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Title

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

AuthorsBuntara, Teddy; Melián-Cabrera, Ignacio; Tan, Qiaohua; Fierro, José Luis G.; Neurock, Matthew; Vries, Johannes G. de; Heeres, Hero J.
KeywordsHydrogenolysis
Ring opening
DFT calculations
1,2,6-Hexanetriol
Rh–ReOx/SiO2 catalysts
THF–dimethanol
Issue Date1-Jul-2013
PublisherElsevier
CitationCatalysis Today 210: 106-116 (2013)
AbstractThe 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.
Publisher version (URL)https://doi.org/10.1016/j.cattod.2013.04.012
URIhttp://hdl.handle.net/10261/181987
DOI10.1016/j.cattod.2013.04.012
ISSN0920-5861
Appears in Collections:(ICP) Artículos
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