Elucidation of the Catalytic Pathway for the Direct Conversion of Furfuryl Alcohol into γ-Valerolactone over Al2O3-SiO2 Catalysts

Pichaya Chuangpusri; Sasiradee Jantasee; Patcharaporn Weerachawanasak; Weerachon Tolek; Chawalit Ngamcharussrivichai; Duangamol N Tungasmita; Noppadon Sathitsuksanoh; Joongjai Panpranot

doi:10.1021/acsomega.3c05412

Elucidation of the Catalytic Pathway for the Direct Conversion of Furfuryl Alcohol into γ-Valerolactone over Al₂O₃-SiO₂ Catalysts

ACS Omega. 2023 Dec 1;8(49):46560-46568. doi: 10.1021/acsomega.3c05412. eCollection 2023 Dec 12.

Authors

Pichaya Chuangpusri¹, Sasiradee Jantasee², Patcharaporn Weerachawanasak³, Weerachon Tolek¹, Chawalit Ngamcharussrivichai⁴, Duangamol N Tungasmita⁵, Noppadon Sathitsuksanoh⁶, Joongjai Panpranot^{1

7}

Affiliations

¹ Center of Excellence on Catalysis and Catalytic Reaction Engineering, Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok 10330, Thailand.
² Department of Chemical and Materials Engineering, Faculty of Engineering, Rajamangala University of Technology Thanyaburi, Pathum, Thani 12110, Thailand.
³ Industrial Chemistry, Department of Chemistry, Faculty of Science, King Mongkut's Institute of Technology Ladkrabang Bangkok 10520, Thailand.
⁴ Department of Chemical Technology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand.
⁵ Department of Chemistry, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand.
⁶ Department of Chemical Engineering, University of Louisville, 216 Eastern Parkway, Louisville, Kentucky 40292, United States.
⁷ Bio-Circular-Green-economy Technology & Engineering Center, BCGeTEC, Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok 10330, Thailand.

Abstract

The one-pot conversion of furfuryl alcohol (FA) into GVL was investigated over the sol-gel-synthesized Al₂O₃-SiO₂ (AlSi) catalysts with various Al₂O₃ loadings (0.2-10 wt %) and commercial zeolites including MFI-1, H-ZSM5, H-beta, and HY-15 in a batch reactor under mild reaction conditions (130 °C, 1 bar N₂, and 15-120 min). The reaction pathways depend largely on the acid properties of the catalysts, especially the types of Bronsted (B) and Lewis (L) acid sites. A tandem alcoholysis/hydrogenation/cyclization sequence is dominant on the AlSi catalysts (Al ≥ 4%) and all the zeolites except MFI-1, resulting in complete conversion of FA and GVL with an yield 64-75% with IPL as the major side-product, regardless of the differences in their B/L ratios 0.06-1.35. In the absence of B acid sites (i.e., 0.2% AlSi and MFI-1 catalysts), FA could be straightforwardly converted into GVL on the weak Lewis acid sites from the isolated silanol groups using 2-propanol as a hydrogen source. The AlSi catalysts are promising tunable catalysts for FA conversion with good recyclability.