Abstract
Tetrahydropyran (THP) represents an O-containing hetero-cyclic compound that can be used as a promising solvent or monomer for polymer synthesis. In this work, Cu–ZnO/Al2O3 catalysts have been prepared by a facile precipitation–extrusion method and used for the synthesis of THP through gaseous-phase hydrogenolysis of tetrahydrofurfuryl alcohol (THFA). The effect of the molar ratio of Cu/Zn/Al, reaction temperature, and hydrogen pressure was investigated. An 89.4% selectivity of THP was achieved at 270 °C and 1.0 MPa H2. Meanwhile, the optimum molar ratio of Cu/Zn/Al was determined to be 4:1:10. The Cu–ZnO/Al2O3 catalyst exhibited high catalytic activity and stability for 205 h on-stream. A possible reaction mechanism involving several consecutive reactions was proposed: THFA was firstly rearranged to 2-hydroxytetrahydropyran (2-HTHP), followed by the dehydration of 2-HTHP to 3,4-2H-dihydropyran (DHP) over acid sites; finally, the DHP was hydrogenated to THP. The synergy of acid sites and metal sites of Cu–ZnO/Al2O3 played an important role during the production of THP.
Highlights
Catalytic upgrading of biomass-derived furfural or its derivatives to value-added chemicals has received great attention in recent years [1,2,3]
The porosity and pore-size distribution of the calcined Cu–ZnO/Al2 O3 extrudate catalysts were determined by N2 adsorption–desorption
The γ-Al2 O3 exhibited a 12 nm mean diameter (Figure S1)
Summary
Catalytic upgrading of biomass-derived furfural or its derivatives to value-added chemicals has received great attention in recent years [1,2,3]. Tetrahyrofurfuryl alcohol (THFA) can be obtained through hydrogenation of furfural at a very high yield [12], and from which various useful chemicals, such as 1,5-pentadiol (15PDO) [13,14,15,16,17,18,19,20,21,22,23,24,25], 3,4-2H-dihydropyran (DHP) [26,27,28], and 4-penten-1-ol can be produced [29,30]. The catalytic conversion of furanics has been extensively studied over noble metal catalysts. Among non-noble metals, copper-based catalysts were widely used in hydrogenation and hydrogenolysis reactions due to their good catalytic performance and low cost. The current work was beneficial to develop the downstreams of TFHA over non-noble catalysts
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