MF 005-17 and the joined project “value chains based on CO 2 ”) funded by the Excellence Initiative by the German federal and state governments to promote science and research at German universities. This work was performed as part of the Cluster of Excellence Fuel Science Center (EXC 2186, ID: 390919832) funded by the Excellence Initiative by the German federal and state governments to promote science and research at German universities. We are also thankful to the China Scholarship Council for providing financial support for Jie Ren (No. 201806420028) to pursue his Ph.D. study at RWTH Aachen University.
© 2021 Elsevier B.V.
- CO methanation
- Oxygen vacancy
- perovskite-derived catalysts
- Structure-performance relationships