Atomic Layer Deposition of the Geometry Separated Lewis and Brønsted Acid Sites for Cascade Glucose Conversion.

Abstract

Solid acid catalysts with bi-acidity are promising as workhouse catalysts in biorefining to produce high-quality chemicals and fuels. Herein, we report a new strategy to develop bi-acidic cascade catalysts by separating both acid sites in geometry via the atomic layer deposition (ALD) of Lewis acidic alumina on Brønsted acidic supports. Visualized by transmission electron microscopy and electron energy loss spectroscopy mapping, the ALD-deposited alumina forms a conformal alumina domain with a thickness of around 3 nm on the outermost surface of mesoporous silica-alumina. Solid state nuclear magnetic resonance investigation shows that the dominant Lewis acid sites distribute on the outermost surface, whereas intrinsic Brønsted acid sites locate inside the nanopores within the silica-rich substrate. In comparison to other bi-acidic solid catalyst counterparts, the special geometric distance of Lewis and Brønsted acid sites minimized the synergetic effect, leading to a cascade reaction environment. For cascade glucose conversion, the designed ALD catalyst showed a highly enhanced catalytic performance.