Computational studies of reaction mechanisms of methane monooxygenase and ribonucleotide reductase.

摘要: An overview of the computational efforts made by our group during last few years in field nonheme diiron proteins is presented. Through application ab initio methodology to a reasonable set molecular models, significant progress understanding how soluble Methane Monooxygenase system achieves hydroxylation methane and catalytic cycle Ribonucleotide Reductase initiated. In particular, current studies reveal more detail (1) nature key intermediates reaction cycles these two metalloenzymes, (2) details iron centers regulate systems, (3) important aspects carboxylate ligands active sites may tailor enzymatic needs metalloprotein. This knowledge also leads novel connections between enzymes. The coordinative unsaturation shifts investigated herein are properties that likely be general impact proteins. control redox chemistry enzyme binuclear metal center, analyzed here, should find common ground among other bimetallic systems as well.