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.

中文翻译：

---

负载型钌催化剂存在下的氨合成和分解

摘要

^{基于4%Ru–13.6%Cs/Sibunit和4%Ru–5.4%Ba–7.9%Cs/Sibunit在氨分解(10 5} Pa, 350–470°C)和氨合成过程中的催化性能分析(6 × 10 ^{5 –5} × 10 ^{6 Pa, 400–430°C)，可逆反应 N} ₂ + 3H ₂ \( \rightleftharpoons \) 2NH ₃中氮形成/消耗速率的解析表达式已正确导出描述化学反应速率对正向反应和逆向反应的反应混合物组分的分压的依赖性。用于推导动力学方程的方法基于这样的假设：钌表面的吸附位点充满氢，随后在竞争相互作用过程中被氮取代。利用所提出的动力学方程，确定了在 4%Ru–13.6%Cs/Sibunit 和 4%Ru–5.4%Ba–7.9%Cs/Sibunit 催化剂存在下氨合成和分解的平衡常数和表观活化能；这些值与已发布的数据非常吻合。