期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 33, 页码 11127-11136出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c02998
关键词
Pd@UiO-SO3H; Aromatic aldehydes; Adsorption configuration; C=O hydrogenation; C-O hydrogenolysis
资金
- National Natural Science Foundation of China [21878138, 91200157, 21706112]
- Postdoctoral Science Foundation of China [2017M622104, 2018T110660]
The study introduces metal-organic framework (MOF) encapsulating metal-acid interfaces as catalysts for C-O hydrogenolysis of biomass-derived aromatic aldehydes. These catalysts show higher activity and selectivity compared to traditional supported catalysts, with Pd@UiO-SO3H exhibiting the best performance.
Developing an efficient and selective catalyst for C-O hydrogenolysis of biomass-derived aromatic aldehydes, such as 5-methylfurfural (MF), 5-hydroxymethylfurfural (HMF), and vanillin (VA), is highly significant for the synthesis of biofuel and fine chemicals. Herein, metal-organic framework (MOF)-encapsulating metal-acid interfaces (Pd@UiO-CH2SO3H, Pd@UiO-PhSO3H) were first reported. Compared with traditionally supported catalysts (Pd/UiO-SO3H, Pd/UiO-NH2), Pd-acid-interface-encapsulated MOFs show much higher activity and selectivity for MF to 2,5-dimethylfuran (DMF), HMF to DMF, and VA to 2-methoxy-4-methylphenol (MMP) reactions. In particular, Pd@UiO-SO3H shows the best catalytic performance with 89.0 and 86.0% DMF yield from MF and HMF and a 99.4% MMP yield from VA based on its suitable hydrophilicity, high hydrogen activation ability, and abundant Pd-SO3H interface active sites. According to the catalytic performance of Pd/UiO-NH2 and the results of an ATR-IR test, the acidic sites on the Pd-acid interface can accelerate the activation of the hydroxyl group for these hydrogenolysis reactions. This work provides an effective design strategy for the preparation of MOF-encapsulating metal-acid interfaces and shows the powerful synergistic effect of hydrogenation and acid catalysis.
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