(626h) Single-Atom Active Sites for Natural Gas to Liquid Fuel Conversion

In this work, we
will discuss the study of large macrocyclic molecules, transition metal phthalocyanines,
as the single-atom metal active sites for the methane catalytic oxidation.  The
hypothesis of this work is that single-atom metal active sites (analogous to
metal-oxo species of monooxygenase enzyme) can be created on a porous sheet of
transition metal phthalocyanine (TMPc) deposited on 2D graphene substrate.  We
modeled this catalytic reaction process using ab initio density functional
theory (DFT) to develop an understanding of functionalization, reaction
energetics, and reaction mechanism at the atomic level.  Our results indicate
that this material will have significant advantages over conventional catalysts
for the selective oxidation of natural gas to methanol conversion process at
mild reaction condition.  Our results also indicate that chemical doping of
substrate can play an important role on catalytic activity of TMPc surface by
donating/backdonating necessary electrons from/to the substrate and create
additional activity on the active metal sites during methane oxidation
reaction.  This active sites will provide not only a low energy barrier for C-H
bond dissociation but also a high selectivity towards the desired methanol
product.  This information will be helpful to develop a novel catalyst that will
have significant advantages over conventional catalysts for the selective
oxidation of natural gas to methanol conversion process at mild condition.  

Acknowledgement:

DFT calculation work was
also supported from NSF-XSEDE resources under allocation number [TG-DMR140131].