4.8 Article

Correlating the Synthesis, Structure, and Catalytic Performance of Pt-Re/TiO2 for the Aqueous-Phase Hydrogenation of Carboxylic Acid Derivatives

Journal

ACS CATALYSIS
Volume 11, Issue 9, Pages 5119-5134

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c05612

Keywords

rhenium; hydrogenation; succinic acid; structure-activity; bimetallic catalyst; bifunctional; catalyst preparation

Funding

  1. German Federal Ministry of Education and Research (BMBF) [FKZ IBO-03 031B0249, 031B0487 A]
  2. German Chemical Industry Fund (Fonds der chemischen Industrie, FCI)

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This study extensively compares the synthesis protocols and materials of Pt-Re bimetallic catalysts, revealing common features like Pt-0 nanoparticles and partially reduced Re species. Differences in active site numbers and Re reduction extent affect catalytic performance, with the optimal catalyst outperforming a previous benchmark in the reduction of N-(2-hydroxyethyl)succinimide.
Pt-Re bimetallic catalysts have many applications, ranging from catalytic reforming to the reduction of carboxylic acid derivatives. However, the exact role of Re in these systems has remained a matter of discussion, partly due to the plethora of suggested synthesis protocols and analysis conditions. This study presents an extensive comparison of such literature protocols and the resulting materials. In detail, characterization by N-2 physisorption, X-ray diffraction, temperature-programmed reduction, CO pulse chemisorption, Fourier-transform infrared spectroscopy of adsorbed CO, scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, and in situ X-ray photoelectron spectroscopy is combined with catalytic testing to yield synthesis-structure-activity correlations. Accordingly, the investigated catalysts share common features, such as Pt-0 nanoparticles partially reduced Re species (ReOx-y). The remaining rhenium oxide is spread over the TiO2 support and enhances Pt dispersion in sequential impregnation protocols. While differences in the number of active sites (Pt-0 /ReOx-y) mostly explain catalytic results, small variations in the extent of Re reduction and site composition cause additional modulations. The optimal bimetallic catalyst outperforms Ru/C (previous benchmark) in the reduction of N-(2-hydroxyethyl)succinimide, an important step in the production of a bio-based polyvinylpyrrolidone polymer.

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