Tuning Acid-Base Properties Using Mg-Al Oxide Atomic Layer Deposition.

Abstract

Atomic layer deposition (ALD) was used to coat γ-Al2O3 particles with oxide films of varying Mg/Al atomic ratios, which resulted in systematic variation of the acid and base site areal densities. Variation of Mg/Al also affected morphological features such as crystalline phase, pore size distribution, and base site proximity. Areal base site density increased with increasing Mg content, while acid site density went through a maximum with a similar number of Mg and Al atoms in the coating. This behavior leads to nonlinearity in the relationship between Mg/Al and acid/base site ratio. The physical and chemical properties were elucidated using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 physisorption, and CO2 and NH3 temperature-programmed desorption (TPD). Fluorescence emission spectroscopy of samples grafted with 1-pyrenebutyric acid (PBA) was used for analysis of base site proximity. The degree of base site clustering was correlated to acid site density. Catalytic activity in the self-condensation of acetone was dependent on sample base site density and independent of acid site density.