Na-β-Al2O3 stabilized Fe2O3 oxygen carriers for chemical looping water splitting: correlating structure with redox stability

Chemical looping is an emerging technology to produce high purity hydrogen from fossil fuels or biomass with the simultaneous capture of the CO2 produced at the distributed scale. This process requires the availability of stable Fe2O3-based oxygen carriers. Fe2O3-Al2O3 based oxygen carriers exhibit a decay in the H-2 yield with cycle number, due to the formation of FeAl2O4 that possesses a very low capacity for water splitting at typical operating conditions of conventional chemical looping schemes (700-1000 degrees C). In this study, the addition of sodium (via a sodium salt) in the synthesis of Fe2O3-Al2O3 oxygen carriers was assessed as a means to counteract the cyclic deactivation of the oxygen carrier. Detailed insight into the oxygen carrier's structure was gained by combined X-ray powder diffraction (XRD), X-ray absorption spectroscopy (XAS) at the Al, Na and Fe K-edges and scanning transmission electron microscopy/energy-dispersive X-ray spectroscopy (STEM/EDX) analyses. The addition of sodium prevented the formation of FeAl2O4 and stabilized the oxygen carrier via the formation of a layered structure, Na-beta-Al2O3 phase. The material, i.e. Na-beta-Al2O3 stabilized Fe2O3, showed a stable H-2 yield of ca. 13.3 mmol g(-1) over 15 cycles.