Synergistic Catalytic Effects of Alloys of Noble Metal Nanoparticles Supported on Two Different Supports: Crystalline Zeolite Sn-Beta and Carbon Nanotubes for Glycerol Conversion to Methyl Lactate

Abstract

Two multifunctional catalytic systems comprising Sn-based/doped crystalline zeolite Beta were synthesized, and they were employed as heterogeneous catalysts in the selective conversion of glycerol to methyl lactate. The first catalytic system, named Au-Pd-Sn-deAl-7.2-Beta-DP, was created through the post-synthesis dealumination of the parent zeolite Beta (Si/Al = 10) using 7.2 M HNO3. Subsequently, it was grafted with 27 mmol of SnCl4, resulting in Sn-deAl-7.2-Beta. Following this, Au and Pd nanoparticles were supported on this catalyst using the deposition–precipitation (DP) method. The second catalytic system was a physical mixture of Au and Pd nanoparticles supported on functionalized carbon nanotubes (Au-Pd-F-CNTs) and Sn-containing zeolite Beta (Sn-deAl-7.2-Beta). Both catalytic systems were employed in glycerol partial oxidation to methyl lactate under the following conditions: 140 °C for 4.5 h under an air pressure of 30 bar. The Au-Pd-Sn-deAl-7.2-Beta-DP catalytic system demonstrated 34% conversion of glycerol with a 76% selectivity for methyl lactate. In contrast, the physical mixture of Au-Pd-F-CNTs and Sn-deAl-7.2-Beta exhibited higher activity, achieving 58% glycerol conversion and a nearly identical selectivity for methyl lactate (77%). The catalytic results and catalyst structure were further analyzed using various characterization techniques, such as X-ray diffraction (XRD), N2 physisorption, scanning electron microscopy (SEM), X-ray fluorescence (XRF), transmission electron microscopy (TEM), UV-vis spectroscopy, and pyridine Fourier transform infrared (FTIR). These analyses emphasized the significance of adjusting the quantity of active sites, particle size, and active sites proximity under the chosen reaction conditions.