In this talk, single-metal atom catalytic site on a low dimensional porous surfaces such as phthalocyanine/porphyrin functionalized graphene materials have been screened and characterized for the CâH bond activation of methane to methanol conversion process using first principles density functional theory (DFT) calculations. The radical mechanism, the predominant mechanism for the CâH bond activation process of methane, was observed for these type of materials. An inverse correlation between the metal-oxo species formation energy and the CâH bond activation energy was observed and both of them have a nice correlation with an electronic descriptor known as metal charge state of the metal-oxo species of these materials. The optimal performance of the catalysts can then be screened based on this correct electronic descriptor which does not break away the relationship. The catalytic activity of this system can further be tuned by controlling the metal charge state of the metal center via
both substrate doping and ligand exchange.
Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund (ACS-PRF, 58740-UR6) for support of this research. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1548562, TACC at the stampede2 through allocation [TG-DMR140131]. Use of the Center for Nanoscale Materials was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.