In this study, we investigated the catalytic performance
and kinetic
model of novel lanthanoid oxide-supported Ru catalysts for NH3 synthesis in mild conditions (P ≤
8 MPa, T ≤ 425 °C), Ru/Ce0.5La0.4Ti0.1Ox (termed as Ru/CeLaTiOx). It was found that Ru/CeLaTiOx significantly
outperformed conventional Ru/MgO and Ru/CeO2 catalysts
across the evaluated operating conditions. High NH3 synthesis
rates up to ∼30 mmol gcat
–1 h–1 were attainable under conditions of 400 °C,
5 MPa, and H2/N2 ratios between 1.0 and 1.5.
Optimization of the Langmuir–Hinshelwood (LH) kinetic model
incorporating nitrogen hydride (NHx) adsorption was performed,
which revealed their strong influence compared to adsorbed N and H
adatoms as intermediate species. Further, the model kinetics showed
favorable dependence toward N2 and H2 concentrations,
which highlights operational advantage of the introduced catalysts
for renewable-derived NH3 synthesis over the currently
commercial Fe and Ru catalysts. Process simulation analysis incorporating
the above-mentioned catalysts and heat recovery system was performed,
which attained predicted process efficiency and specific energy consumption
of 62.8% and 8.32 GJ/ton NH3 for the synthesis loop, respectively.