Ni metal is a widely used catalyst for ethanol steam reforming due to its ability to activate C-C and C-H bonds; however, Ni suffers from poor selectivity and fast deactivation. It has been previously shown that the performance of nickel can be dramatically improved by the addition of a CeO2 co-catalyst. Here we investigate the nature and length scaling for bifunctional activity at the phase boundary between Ni and CeO2. We show that deposition of CeO2 nanoparticles onto a planar Ni surface leads to two types of interfaces: 1) the nanoscale interface defined by the contact of individual CeO2 nanoparticles with the metal catalyst and 2) a larger, mesoscale interface defined by the boundary between domains of a self-assembled nanoparticles and the surrounding clean metal substrate. Measuring reaction kinetics as a function of CeO2 coverage on Ni reveals that the kinetics of H2 production during ESR are strongly dependent on the mesoscale morphology of CeO2 nanoparticles on the Ni surface. On active catalysts, we find that Ni and CeO2 phases are separated by the growth of carbon nanotubes that carry Ni away from the surface via a tip-growth mechanism. Using ambient pressure XPS, we find that surface hydroxyl groups, which form on CeO2 migrate along the carbon nanotubes to the Ni tips, dramatically enhancing the kinetics of hydrogen production.

Bifunctional catalysis at multiple length scales: Understanding the metal-support interface during ethanol steam reforming on nickel-cerium oxide catalysts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.