Electronic structure calculations of oxidation reactions on nanoporous gold

纳米多孔金氧化反应的电子结构计算

• 批准号: 269856222
• 负责人: Professor Dr. Thorsten Klüner
• 金额: --
• 依托单位: Arbeitsgruppe Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Units
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/269856222?language=en
• 关键词: Electronic; structure; calculations; oxidation; reactions

This scientific proposal is devoted to elucidation of the detailed mechanisms involved in the total and partial oxidation of methanol on model AuCu alloy surfaces as well as the elucidation of the detailed mechanism involved in the oxidation of propylene on model AuAg and AuCu alloy surfaces. Along these lines, atomistic insight into complex chemical processes on nanoporous Au will be obtained. Theoretical prediction of the key reaction intermediates, their adsorption geometry, binding strengths, vibrational frequencies, as well as modeling of STM images will support the analysis and interpretation of experimental data. In particular, we will provide a mechanistic description of the reactivity (as a function of the ad-metal concentration and that of active forms of oxygen, OH and water) and rate constants of critical reaction steps calculated on the basis of electronic structure calculations. Our DFT and highly accurate ab initio calculations of the propylene oxidation will be compared to AIMD simulations to provide a complete understanding of the underlying processes.

该科学建议致力于阐明模型AuCu合金表面上甲醇的全部和部分氧化所涉及的详细机制，以及阐明模型AuAg和AuCu合金表面上丙烯的氧化所涉及的详细机制。沿着这些路线，将获得复杂的化学过程的纳米多孔Au原子的见解。关键反应中间体的理论预测，它们的吸附几何形状，结合强度，振动频率，以及STM图像的建模将支持实验数据的分析和解释。特别是，我们将提供一个机械的反应性（作为广告金属浓度和活性形式的氧，OH和水的函数）和速率常数的关键反应步骤的基础上计算的电子结构计算的描述。我们的DFT和丙烯氧化的高精度从头计算将与AIMD模拟进行比较，以提供对潜在过程的完整理解。