Enhanced hydrogen storage in Ni/Ce composite oxides

• Published in: Physical chemistry chemical physics : PCCP 2007-01, Vol.9 (45), p.6032-6039
• Main Authors: Berlouis, Léonard E A, Jubin, Clotilde, McMillan, Brian G, Morrow, James, Spicer, Mark D, Tang, Leung P, Bordelanne, Olivier, Weston, Michael
• Format: Article
• Language: English
• Subjects: Calcium Compounds - chemistry; Carbon Dioxide - chemistry; Catalysis; Cerium - chemistry; Hydrogen - chemistry; Nanotechnology - methods; Nickel - chemistry; Oxides - chemistry; Surface Properties; Temperature; Thermogravimetry; Time Factors; Water - chemistry; X-Ray Diffraction
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/b710026d

The properties of dried (but not calcined) coprecipitated nickel ceria systems have been investigated in terms of their hydrogen emission characteristics following activation in hydrogen. XRD and BET data obtained on the powders show similarities to calcined ceria but it is likely that the majority of the material produced by the coprecipitation process is largely of an amorphous nature. XPS data indicate very little nickel is present on the outermost surface of the particles. Nevertheless, the thermal analytical techniques (TGA, DSC and TPD-MS) indicate that the hydrogen has access to the catalyst present and the nickel is able to generate hydrogen species capable of interacting with the support. Both unactivated and activated materials show two hydrogen emission features, viz. low temperature and high temperature emissions (LTE and HTE, respectively) over the temperature range 50 and 500 degrees C. A clear effect of hydrogen interaction with the material is that the activated sample not only emits much more hydrogen than the corresponding unactivated one but also at lower temperatures. H(2) dissociation occurs on the reduced catalyst surface and the spillover mechanism transfers this active hydrogen into the ceria, possibly via the formation and migration of OH(-) species. The amount of hydrogen obtained (~0.24 wt%) is approximately 10x higher than those observed for calcined materials and would suggest that the amorphous phase plays a critical role in this process. The affiliated emissions of CO and CO(2) with that of the HTE hydrogen (and consumption of water) strongly suggests a proportion of the hydrogen emission at this point arises from the water gas shift type reaction. It has not been possible from the present data to delineate between the various hydrogen storage mechanisms reported for ceria.