Abstract
Based on analysis of the catalytic properties of 4%Ru–13.6%Cs/Sibunit and 4%Ru–5.4%Ba–7.9%Cs/Sibunit in the ammonia decomposition (105 Pa, 350–470°C) and ammonia synthesis processes (6 × 105–5 × 106 Pa, 400–430°C), an analytical expression for nitrogen formation/consumption rate in the reversible reaction N2 + 3H2 \( \rightleftharpoons \) 2NH3 has been derived to correctly describe the dependence of the chemical reaction rate on the partial pressures of the reaction mixture components for both the forward and reverse reactions. The approach used to derive the kinetic equation is based on the assumption that the adsorption sites of the ruthenium surface are filled with hydrogen, which is subsequently displaced by nitrogen during competitive interaction. Using the proposed kinetic equation, the equilibrium constants and apparent activation energies for ammonia synthesis and decomposition in the presence of 4%Ru–13.6%Cs/Sibunit and 4%Ru–5.4%Ba–7.9%Cs/Sibunit catalysts have been determined; the values are in good agreement with the published data.
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This work was supported by the Ministry of Science and Higher Education of the Russian Federation within the framework of a state task to Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences (project no. AAAA-A21-121011390009-1).
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Translated by M. Timoshinina
The paper is based on the proceedings of the 7th International School-Conference for Young Scientists “Catalysis: From Science to Industry” (October 11–15, 2022, Tomsk, Russia).
Abbreviations and notation: r, chemical reaction rate; V, volumetric flow rate of reaction mixture components; P, total pressure, partial pressures of reaction mixture components; X, nitrogen or ammonia conversion; T, temperature; k, chemical reaction rate constant; A, preexponential factor; Ea, activation energy for chemical reaction; K, equilibrium constant of chemical reaction; q, heat of adsorption of the reaction medium component on the ruthenium surface; θ, surface coverage of ruthenium by the reaction medium component.
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Shlyapin, D.A., Borisov, V.A., Temerev, V.L. et al. Ammonia Synthesis and Decomposition in the Presence of Supported Ruthenium Catalysts. Kinet Catal 64, 815–825 (2023). https://doi.org/10.1134/S0023158423060137
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DOI: https://doi.org/10.1134/S0023158423060137