In an effort to move toward a CO2-neutral energy cycle, alternate high energy carriers such as hydrogen (H2) have been studied. However, the safe storage and transport of H2, an explosive (in air) and flammable gas, poses challenges. As an alternative, the controlled storage and release of H2 has been widely studied in hydrogen storage materials. Promising examples of these materials are ammonia-borane (AB) and formic acid (FA). Hydrogen storage materials also have the potential to act as a convenient in-situ source of H2 for hydrogenation reactions, that typically require high temperatures and external pressurized hydrogen to occur.<br/><br/>In this work, we synthesized CuNi nanoparticles (NPs) to act as both dehydrogenation catalysts for the methanolysis of AB and subsequent tandem hydrogenation catalysts for nitro/nitrile hydrogenation. With our catalyst, supported on graphene (G), we are able to perform both reactions in one pot at room temperature, without the use of external pressurized hydrogen. AB dehydrogenation activity under these mild conditions reaches a turnover frequency (TOF) of 49.1 / min which rivals, and in many cases outperforms, noble metal catalysts. Subsequent nitro/nitrile hydrogenation in the same pot demonstrates the potential for using a NP catalyst efficienctly for two different reactions, therefore using greener reaction conditions. Our work furthers the understanding of non-noble metal catalysts for the dehydrogenation of hydrogen storage materials, as well as demonstrates the potential of using such a system for other hydrogenation reactions relevant for the synthesis of industrial chemicals and fuels. Recent efforts to develop other non-noble metal catalysts for tandem hydrogenation/dehydrogenation reactions will also be highlighted.

Non-noble metal nanoparticle catalysts for dehydrogenation/hydrogenation reactions

254th National Meeting (2017)

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