Investigations on the role of support and synthesis procedure for the Rux–Cuy/CNT‐catalysed hydrogenolysis of glycerol to 1,2‐propanediol

Tailoring support effects plays an important role for controlling activity and selectivity in heterogeneously catalyzed gas–liquid reactions. Sophisticated carbon supports like single‐ and multiwall carbon nanotubes (CNTs) as well as in house produced Globugraphite were used for the synthesis of bimetallic Ru–Cu catalysts, which were tested in a multibatch reactor setup for the chemical hydrogenolysis of glycerol to 1,2‐propanediol (1,2‐PDO) in aqueous solution. In‐depth characterization using multiple tools like inductively coupled plasma optical emission spectrometry, CHNS‐O analysis, N₂‐physisorption, scanning electron microscopy, transmission electron microscopy, energy‐dispersive X‐ray spectroscopy, powder X‐ray diffraction, H₂‐temperature programmed reduction, laser diffraction, and point of zero charge measurements revealed the dominating effects that the various carbon supports exert on the catalytic performance. The best‐performing catalyst synthesized by wetness impregnation consisted of Ru–Cu₃ nanoparticles (NPs) from mixed RuCl₃ and Cu(NO₃)₂ precursors dispersed on multiwall CNT Baytubes with a productivity of p = 12.74 g₁,₂‐PDO gactive metal ⁻¹ h⁻¹ . Its superior activity combined with high 1,2‐PDO selectivity (S= 75%) can be explained both by the nature of the highly dispersed Ru and Cu NPs showing the lowest reduction peak temperature on entangled tubes of CNT agglomerates demonstrating a high mesopore volume for optimal reactant accessibility and the highest specific surface area of all investigated materials. This lays the foundation for implementing this highly active and selective catalyst in a future SMART reactor for glycerol valorisation.

Content

Subjects

1,2-propanediol

carbon nanotubes

glycerol hydrogenolysis

heterogeneous catalysis

structure-activity-selectivity-relationship

DDC Class

660.2: Chemical Engineering

Funding References

Funding(s)

SFB 1615 - SMARTe Reaktoren für die Verfahrenstechnik der Zukunft