Simultaneous Mesoporosity Generation and Lewis Acidity Enhancement in Zr-Based Metallosilicalite for Promoting the Conversion of Ethanol-Acetaldehyde to 1,3-Butadiene

Graphical Dissolution-recrystallization strategy benefits both the porosity and Lewis acidity in Zr- β zeolite, which promotes catalytic conversion of ethanol-acetaldehyde. Zr based metallosilicalites, especially Zr- ß , is promising catalyst for the conversion of ethanol to 1,3-butadiene, which is considered to be a sustainable alternative to petroleum steam cracking. However it is suffering from deactivation derived from coking and unsatisfied catalytic activity derived from deficient Lewis acidity. For these issues, a dissolution-recrystallization process through tetraethyl ammonium hydroxide treatment (TEAOH) for enhancing porosity and Lewis acidity of Zr- ß zeolite was developed in this study. A balance of dissolution and recrystallization existed in this process, which was produced by OH − etching and templating of TEA + ions, creating additional mesoporosity. Zirconium active sites maintained tetrahedral coordination, while the Lewis acidity was enhanced by creating higher proportion open sites in framework. The recrystallized Zr- ß exhibited higher catalytic activity and stability in the conversion of ethanol-acetaldehyde to butadiene due to the compromise of microporosity and mesoporosity, as well as the appropriate enhancement of Lewis acidity.