Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation.

Liu, Yan; Qin, Lang; Cheng, Zhuo; Goetze, Josh W; Kong, Fanhe; Fan, Jonathan A; Fan, Liang-Shih · Nat Commun · 2019

basic_science · Level V

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Abstract

Chemical looping methane partial oxidation provides an energy and cost effective route for methane utilization. However, there is considerable CO<sub>2</sub> co-production in current chemical looping systems, rendering a decreased productivity in value-added fuels or chemicals. In this work, we demonstrate that the co-production of CO<sub>2</sub> can be dramatically suppressed in methane partial oxidation reactions using iron oxide nanoparticles embedded in mesoporous silica matrix. We experimentally obtain near 100% CO selectivity in a cyclic redox system at 750-935 °C, which is a significantly lower temperature range than in conventional oxygen carrier systems. Density functional theory calculations elucidate the origins for such selectivity and show that low-coordinated lattice oxygen atoms on the surface of nanoparticles significantly promote Fe-O bond cleavage and CO formation. We envision that embedded nanostructured oxygen carriers have the potential to serve as a general materials platform for redox reactions with nanomaterials at high temperatures.