First-principles approach to in-situ model catalyst studies

原位模型催化剂研究的第一原理方法

• 批准号: 235493617
• 负责人: Professor Dr. Karsten Reuter
• 金额: --
• 依托单位: Abteilung Theorie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2016-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/235493617?language=en
• 关键词: First; principles; approach; situ; model

The purpose of in-situ studies of well-defined single-crystal model catalysts is to transport the rigorous atomic-scale understanding inherent to the ultra-high vacuum Surface Science approach to technologically relevant near-ambient conditions. In corresponding feeds and at typically much higher conversion rates heat and mass transfer limitations in the gas-surface system become increasingly important. Such flow effects in the complex in-situ reactor geometries need to be carefully understood, controlled and at best disentangled to reach the aspired molecular-level understanding of the on-going surface chemistry. In the present project we propose to complement these endeavors by advancing a first-principles based multiscale modeling approach that ranges from the elementary surface catalytic processes to the macro-scale flow profiles. By integrating first-principles kinetic Monte Carlo (1pkMC) microkinetic descriptions into the OpenFoam/CatalyticFoam computational fluid dynamics package we specifically want to generate publicly available general-purpose methodology that can explicitly describe the reaction-transport coupling in fully resolved in-situ reactor geometries. On the materials gap side the approach will be extended from single crystals towards model catalysts featuring nanoparticles on a planar support. For both strands we expect even more and intricate transfer limitations than demonstrated in our preceding work on idealized flow geometries. The conceptual discussion and development will further close the gap between physico-chemical and chemical-engineering type research in heterogeneous catalysis. In addition, the established 1pkMC-flow framework will be employed to quantitatively model in-situ X-ray photoelectron spectroscopy data for CO oxidation on Pd(100).

对定义明确的单晶模型催化剂进行原位研究的目的是将超高真空表面科学方法所固有的严格的原子尺度理解转移到技术相关的近环境条件下。在相应的进料中和在通常高得多的转化率下，气体-表面系统中的传热和传质限制变得越来越重要。在复杂的原位反应器几何形状中的这种流动效应需要仔细理解，控制和最好的解开，以达到对正在进行的表面化学的期望的分子水平的理解。在本项目中，我们建议通过推进基于第一性原理的多尺度建模方法来补充这些努力，该方法的范围从基本表面催化过程到宏观尺度流动剖面。通过将第一原理动力学蒙特卡罗（1 pkMC）微动力学描述集成到OpenFoam/CatalyticFoam计算流体动力学软件包中，我们特别希望生成公开可用的通用方法，该方法可以明确描述完全解析的原位反应器几何形状中的反应-传输耦合。在材料间隙方面，该方法将从单晶扩展到具有平面支撑上的纳米颗粒的模型催化剂。对于这两股，我们期望甚至更多和复杂的传输限制比我们在前面的工作中所展示的理想化的流动几何形状。概念的讨论和发展将进一步缩小多相催化研究中物理化学型与化学工程型之间的差距。此外，所建立的1 pkMC流框架将被用来定量模拟CO在Pd（100）上氧化的原位X射线光电子能谱数据。

项目成果

Synergistic Inhibition of Oxide Formation in Oxidation Catalysis: A First-Principles Kinetic Monte Carlo Study of NO + CO Oxidation at Pd(100)

• DOI: 10.1021/acscatal.6b01344
• 发表时间: 2016-07
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Juan M Lorenzi;S. Matera;K. Reuter

Electrons to Reactors Multiscale Modeling: Catalytic CO Oxidation over RuO2

• DOI: 10.1021/acscatal.8b00713
• 发表时间: 2018-04
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Jonathan E. Sutton;Juan M Lorenzi;J. Krogel;Q. Xiong;S. Pannala;S. Matera;A. Savara

Local-metrics error-based Shepard interpolation as surrogate for highly non-linear material models in high dimensions.

基于局部度量误差的 Shepard 插值作为高维高度非线性材料模型的替代

• DOI: 10.1063/1.4997286
• 发表时间: 2017
• 期刊: The Journal of chemical physics
• 作者: J.M. Lorenzi;T. Stecher;K. Reuter;S. Matera
• 通讯作者: S. Matera