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Coverage-dependent Behaviors of Vanadium Oxides for Chemical Looping Oxidative Dehydrogenation.

Chemical looping provides an energy and cost effective route for alkane utilization. However, there is considerable CO 2 co-production caused by kinetically mismatched O 2- bulk diffusion in current chemical looping oxidative dehydrogenation systems, rendering a decreased olefin productivity. This paper describes the successful construction of sub-monolayer or monolayer vanadia nanostructures to suppress CO 2 production in oxidative dehydrogenation of propane by evading the interference of O 2- bulk diffusion (monolayer versus multi-layer). The highly dispersed vanadia nanostructures on titanium dioxide support showed over 90% propylene selectivity at 500 °C, exhibiting highest turnover frequency of 1.9×10 -2 s -1 , which is over 20 times greater than that of conventional crystalline V 2 O 5 oxygen carriers. Combining in situ spectroscopic characterizations and density functional theory calculation, we revealed the loading-reaction barrier relationship through the vanadia/titanium interfacial interaction. This work demonstrates that sub-monolayer or monolayer nanostructures have the potential to serve as a general oxygen carrier materials platform for redox reactions.