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Efficient Transfer Hydrogenation of Furfural via F Doping in Mesoporous ZrO2
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DOI:10.1039/D6NR01841F.png)
Abstract
En 中文
Designing highly active and robust catalysts for transfer hydrogenation of biomass-derived aldehydes remains challenging. Here; we report a F-modified mesoporous ZrO2 (F-mZrO2) obtained through pyrolysis of F-mUiO-66 precursor; offering a simple and scalable strategy to construct mesoporous oxides with tunable surface chemistry. The incorporation of fluorine species electronically modulates neighboring Zr centers; significantly enhancing Lewis acidity and carbonyl-group polarization. Benefiting from this electronic tuning; F-mZrO2 achieves 97.8% yield for furfural (FFA) transfer hydrogenation to furfuryl alcohol (FOL) at 170 °C using isopropanol (IPA). Mechanistic studies with isotopically labeled IPA confirm a classical MPV hydride-transfer pathway. Density functional theory (DFT) calculations further reveal that F modification regulates the electronic structure of Zr sites and increased acidity. Furthermore; the catalyst exhibits excellent stability over multiple cycles with rubost structure. This work demonstrates a generalizable route to tailor the electronic structures of mesoporous oxides via MOF-derived fluorine incorporation; enabling efficient catalysis in biomass upgrading.
Journal
IF:
5.1
Papers:
3.0W
Citations:
11.6W
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