| With the increase in the production of plastics, there is a high demand for developing polymers with controlled degradation. In this thesis, we model the degradation of polymers via first-principles quantum chemistry and identify polymer candidates with enhanced degradation behaviour using virtual high-throughput screening. We investigate two different pathways of polymer degradation, i.e., thermal degradation and hydrolysis, and further develop the necessary computational protocols for a virtual high-throughput screening and materials informatics investigation of degradable polymers. We studied the degradation reaction mechanisms using density functional theory (DFT) at PBE0 level of theory. We selected ethylene di-benzoate (EDB), propylene di-benzoate (PDB), butylene di-benzoate (BDB) and ethyl acetate as representative compounds for polyesters. We used EDB, PDB and BDB to study the thermal degradation, and used ethyl acetate for the hydrolysis mechanism. We validated the calculated activation energies for these degradation mechanisms using experimental results from the literature. Using our in-house library generator (ChemLG), we generated a large library of potential polymers and evaluated their activation energies by casting in a virtual high-throughput screening framework. In addition to identifying the top candidates, we further provide insights into the relationship between polymer structure and the rate of degradation. |
