Advanced catalytic materials are important for the discovery and improvement of processes to produce fuels and valuable chemicals. Among these, ternary metal phosphides are an interesting class of materials expected to have highly tunable catalytic behavior relative to the parent binary phosphides. Single source molecular precursors and solution-based synthesis routes offer significant morphological control over the resulting nanoparticles. Ni-Rh based ternary phosphides were synthesized under controlled conditions to yield tunable structures. Specifically, it was found that Rh preferentially substitutes Ni in the parent Ni2P structure. Through forming a series of Ni2-xRhxP alloy catalysts, it was determined that the preferred location of Rh changes as a function of Rh incorporated. Alternatively, substitutional alloying of Rh with the Ni2P structure could be inhibited by quenching the reaction immediately after reaching 300°C, which instead yieled a Ni2P@Rh2P core-shell structure. Ni1.6Rh0.4P and Ni2P@Rh2P, with the same Rh content, were supported on SiO2 and used in guaiacol hydrodeoxygenation (HDO) and compared to their parent binary metal phosphide catalysts (Ni2P/SiO2 and Rh2P/SiO2). It was observed that the addition of Rh improved the stability of Ni2P under guaiacol HDO reaction conditions. In situ X-ray absorption spectroscopy (XAS) and pair distribution function (PDF) indicated that, although an initial loss of Ni-P bonds was observed after pretreatment in H2 at 350°C, there were no further structural changes when guaiacol was introduced.

Structural tunability in ternary metal phosphides for enhanced catalytic performance in hydrodeoxygenation of biomass-derived model compounds

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.