Theoretical and Experimental Study for Cross-Coupling Aldol Condensation over Mono- and Bimetallic UiO-66 Nanocatalysts

Pazo-Carballo, Cesar; Blanco, Elodie; Camu, Esteban; Leiva, Angel; Hidalgo-Rosa, Yoan; Zarate, Ximena; Dongil, Ana Belen; Schott, Eduardo; Escalona, Nestor


Mono- and bimetallic UiO-66 nanocatalysts were synthesized using the solvothermal synthesis method and evaluated in the aldol condensation reaction of benzaldehyde and acetone in a batch reactor. N2 physisorption, thermogravimetric analysis, temperature-programmed desorption of ammonia, X-ray diffraction, field-emission scanning electron microscopy–energy-dispersive X-ray, X-ray photoelectron spectroscopy, potentiometric titration, and Fourier transform infrared were used to characterize the nanocatalysts. The higher activity exhibited by the Zr/Hf-UiO-66 catalyst could be attributed to the lower orbital energy interaction with benzaldehyde, as shown by density functional theory. A synergetic effect is observed for the bimetallic UiO-66 nanocatalyst between Zr and Hf, obtaining a higher reaction rate than the monometallic nanocatalysts. Meanwhile, this antagonistic effect was shown in the bimetallic catalysts between Zr and Ce, which was less active than the monometallic UiO-66 catalyst due to free COOH generated during the synthesis. Finally, the selectivity results showed that incorporating Hf and Ce on Zr-UiO-66 favors benzalacetone formation by cross-coupling condensation of benzaldehyde and acetone at isoconversion conditions.

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Título de la Revista: ACS Applied Nano Materials
Volumen: 6
Editorial: ACS publiactions
Fecha de publicación: 2023
Página de inicio: 5422
Idioma: Inglés