Mechanism of transfer hydrogenation of carbonyl compounds by zirconium and hafnium-containing metal-organic frameworks
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Author list: Rahaman, Mohammad Shahinur; Tulaphol, Sarttrawut; Hossain, Md. Anwar; Mulvehill, Matthew C.; Spurgeon, Joshua M.; Maihom, Thana; Sathitsuksanoh, Noppadon
Publisher: Elsevier
Publication year: 2022
Volume number: 522
ISSN: 2468-8231
Languages: English-Great Britain (EN-GB)
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Abstract
Liquid phase catalytic hydrogenation is essential to produce platform chemicals from biomass-derived carbonyl compounds. Carbonyl compounds can be upgraded to corresponding alcohols by catalytic transfer hydrogenation using hydrogen-donor solvents and mild reaction conditions. The challenge in transfer hydrogenation is the development of selective, active, and reusable catalysts. Here we show the chemical pathway of transfer hydrogenation of benzaldehyde by Hf- and Zr-containing MOF-808 and UiO-66 catalysts. MOF-808(Hf) was the most selective catalyst with 95% selectivity to benzyl alcohol at 99% conversion. Furthermore, the quantum calculations revealed that the transfer hydrogenation by MOF-808(Hf) proceeded by Meerwein–Ponndorf–Verley (MPV) reduction, which resulted in high selectivity and conversion. These findings of the effects of metal and acid sites of these MOFs enable maximizing the selectivity for transfer hydrogenation. Moreover, understanding these effects provide opportunities for these MOFs in other biomass conversion reactions. © 2022 Elsevier B.V.
Keywords
Carbonyl, Meerwein–Ponndorf–Verley, Transfer hydrogenation
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