The Quest to Reliable Structure-Property Relationships in Methanol Steam Reforming

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Methanol steam reforming, that is, the generation of hydrogen and carbon dioxide from methanol and water is to date one of the most promising heterogeneously catalyzed chemical reactions for on-board hydrogen storage and use. Its particular advantage is mainly based on the high hydrogen-to-carbon ratio (3:1), if the reaction is led highly CO2-selective. To achieve this goal, at the moment a range of also technologically used and already well-characterized catalyst systems are exploited, including copper-zinc oxide catalysts or intermetallic compounds on palladium basis. However, the used catalysts suffer from the severe drawbacks of either being prone to serious sintering upon catalyst activation or even during reaction, or, in the case of palladium-based intermetallic compounds, being structurally highly dynamic systems. This typically hampers the determination of the catalytically active centers leading to high CO2 selectivity. The copper-zirconium oxide catalysts discussed in the project "The Quest to Reliable Structure-Property Relationships in Methanol Steam Reforming" exhibit not only a high CO2 selectivity with at the same time multiple activities compared to used materials, but as a particular advantage also offer also an increased structural and chemical stability. This is mainly due to the inherent chemical inactivity of zirconium oxide, which simplifies the determination of the associated catalytically active and selective sites. To reach the set goal, new grounds of catalyst preparation and synthesis need to be broken as well as dedicated structural and chemical characterization techniques capable of resolving structure, morphology and chemistry during reaction applied to optimize the chemistry of the two components copper and zirconium oxide. Only by this knowledge-based approach, a new catalyst material with enhanced activity and selectivity with at the same time structurally stable catalytic center finally results, enabling setting-up reliable structure-property relationships for methanol steam reforming.