Promotional effects of Ru and Fe on Ni/ZrO2 catalyst during CO2 methanation: A comparative evaluation of the mechanism

doi:10.1016/j.jechem.2023.07.017

Abstract

Abstract: Ni-based catalysts are widely investigated non-noble metal-based systems for CO₂ methanation. However, their industrial application is still limited due to lower activity at low-temperature and catalyst deactivation. Incorporating a second metal such as Ru and Fe is considered as a successful strategy to overcome these challenges through alloy formation or the synergies provided by the interplay of two adjacent metallic sites. Nonetheless, their promotional effect on the CO₂ methanation mechanism under similar conditions has not been reported yet. In this work, Fe and Ru-promoted Ni/ZrO₂ catalysts were investigated to evaluate their promotional effect on the mechanism. The Ni/Fe ratio was first optimized and a CO₂ conversion rate of 37.7 mmolCO₂/(mol_Ni+Fe s) and 96.3% CH₄ selectivity was obtained over the Ni_0.8Fe_0.2/ZrO₂ catalyst. In comparison with Ni_0.8Fe_0.2/ZrO₂, Ni_0.8Ru_0.2/ZrO₂ prepared with the same composition showed higher activity and stability in CO₂ methanation. Characterization results indicate alloys formation and H spillover for Ni_0.8Ru_0.2/ZrO₂ to be responsible for promotion. Besides, in situ DRIFTS studies evidenced the occurrence of both CO₂ dissociative and associative pathways over Ni_0.8Ru_0.2/ZrO₂ catalyst, while solely the CO₂ associative pathway occurred for Ni_0.8Fe_0.2/ZrO₂.

Key words: Ni-based catalyst, Alloy formation, H spillover, CO₂ methanation, Methanation mechanism

Jie Ren, Feng Zeng, Chalachew Mebrahtu, Zhandong Wang, Regina Palkovits. Promotional effects of Ru and Fe on Ni/ZrO₂ catalyst during CO₂ methanation: A comparative evaluation of the mechanism[J]. Journal of Energy Chemistry, 2023, 86(11): 351-361.

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URL: https://www.jenergychem.com/EN/10.1016/j.jechem.2023.07.017

https://www.jenergychem.com/EN/Y2023/V86/I11/351

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Promotional effects of Ru and Fe on Ni/ZrO₂ catalyst during CO₂ methanation: A comparative evaluation of the mechanism

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