有载体钌催化剂存在时的氨合成和分解

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Kinetics and Catalysis Pub Date : 2023-12-12 DOI:10.1134/s0023158423060137
D. A. Shlyapin, V. A. Borisov, V. L. Temerev, K. N. Iost, Z. A. Fedorova, P. V. Snytnikov
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引用次数: 0

摘要

摘要基于对 4%Ru-13.6%Cs/Sibunit 和 4%Ru-5.4%Ba-7.基于对 4%Ru-13.6%Cs/Sibunit 和 4%Ru-5.4%Ba-7.9%Cs/Sibunit 在氨分解(105 Pa,350-470°C)和氨合成(6×105-5×106 Pa,400-430°C)过程中的催化特性的分析,推导出了可逆反应 N2 + 3H2 \( \rightleftharpoons \) 2NH3 中氮形成/消耗速率的分析表达式,以正确描述正向和逆向反应中化学反应速率对反应混合物组分分压的依赖性。推导动力学方程所采用的方法是基于以下假设:钌表面的吸附位点充满了氢,氢随后在竞争性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;其数值与已公布的数据非常一致。
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Ammonia Synthesis and Decomposition in the Presence of Supported Ruthenium Catalysts

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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来源期刊
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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