In this thesis, Xiaoshi Wang investigates the function and
mechanism of a newly discovered heme-thiolate peroxygenase, AaeAPO.
This enzyme class comes from Agrocybe aegerita and is used in the
conversion of inert hydrocarbons to alcohols. Xiaoshi's work
focuses on an extracellular P450 enzyme which is not limited in its
stability and lack of solubility and therefore is relevant for
widespread industrial use. The author demonstrates that the
peroxygenase catalyzes a wide range of reactions. In some cases the
author even describes very difficult transformations in molecules
that are highly inert. Her detailed investigations provide a
mechanistic framework for how the peroxygenase catalyzes such a
large number of reactions. A major highlight of this thesis is the
identification of key short-lived intermediates in the catalytic
cycle of the peroxygenase, using rapid kinetic and spectroscopic
methods, as well as the elucidation of the thermodynamic properties
of these high-energy intermediates. This work adds new insight into
an important class of enzymes.
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