(553e) Theoretical Investigations of Modified Active Site Models for Fe-Only Hydrogenases

Designing inexpensive and efficient catalysts for hydrogen activation is a great challenge. Biomimetic studies of hydrogenase enzymes provide a new approach for this purpose. Based on the generally accepted catalytic mechanism for hydrogenases, we propose a modified structure of the Fe-only hydrogenase active site and study the activities of the models using density functional theory. It is found that changes in the nature of the ligands and in the species of the bases representing the environment can improve the catalytic activities. The investigations provide a new approach for biomimetic catalyst design.