Department of Chemical & Petroleum Engineering, University of Pittsburgh, Pittsburgh, PA 15261, USA.
Faraday Discuss. 2017 Sep 8;201:221-232. doi: 10.1039/c7fd00038c.
Designing better porous materials for gas storage or separations applications frequently leverages known structure-property relationships. Reliable structure-property relationships, however, only reveal themselves when adsorption data on many porous materials are aggregated and compared. Gathering enough data experimentally is prohibitively time consuming, and even approaches based on large-scale computer simulations face challenges. Brute force computational screening approaches that do not efficiently sample the space of porous materials may be ineffective when the number of possible materials is too large. Here we describe a general and efficient computational method for mapping structure-property spaces of porous materials that can be useful for adsorption related applications. We describe an algorithm that generates random porous "pseudomaterials", for which we calculate structural characteristics (e.g., surface area, pore size and void fraction) and also gas adsorption properties via molecular simulations. Here we chose to focus on void fraction and Xe adsorption at 1 bar, 5 bar, and 10 bar. The algorithm then identifies pseudomaterials with rare combinations of void fraction and Xe adsorption and mutates them to generate new pseudomaterials, thereby selectively adding data only to those parts of the structure-property map that are the least explored. Use of this method can help guide the design of new porous materials for gas storage and separations applications in the future.
为了在气体存储或分离应用中设计更好的多孔材料，人们通常会利用已知的结构-性质关系。然而，只有在聚合和比较许多多孔材料的吸附数据时，可靠的结构-性质关系才会显现出来。从实验中收集足够的数据非常耗时，即使是基于大规模计算机模拟的方法也面临挑战。当可能的材料数量太大时，不有效地对多孔材料空间进行采样的计算筛选方法可能无效。在这里，我们描述了一种通用且高效的计算方法，用于绘制多孔材料的结构-性质空间，该方法可用于与吸附相关的应用。我们描述了一种生成随机多孔“伪材料”的算法，我们通过分子模拟计算它们的结构特征（例如，表面积、孔径和空隙率）和气体吸附特性。在这里，我们选择关注空隙率和在 1 巴、5 巴和 10 巴下的 Xe 吸附。然后，该算法会识别具有空隙率和 Xe 吸附罕见组合的伪材料，并对其进行突变以生成新的伪材料，从而仅选择性地向结构-性质图中探索最少的部分添加数据。该方法的使用可以帮助指导未来用于气体存储和分离应用的新型多孔材料的设计。
