(618h) Computational Study of Methane Activation on ?-Al2O3

Despite the large availability of methane in shale gas reservoirs, its utilization has been a longstanding challenge in the chemical industry. Due to the high C-H bond strength of methane, an industrially-viable process for the efficient and selective conversion of methane to higher value chemicals has not been realized yet. Towards activating the C-H bond of methane, various metal oxides have been widely explored. However, the detailed C-H activation mechanisms on metal oxides are not fully understood, thus, limiting the development of models describing C-H activation behavior with catalyst properties. Herein, using density functional theory calculations we studied the C-H activation of methane on various sites of low-index surface facets of γ-Al₂O₃. The feasibility of C-H activation on different metal-oxygen (acid-base) site pairs was assessed through two potential mechanisms (radical and polar). By identifying key catalyst properties we developed structure-activity relationships for C-H activation of methane on γ-Al₂O₃. The obtained relationships can be utilized to accelerate the discovery of active C-H activation catalysts.