Cascade Reactions for the Continuous and Selective
Production of Isobutene from Bioderived Acetic Acid Over Zinc-Zirconia
Catalysts
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Abstract
Bio-oil
(obtained from biomass fast pyrolysis) contains a high
concentration of acetic acid, which causes problems related to its
storage and handling. Acetic acid was upgraded directly to isobutene
over a Zn<sub><i>x</i></sub>Zr<sub><i>y</i></sub>O<sub><i>z</i></sub> binary metal oxide. The reaction proceeds
via a three-step cascade involving ketonization, aldol condensation,
and C–C hydrolytic bond cleavage reactions, which was corroborated
by isotopic labeling studies. Separately, ZnO and ZrO<sub>2</sub> are
incapable of producing isobutene from either acetic acid or acetone.
In contrast, under optimal conditions, a Zn<sub>2</sub>Zr<sub>8</sub>O<sub><i>z</i></sub> catalyst generates a ca. 50% isobutene
yield, which corresponds to 75% of the theoretical maximum. Spectroscopic
investigations revealed that a balanced concentration of acid and
base sites is required to maximize isobutene yields