Study and development of new metal-organic frameworks based membranes for separation of multicomponent gas mixtures

用于分离多组分气体混合物的新型金属有机骨架膜的研究和开发

• 批准号: 2607010
• 金额: --
• 依托单位: University of Nottingham
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2021
• 资助国家: 英国
• 起止时间: 2021 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2607010
• 关键词: Study; development; new; metal; organic

This project is focused on development of new metal-organic frameworks (MOFs) based materials for purification/separation of multicomponent gas mixtures. We perform computational modelling in order to design new MOFs membranes for applications of industrial importance including biogas separation and hydrogen adsorption. We develop atomic-scale computational models directly connected to the sorption of gases under realistic conditions and allowing to address its fundamental aspects at the same time. These models are realized in the frame of multi-level workflow, combining both quantum and classical approaches, which provides an opportunity to investigate sorption behaviour of MOFs at a wide range of pressures. While classical force fields cover the normal-pressure region, quantum-level methods are used to study sorption processes under low-pressures, where classical approaches tend to fail quite miserably. We pay significant attention to implementation of the quantum chemical approaches, since MOFs are well-known to be very challenging objects for quantum theory consideration due to the typical big sizes of unit-cell combined with multireference nature of transition metals d-shell. This is reflected in the fact, that routinely used quantum approaches suffer from convergence problems and low computational effectiveness, when applied to MOFs. Therefore, we plan to develop a hybrid quantum chemical model, based on group function concept, allowing effective separation of the system into part, where multireference effects are essential, and environment, allowing single-reference or even force field treatment. Propose methodology will provide an effective and powerful tool for modeling of MOFs with possible applications going beyond sorption properties.

该项目的重点是开发用于净化/分离多组分气体混合物的新型金属有机框架（MOF）材料。我们进行计算建模，以便设计新的 MOF 膜，用于具有重要工业意义的应用，包括沼气分离和氢气吸附。我们开发了与现实条件下气体吸附直接相关的原子级计算模型，并同时解决了其基本问题。这些模型是在多级工作流程的框架下实现的，结合了量子和经典方法，为研究 MOF 在各种压力下的吸附行为提供了机会。虽然经典力场覆盖常压区域，但量子级方法用于研究低压下的吸附过程，而经典方法往往会严重失败。我们非常关注量子化学方法的实施，因为众所周知，由于晶胞的典型大尺寸与过渡金属 d 壳层的多参考性质相结合，MOF 是量子理论考虑中非常具有挑战性的对象。这反映在以下事实中：常规使用的量子方法在应用于 MOF 时会遇到收敛问题和计算效率低的问题。因此，我们计划开发一种基于群函数概念的混合量子化学模型，允许将系统有效地分离为多参考效应至关重要的部分和允许单参考甚至力场处理的环境。所提出的方法将为 MOF 建模提供有效且强大的工具，其可能的应用超出了吸附特性。