Tandem Upgrading of Bio-Furans to Benzene, Toluene, and p-xylene by Pt1Sn1 Intermetallic Coupling Ordered Mesoporous SnO2 Catalyst.

Abstract

Benzene, toluene, and p-xylene (BTpX) are among the most important commodity chemicals, but their productions still heavily rely on fossil resources and thus pose serious environmental burdens and energy crisis. Herein, the tandem upgrading of bio-furans is reported to high-yield BTpX by rationally constructing a versatile Pt1Sn1 intermetallic coupling ordered-mesoporous SnO2 (OM-SnO2) catalyst. It is shown that with increasing reduction temperature from 200 to 350°C, Pt nanoparticles (NPs) are first formed on OM-SnO2, then converted to Pt3Sn1 intermetallic nanoparticles (iNPs), and finally to Pt1Sn1 iNPs with a gradually-thickened SnO2 overlayer. Impressively, the Pt1Sn1 iNPs and defect-rich OM-SnO2 in the optimized Pt@OM-SnO2 can serve as the highly-active species for the hydrogenolysis of 5-hydroxymethylfuran to 2,5-dimethylfuran and the aromatization of 2,5-dimethylfuran with acrylic acid to p-xylene, affording the highest yields of 99.1% and 96.1%, respectively. More importantly, it can perfectly realize the tandem upgrading of furan, furfural and 5-hydroxymethylfuran to benzene, toluene and p-xylene with high yields of 94.6%, 94.2% and 95.2%, respectively, representing a new tandem catalytic system to realize the high-yield BTpX productions from their corresponding bio-furans. This catalyst also shows good recyclability and excellent scalability, which together with its superior activity/selectivity suggest a high potential for sustainable BTpX productions.