Accessible Acid-Site Retention in Solvent-Free Acetone Aromatization over Mesoporous Amorphous Silica-Alumina
Abstract
Conversion of bio-based acetone to mesitylene via catalytic reactions is an effective pathway that can transform biocompatible ketones directly to sustainable alkyl aromatics; however, there are many processes involved in acetone transformation to mesitylene, namely, C-C coupling, dehydration, cyclization, aromatication, and carbonaceous deposition growth, which should be optimized for the reaction to take place. Solvent-free continuous conversion of acetone to mesitylene over commercially available amorphous silica-alumina catalysts depends greatly on the presence of active acid centers throughout operation time. The composition of Siralox 30 includes 30 wt\% SiO$_2$, a mesoporous structure, a specific BET surface area of 199 m$^2$ g$^{-1}$, a total pore volume of 0.59 cm$^3$ g$^{-1}$, average pore diameter of 12.3 nm, and acidity of 0.30 mmol NH$_3$ g$^{-1}$. Acetone conversion rises from approximately 17\% to 63\% between 200 $^\circ$C and 300 $^\circ$C at 75 bar, with mesitylene selectivity having its maximum near 260 $^\circ$C. Mesitylene yield of approximately 10.1\% can be obtained using Siralox 30 at 260 $^\circ$C and $W/F = 12.5$ g$_{cat}$ h mol$^{-1}$, remaining stable for over 50 hours on stream. On the contrary, spent Siralox 30 keeps virtually all its mesoporous volume, while HY-5 demonstrates considerable reduction in microporous surface area and about 20 wt\% weight loss. Durable acetone aromatization therefore depends on a retained Br{\o}nsted-Lewis acid environment in open mesopores rather than on maximum fresh surface area or maximum acid-site concentration.