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Research
Thrusts

THRUST 3

Catalytic Bias

Mechanisms for controlling directional catalytic rates in proton-coupled electron transfer reactions. We are examinig the mechanisms by which catalytic redox centers can be tuned (1) the reduction potentials of bound redox cofactors, (2) the pKas of groups involved in proton transport and (3) binding affinities for substrates, products and inhibitors, since all of these factors can be expected to shape the reactivity of bound flavins and FeS clusters. Our approach integrates informatic, spectroscopic, electrochemical, kinetic, biophysical and biochemical methods. Our goal is define the structural determinants and limits of control of catalytic bias in model metallo- and flavoenzymes These studies, integrated with the insights gained in Thrusts 1 and 2, will advance our long-term goal of defining the fundamental parameters associated with control of electron flow in chemical bond forming reactions.