Mechanically mixed Pd salt nanoparticles with polycrystalline CeO2 powder yielded an active Pd-O-Ce interface with high activity for the dry reforming of methane (DRM: CH4+CO2 --&gt; 2CO + 2H2) where the breaking of the C-H bond is the reaction’s limiting step. A synergistic interaction between embedded Pd onto CeO2 led to rapid catalytic turnover. Pd-based formulation was effective in methane activation, while the CeO2 facilitated the dispersion and Pd-Ce interfacial interaction. Activity of the milled Pd/CeO2 greatly surpassed that of the conventional incipient wetness method on tests carried out in a bed-flow reactor setup. These catalysts were also tested for CO2 hydrogenation where the milled sample produced mainly CO through the reverse water gas shift at a higher rate than the incipient wetness method. Drastic changes between both materials were traced to the unique Pd-CeO2 interface granting better O-transfer capabilities. The catalyst’s structural integrity and chemical state evolution during reaction were probed employing in-situ characterization tools. Methane Temperature Programmed Reduction (CH4-TPR) results showed remarkable activation of methane at low temperatures and high CH4 conversion while in-situ XRD and XAS were used to pinpoint the active structure evolution and electronic environment. Stability experiments were run under reaction conditions and further analyzed using HRTEM showing no sintering or coking of the metal even after 24 hours of exposure at elevated temperatures. In addition, possible reaction pathways and stable surface intermediates were identified using DRIFTS. A systematic combined in-situ approach was used to understand how Pd-Ce interfacial interactions ultimately play a role in the overall activity and stability of the catalyst.

In situ methane activation performance of Pd-embedded ceria catalyst prepared by a one-step dry ball-milling method

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.