This thesis aims to develop computational methods an‎d identify key factors for enhancing the efficiency of catalytic reactions an‎d metal–water systems. In the first part, a novel parameterization for studying Au–H₂O systems was introduced, based on generating new pair parameters using the DFTB module in Materials Studio 2020. Extensive tests on clusters, monolayer an‎d bilayer surfaces, an‎d metal–water complexes showed that the DFTB-AuOH library accurately reproduces the structural an‎d energetic characteristics of these systems, an‎d its predicted dynamic behavior closely aligns with DFT calculations. Subsequently, in the second part of the thesis, a similar parameterization was performed for Ag–H₂O systems, leading to the introduction of the DFTB-AgOH library. The results demonstrated that this library correctly predicts stable structures an‎d adsorption sites of water molecules on silver surfaces, while often outperforming previous parameter sets (DFTB-HYB). In the third part of the thesis, the focus was placed on the WGS reaction as a key process in hydrogen production an‎d the development of high-efficiency renewable energy carriers. According to the known mechanism of this reaction, the weakening of the CO bond constitutes the critical first step for lowering the activation barrier an‎d facilitating the reaction. Accordingly, a novel approach utilizing the bidentate nature of CO an‎d the formation of a carboxyl-bridge (iso-carbonyl) complex with transition metal oxides an‎d Lewis acids was pursued. Computational results showed that heavy transition metals such as Rh, Ir, an‎d Ni, together with strong group 13 Lewis acids like Al, Ga, an‎d In, exhibit the highest ability to transfer charge to the anti-bonding orbital of CO, significantly stretching an‎d weakening the bond. Ultimately, pairs such as AlCl3—CO—Ni2O2, Ga2O3—CO—Rh2O, an‎d B2O3—CO—Rh2O were identified as the most effective combinations for CO bond activation.

حسين فرخ پور

حسن حداد زاده

رضا اميديان , محسن افتاده , حسين توكل