COMPUTATIONAL INVESTIGATION OF THE INTERACTION OF MULTI-FUNCTIONALIZED POROUS AROMATIC FRAMEWORKS WITH PURE SO2 AND GAS MIXTURES
Restricted (Penn State Only)
- Author:
- Wang, Yuxiang
- Graduate Program:
- Materials Science and Engineering
- Degree:
- Doctor of Philosophy
- Document Type:
- Dissertation
- Date of Defense:
- August 02, 2023
- Committee Members:
- Susan Sinnott, Chair & Dissertation Advisor
Ismaila Dabo, Major Field Member
Lauren Zarzar, Outside Field Member
Adri van Duin, Outside Unit & Field Member
John Mauro, Program Head/Chair - Keywords:
- Functionalized Porous Aromatic Frameworks
Acid Gas Adsorption
Grand Canonical Monte Carlo Simmulations - Abstract:
- In recent years, advancements in computer processors and the development of computational resources have enabled atomic-scale computation and simulation in materials science to became powerful tools that can be used to better understand nano-scale structures and their correlations to macroscopic properties. The insights revealed by these calculations and simulations, are often difficult to obtain from experimental measurements, and are essential to not only screening and designing new materials with desired properties, but also to predicting or verifying material properties in conjunction with experimental data. In this dissertation, multiple atomistic-scale computational methods, such as density functional theory calculations, grand canonical Monte Carlo simulations, and other structural modeling procedures and tools, are utilized to explore and investigate the atomistic structures, gas adsorption behavior, and associated gas separation of a unique family of porous materials – the porous aromatic frameworks (PAFs). In particular, these methods are used to screen and examine several various PAF structures that have different chemical functional groups attached to the aromatic rings that make up the PAFs. These methods additionally consider several possible configurations of functional groups and functional group locations, in terms of their abilities to enhance gas adsorption by the PAFs, as well as the use of PAFs to separate acid gases from gaseous mixtures under different pressures. The results indicated that multiple combinations of PAF functionalization, especially -OH and -COOH are able to greatly enhance low-pressure acid gas adsorption. In addition, for binary gas mixtures with dilute concentrations of acid gases, PAFs with electron-donating groups such as -COOH exhibit strong interactions with acid gases at low pressures, resulting in high acid gas loadings and selectivity. At elevated pressures, the maximum adsorption limits of the PAFs are dominated by pore volumes, which are greatly dependent on the size of the chemical functional groups. Furthermore, the results from investigating PAFs with two different functional groups for selective adsorption indicated that mixing two different functional groups on PAF’s aromatic rings has great potential to further enhance acid gas loading and adsorption selectivity.