Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 3, 2025

High-entropy metal-organic frameworks (HE-MOFs) hold promise as versatile materials, yet current rare examples are confined to low-valence elements in the fourth period, constraining their design and optimization for diverse applications. Here, a novel high-entropy, defect-rich small-sized (32 nm) UiO-66 (ZrHfCeSnTi HE-UiO-66) has been synthesized first time, leveraging increased configurational entropy achieve high tolerance doping with metal ions. The lattice distortion of HE-UiO-66 induces exposure nodes create coordination unsaturated sites concentration 322.4 μmol/g, which increases abundance Lewis acid-base sites, thereby achieving significant improvement performance catalytic transfer hydrogenation (CTH) reaction. Systematic investigation manifests that special electronic structure enhances interaction bonding substrate molecules reduces energy barrier hydrogen process. Our approach offers new strategy constructing MOFs. offer potential but existing largely limited restricting various defect-rich, framework enhance hydrogenation.

Language: Английский

A High-Activity Composite Catalyst via Sol-Gel-Assisted Self-Propagating High-Temperature Synthesis for Catalytic Transfer Hydrogenation

Applied Catalysis A General, Journal Year: 2025, Volume and Issue: unknown, P. 120164 - 120164

Published: Feb. 1, 2025

Language: Английский

Zirconium Phosphate-Pillared Zeolite MCM-36 for Green Production of γ-Valerolactone from Levulinic Acid via Catalytic Transfer Hydrogenation

Molecules, Journal Year: 2024, Volume and Issue: 29(16), P. 3779 - 3779

Published: Aug. 9, 2024

γ-valerolactone (GVL), derived from biomass, is a crucial platform compound for biofuel synthesis and various industrial applications. Current methods synthesizing GVL involve expensive catalysts high-pressure hydrogen, prompting the search greener alternatives. This study focuses on novel zirconium phosphate (ZrP)-pillared zeolite MCM-36 derivative catalyst converting levulinic acid (LA) to using alcohol as hydrogen source. The incorporation of ZrP significantly contributes mesoporosity greatly enhances acidity catalysts. Additionally, we employed 31P MAS NMR comprehensively investigate influence phosphorus species both catalytic conversion LA GVL. By adjusting Zr-to-P ratios, synthesized with enhanced acidity, achieving high selectivity exhibited recyclability, showing only minor deactivation over course five cycles. Furthermore, was successfully applied one-pot furfural GVL, showcasing its versatility in biomass conversion. highlights potential MCM-ZrP1 sustainable offers insights future research renewable energy technologies.

Language: Английский