Development of ruthenium-based catalysts for ammonia synthesis via polyol reduction method

In this work, ruthenium-based catalysts were synthesized via polyol reduction method with different metal oxides as support and caesium as promoter. The samples were characterized through XRD, ICP-OES, nitrogen physisorption and XPS. Then, the catalysts were tested for ammonia synthesis in the range of temperatures 548–673 K and pressures 1–5 MPa. The synthesized catalysts allowed an ammonia production rate approximately four times higher compared with the performances of similar catalytic formulations in literature (tested at same conditions). The best performance were achieved with the Cs–Ru/CeO 2 (1% wt Cs, 5% wt Ru), reaching an ammonia production of nearly 73 mmol h −1 ∙g cat −1 at 673 K and 5 MPa. As showed by the XPS analysis, the increased Ce 3+ /Ce 4+ ratio led to an enhancement of oxygen vacancies, which favoured the dissociative adsorption of nitrogen, that is the limiting step in the ammonia synthesis reaction. Such high catalytic activity can be ascribed to the beneficial effect of the polyol reduction method for the maximization of the exposure of active sites. • Ru-catalysts were synthesized via polyol reduction and tested for NH 3 production. • Cs–Ru/CeO 2 enabled a NH 3 production rate of 43 mmol h −1 ∙g cat −1 at 673 K and 1 MPa. • Increased Ce 3+ /Ce 4+ ratio enhanced oxygen vacancies favouring N 2 adsorption.

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Publication Details

Journal
International Journal of Hydrogen Energy
Published
2024-09-02
DOI
https://doi.org/10.1016/j.ijhydene.2024.08.408
Citations
8
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
Field-Weighted Citation Impact
0.86
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article

Development of ruthenium-based catalysts for ammonia synthesis via polyol reduction method

Luca Di Felice, Assia Saker, Giulia De Felice, Fausto Gallucci et al.
8 citations
International Journal of Hydrogen Energy
Ammonia Synthesis and Nitrogen Reduction
0.86
article

Development of ruthenium-based catalysts for ammonia synthesis via polyol reduction method

Luca Di Felice, Assia Saker, Giulia De Felice, Fausto Gallucci, Gaetano Anello, Giulia De Luna
article en
8 citations

Abstract

In this work, ruthenium-based catalysts were synthesized via polyol reduction method with different metal oxides as support and caesium as promoter. The samples were characterized through XRD, ICP-OES, nitrogen physisorption and XPS. Then, the catalysts were tested for ammonia synthesis in the range of temperatures 548–673 K and pressures 1–5 MPa. The synthesized catalysts allowed an ammonia production rate approximately four times higher compared with the performances of similar catalytic formulations in literature (tested at same conditions). The best performance were achieved with the Cs–Ru/CeO 2 (1% wt Cs, 5% wt Ru), reaching an ammonia production of nearly 73 mmol h −1 ∙g cat −1 at 673 K and 5 MPa. As showed by the XPS analysis, the increased Ce 3+ /Ce 4+ ratio led to an enhancement of oxygen vacancies, which favoured the dissociative adsorption of nitrogen, that is the limiting step in the ammonia synthesis reaction. Such high catalytic activity can be ascribed to the beneficial effect of the polyol reduction method for the maximization of the exposure of active sites. • Ru-catalysts were synthesized via polyol reduction and tested for NH 3 production. • Cs–Ru/CeO 2 enabled a NH 3 production rate of 43 mmol h −1 ∙g cat −1 at 673 K and 1 MPa. • Increased Ce 3+ /Ce 4+ ratio enhanced oxygen vacancies favouring N 2 adsorption.

International Journal of Hydrogen EnergyVol. 86
Eindhoven University of Technology (NL)
Openalex Percentile: Top 31%
Ammonia Synthesis and Nitrogen Reduction
0.86
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