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Gas separation in microporous materials: A computational study of the influence of structural features on the selectivity

微孔材料中的气体分离：结构特征对选择性影响的计算研究

基本信息

批准号：
214172356
负责人：
Dr. Michael Fischer
金额：
--
依托单位：
Fachgebiet Kristallographie und Geomaterialforschung
依托单位国家：
德国
项目类别：
Research Fellowships
财政年份：
2011
资助国家：
德国
起止时间：
2010-12-31 至 2013-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/214172356?language=en
关键词：
Gas separation microporous materials computational

项目摘要

In this project, computational chemistry techniques are employed to evaluate the potential of different microporous materials (zeolites, metal-organic frameworks, nanoporous molecular crystals) for adsorption-based gas separation applications. A particular emphasis is put on a detailed analysis of the role of specific interaction sites, such as extra-framework cations, coordinatively unsaturated metal sites, or functional groups, in conjunction with confinement to micropores. The investigation addresses different gas mixtures that are of relevance for industrial processes, for example in the removal of carbon dioxide from flue gases or from natural gas, or in the separation of alkane/alkene mixtures.The project follows a hierarchical approach: Firstly, grand-canonical Monte Carlo (GCMC) simulations using empirical interaction parameters are carried out for a wide variety of candidate materials, permitting an initial estimation of the adsorption selectivity. A more thorough GCMC study of the separation properties is then carried out for the most interesting systems that were identified in this screening. The relationships between the observed separation behaviour and the structural properties of the material (specific interaction sites, pore size, pore topology) are analyzed in detail. In the following, quantum-chemical calculations are carried out to develop a better understanding of the interactions between specific sites and adsorbed molecules. Molecular dynamics calculations are performed to analyze the impact of these sites on the diffusion of guest molecules. In the final part of the project, the adsorption properties of hypothetical zeolites are predicted. Due to their structural versatility, these systems are particularly well suited for a systematic study of the influence of the pore topology.

在该项目中，采用计算化学技术来评估不同微孔材料（沸石、金属有机框架、纳米多孔分子晶体）用于基于吸附的气体分离应用的潜力。一个特别强调的是放在一个具体的相互作用的网站，如框架外阳离子，配位不饱和金属网站，或官能团，结合限制微孔的作用的详细分析。该研究针对与工业过程相关的不同气体混合物，例如从烟道气或天然气中去除二氧化碳，或分离烷烃/烯烃混合物。该项目采用分层方法：首先，使用经验相互作用参数对各种候选材料进行巨正则蒙特卡罗（GCMC）模拟，允许对吸附选择性进行初始估计。一个更彻底的GCMC研究的分离性能，然后进行了最有趣的系统，确定在这个筛选。详细分析了所观察到的分离行为和材料的结构性质（特定的相互作用位点，孔径，孔拓扑结构）之间的关系。在下文中，进行量子化学计算以更好地理解特定位点和吸附分子之间的相互作用。分子动力学计算进行分析这些网站上的客体分子的扩散的影响。在项目的最后部分，预测了假设的沸石的吸附性能。由于其结构的多功能性，这些系统特别适合于系统研究孔拓扑结构的影响。