Computationally Effective Approach for Studies of Mechanism and Thermodynamics of Heterogeneous Catalytic Processes on Metal Oxides

IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL International Journal of Quantum Chemistry Pub Date : 2024-08-28 DOI:10.1002/qua.27470
Ekaterina G. Ragoyja, Vitaly E. Matulis, Oleg A. Ivashkevich, Dmitry A. Lyakhov, Dominik Michels
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Abstract

To understand the nature of heterogeneous catalytic processes and improve their efficiency, it is necessary to conduct both experimental and theoretical studies. At the same time, there is no unified approach to obtaining the necessary data using quantum chemistry methods. In this work, problems of the existing calculational approaches are analyzed. The obtained information is used to develop the original three-layer embedded cluster model approach, which is shown to be the most effective. The general algorithm for obtaining such models for various oxides is formulated. The sufficient accuracy of the proposed models in predicting geometric and energy characteristics, vibrational frequencies, activation barriers, and thermodynamic characteristics is verified. The specifics of calculating the thermodynamic characteristics of heterogeneous processes using the proposed cluster models is studied in detail. The developed approach is an effective tool for studying the mechanism of heterogeneous catalytic processes both by itself and in combination with experiment.

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研究金属氧化物上异质催化过程的机理和热力学的有效计算方法
要了解异相催化过程的本质并提高其效率,就必须同时进行实验和理论研究。同时,利用量子化学方法获取必要数据还没有统一的方法。本研究分析了现有计算方法存在的问题。所获得的信息被用于开发独创的三层嵌入式聚类模型方法,该方法被证明是最有效的。本文还提出了针对各种氧化物获取此类模型的通用算法。验证了所提出的模型在预测几何和能量特征、振动频率、活化势垒和热力学特征方面的足够准确性。详细研究了使用所提出的群集模型计算异质过程热力学特性的具体细节。所开发的方法是研究异相催化过程机理的有效工具,既可单独使用,也可与实验相结合。
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来源期刊
International Journal of Quantum Chemistry
International Journal of Quantum Chemistry 化学-数学跨学科应用
CiteScore
4.70
自引率
4.50%
发文量
185
审稿时长
2 months
期刊介绍: Since its first formulation quantum chemistry has provided the conceptual and terminological framework necessary to understand atoms, molecules and the condensed matter. Over the past decades synergistic advances in the methodological developments, software and hardware have transformed quantum chemistry in a truly interdisciplinary science that has expanded beyond its traditional core of molecular sciences to fields as diverse as chemistry and catalysis, biophysics, nanotechnology and material science.
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