(509de) High Throughput Screening of Bio-Inspired Mo/W Catalysts

A rational approach to establish an enzyme’s blueprint and understand what can be translated into mimics is needed for rational, bioinspired catalyst design. The essential step is to unravel the structure-property relationship for the catalytic active sites. The enzymes containing Mo/W are found to catalyze several essential redox reactions in metabolism. Numerous efforts have been made to synthesize the Mo/W-containing inorganic molecular complexes and understand their structure-property relationships with the goal of mimicking the catalytic function enzymes. In this talk, I will present one type of Mo/W-containing enzyme-formate dehydrogenase (FDH) as an example for bio-inspired molecular complexes design. Due to the challenges in elucidation of catalyzing mechanisms in enzymatic reactions, stability and fine-tuned ligand of molecular complexes, the complete structure-property relationship has not been established yet. In our study, we carried out a high-throughput screening on all mononuclear Mo/W complexes recorded in Cambridge Structural Database (CSD) and narrowed down our focus on the complexes with structural analogue to FDH. Combining DFT simulations and high throughput virtual screening of hundreds of complexes, we systematically investigated the effects of monodentate chalcogen ligands and transition metals in their structural, electronic and catalytic properties. We also compared the results from DFT simulations on molecular complexes with QM/MM simulations on enzyme’s cofactor. Our work will help clarify ligand-metal interactions statistically and construct the comprehensive structure-property relationship for Mo/W-containing complexes.