Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 312, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121376
Keywords
Heterogeneous catalysis; Carbon dioxide; Methane; Reaction mechanism; In situ DRIFTS
Funding
- Portuguese Foundation for Science and Technology (FCT) [SFRH/BD/128986/2017]
- National Funds through FCT/MCTES [SFRH/BD/128986/2017, LA/P/0045/2020, UIDB/50020/2020]
- FCT funding under the Scientific Employment Stimulus-Institutional Call [UIDP/50020/2020]
- Independent Research Fund Denmark [CEE-CINST/00049/2018, 6111-00237]
- Villum Foundation [0217-00146B]
- FCT [13158]
- [PTDC/NAN-MAT/28745/2017]
- Fundação para a Ciência e a Tecnologia [PTDC/NAN-MAT/28745/2017, SFRH/BD/128986/2017] Funding Source: FCT
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Understanding the reaction mechanism on different materials can optimize the development of cost-efficient, high-performing catalysts for CO2 methanation at low temperatures. Ni nanoparticles supported on a carbon/CeO2 composite and pure CeO2 show excellent low-temperature activity, achieving up to 87% CO2 conversion with full selectivity towards CH4 at 370 degrees C. The study of the reaction mechanism reveals that the CO2 methanation reaction follows a combination of the CO and formate pathways on pure CeO2, while it only follows the formate pathway on the carbon/CeO2 composite.
The development of novel cost-efficient, high-performing catalysts for CO2 methanation that are active at low temperatures can be optimized through the understanding of the reaction mechanism on different materials. A series of Ni-based catalysts supported on CeO2 and carbon/CeO2 composites was investigated, showing that Ni nanoparticles supported on a carbon/CeO2 composite with a 50:50 wt ratio and on pure CeO2 have excellent lowtemperature activity and achieve up to 87% CO2 conversion with full selectivity towards CH4 at 370 degrees C. Importantly, meaningful insights on the reaction mechanism were gathered for the different types of materials by using the emerging ME-PSD-DRIFTS technique. The study of the rate of formation/consumption of the various intermediates showed that the CO2 methanation reaction follows a combination of the CO and formate pathways in the case of Ni on pure CeO2; however, in the case of Ni on the carbon/CeO2 composite, it follows only the formate pathway.
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