Abstract

As an emerging subclass of advanced nanoporous materials, covalent triazine frameworks (CTFs) possess distinct properties such as high specific surface area, large pore volume, exceptional thermal/chemical stability, and structural designability. Thus, they have many real-world applications, including, but not limited to, catalysis, energy storage and conversion, adsorption, chemical sensing, and separation. In this doctoral dissertation, three projects related to CTF materials have been performed. Firstly, two electron-rich π-conjugated CTFs with high specific surface area and pore volume were synthesized via the facile and convenient Friedel-Crafts alkylation reaction of cyanuric chloride and trans-stilbene (TS) as well as diphenylacetylene (DPA), containing conjugated C=C double bond and C≡C triple bond functionalities, respectively. The iodine-capturing performance of these two electron-rich CTFs was investigated in a combined experimental-computational approach. Secondly, to design novel functionalized CTFs suitable for heavy metal cations removal from aqueous solutions, a DFT-assisted computational screening approach was employed on various CTFs featuring different electron-rich functionalities with negatively charged atom(s) for efficient adsorption of Cd2+, Pb2+, and Hg2+ cations as three most biohazardous heavy metal species. The metal removal process was also investigated in a combined experimental-computational approach. Thirdly, the gas adsorption and sensing properties of the pristine CTF-1 covalent triazine framework and its platinum atom (Pt)-doped counterpart were investigated computationally for SF6 decomposition products (i.e., H2S, SO2, SOF2, and SO2F2 gases) using the density-functional theory (DFT) method. In this framework, density of states (DOS) analysis examined the adsorption and sensing mechanisms. Computational and experimental results obtained in this dissertation confirmed the promising performance of the CTF materials in efficiently eliminating environmental micropollutants via adsorption.