摘        要：In this seminar, I will present my computational studies on catalysis (including heterogeneous
catalysis, molecular catalysis, and electrocatalysis) for alkane functionalization, methane to
methanol transformation, and solar fuel production. The goals are to understand existing
industrially important catalysts so that they can be improved and put into practical use soon, and
to develop inexpensive and efficient catalysts for low-carbon fuel production.
For heterogeneous catalysis, I have studied the mechanism of n-butane selective oxidation to
maleic anhydride on a vanadium phosphorus oxide surface (VPO). Surprisingly, I found that
O(1)=P on the VVOPO4 surface is the active center for initiating the VPO chemistry through the
extraction of H from alkane C-H bonds. This work not only sheds light on the VPO chemistry
but also demonstrates the importance of main group oxos in heterogeneous catalytic reactions. I
then proposed a series of organometallic molecules that activate C–H bonds through this unique
mechanism.
My research for molecular catalysis has been focus on methane-to-methanol transformation,
particular on oxy-functionalization, in which C-O bond is formed. I have discovered a new
mechanism for generating C-O bonds from metalhydrocarbyls. This mechanism proceeds
through an intermolecular hydrocarbyl migration to the oxo of a separate oxidant leading to oneelectron
reduction for metals on both the reactant and oxidant. It represents one of the few for
oxy-functionalizing metal-carbon bonds.
For electrocatalysis, I have studied the electrochemical oxygen evolution reaction (OER) of
water and the oxygen reduction reaction (ORR) on metal-porphyrin-like centers incorporated
into carbon nanostructures. I discovered that the overpotential for OER and ORR can be reduced
over a range greater than 0.30 V by choice of the axial ligand. Based on this discovery, I have
proposed two novel designs of electrocatalysts for OER and ORR.