Catalyst studies on the ring opening of tetrahydrofuran-dimethanol to 1,2,6-hexanetriol

Teddy Buntara, Ignacio Melián-Cabrera, Qiaohua Tan, José L.G. Fierro, Matthew Neurock, Johannes G. De Vries, Hero J. Heeres

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52 Scopus citations

Abstract

The metal catalyzed hydrogenolysis of the biomass-derived THF-dimethanol to 1,2,6-hexanetriol using heterogeneous catalysts was investigated. Bimetallic Rh-Re catalysts (4 wt% Rh and a Re/Rh (mol. ratio of 0.5) on a silica support gave the best performance and 1,2,6-hexanetriol was obtained in 84% selectivity at 31% conversion (120 C, 80 bar, 4 h); the selectivity reaches a maximum of 92% at 80 C. The product distribution at prolonged reaction times or higher temperatures or both shows the formation of diols and mono-alcohols, indicating that the 1,2,6-hexanetriol is prone to subsequent hydrodeoxygenation reactions. Different silica supports were investigated and optimal results were obtained with an amorphous silica featuring an intermediate surface area and an average mesopore size of about 6 nm. TPR and XPS surface analysis support the presence of mixed Rh and Re particles. The redox Reδ+/ReTotal surface ratio correlates with the conversion in a volcano type dependency. Both gas phase as well as Rh200Re1OH cluster DFT calculations support an acid-metal bifunctional mechanism and explain the products distribution.

Original languageEnglish (US)
Pages (from-to)106-116
Number of pages11
JournalCatalysis Today
Volume210
DOIs
StatePublished - Jul 1 2013

Keywords

  • 1,2,6-Hexanetriol
  • DFT calculations
  • Hydrogenolysis
  • Rh-ReO /SiO catalysts
  • Ring opening
  • THF-dimethanol

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    Buntara, T., Melián-Cabrera, I., Tan, Q., Fierro, J. L. G., Neurock, M., De Vries, J. G., & Heeres, H. J. (2013). Catalyst studies on the ring opening of tetrahydrofuran-dimethanol to 1,2,6-hexanetriol. Catalysis Today, 210, 106-116. https://doi.org/10.1016/j.cattod.2013.04.012