Dynamic Catalyst Restructuring and Interface Instabilities: A Combined Experimental and Computational Study

动态催化剂重组和界面不稳定性：实验和计算相结合的研究

• 批准号: 409299786
• 负责人: Professor Dr. Ronald Imbihl
• 金额: --
• 依托单位: Institut für Physikalische Chemie und Elektrochemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2018
• 资助国家: 德国
• 起止时间: 2017-12-31 至 2021-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/409299786?language=en
• 关键词: Dynamic; Catalyst; Restructuring; Interface; Instabilities

In the bistable regime of the NH3+ O2 and the CH3OH + O2 reactions on a Rh(110) surface a novel type of interface instability has been observed recently. Under reaction conditions of equistability of the two phases the interface oxygen rich/oxygen poor is not stationary but exhibits localized excitations which travel pulse-like along the front line. In the current project we try to determine the mechanism of the traveling interface instabilities in a combined experimental/theoretical approach. Based on the idea that the instability is due to a coupling between reaction-induced surface roughening and local excitations of the reaction we try to set up a realistic mathematical model that reproduces the observed phenomena. In Hannover we will conduct in situ microscopy in order to identify the essential steps of the proposed mechanism. In close collaboration between the groups at Hannover and Moscow a realistic reaction-diffusion model shall be developed. The simulation and the analysis of the simulation results will be conducted by the Moscow group. If successful, the simulation would provide us with a potential mechanism for reaction-induced roughening in catalysis.

在Rh（110）表面上的NH_3 + O_2和CH_3OH + O_2反应中，发现了一种新的界面不稳定性。在两相等稳定性的反应条件下，富氧/贫氧界面不是静止的，而是呈现出沿着前线脉冲状传播的局部激发。在目前的项目中，我们试图确定的机制，结合实验/理论的方法的行进界面不稳定性。基于不稳定性是由于反应引起的表面粗糙化和反应的局部激发之间的耦合的想法，我们试图建立一个现实的数学模型，再现所观察到的现象。在汉诺威，我们将进行原位显微镜，以确定所提出的机制的基本步骤。在汉诺威和莫斯科的小组之间密切合作下，应开发一个现实的反应扩散模型。模拟和模拟结果分析将由莫斯科小组进行。如果成功的话，模拟将为我们提供一个潜在的机制，反应诱导粗糙催化。

项目成果

Simulation of traveling interface pulses in bistable surface reactions.

双稳态表面反应中行进界面脉冲的模拟

• DOI: 10.1103/physreve.100.042206
• 发表时间: 2019
• 期刊: Physical review. E
• 作者: Alexei Makeev;Ronald Imbihl
• 通讯作者: Ronald Imbihl

Redistribution dynamics of ultrathin vanadium oxide layers under catalytic conditions and activation of diffusion by surface acoustic waves

催化条件下超薄氧化钒层的重新分布动力学和表面声波扩散激活

• DOI: 10.15488/9805
• 发表时间: 2020
• 作者: Bernhard von Boehn

Dynamics of Ultrathin Vanadium Oxide Layers on Rh(111) and Rh(110) Surfaces During Catalytic Reactions

Rh(111) 和 Rh(110) 表面超薄氧化钒层催化反应过程中的动力学

• DOI: 10.3389/fchem.2020.00707
• 发表时间: 2020
• 期刊: Frontiers in Chemistry
• 影响因子: 5.5
• 作者: Bernhard von Boehn;Ronald Imbihl
• 通讯作者: Ronald Imbihl

Structural Transitions Driving Interface Pulses in Methanol Oxidation on Rh(110) and VOx/Rh(110): A LEEM Study

Rh(110) 和 VOx/Rh(110) 甲醇氧化中结构转变驱动界面脉冲：LEEM 研究

• DOI: 10.1021/acs.jpcc.1c06106
• 发表时间: 2021
• 期刊: The Journal of Physical Chemistry C
• 作者: Bernhard von Boehn;Jon-Olaf Krisponeit;Jens Falta;Ronald;Imbihl
• 通讯作者: Imbihl