Theoretical Investigation of On-Purpose Propane Dehydrogenation over the Two-Dimensional Ru-Pc Framework

摘要

The on-purpose dehydrogenation of light alkanes has received considerable interest for producing olefins from abundant and cheap feedstock. The prevalent catalysts have been limited to Pt-Sn/Al2O3 and Cr2O3/Al2O3. In this work, we demonstrate by density functional theory that two-dimensional Ru-phthalocyanine (2D Ru-Pc) is a potential single-atom catalyst for selective alkene production via direct C-H bond activations. By analyzing the reaction pathways and the electronic structures of the transition states, we show that the catalytic origin of 2D Ru-Pc in C-H bond activations is the highly exposed d orbitals of the single Ru atom. The alkene selectivity can be attributed to the weak Ru-pi binding interaction between the produced alkene and the 2D Ru-Pc catalyst. The distinct catalytic selectivity of such a 2D Ru-Pc catalyst may inspire further investigations of selective dehydrogenation of light alkanes on single-metal catalysts.