期刊
CHEMICAL SCIENCE
卷 6, 期 8, 页码 4940-4945出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5sc00854a
关键词
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资金
- EPSRC [EP/G007594/4]
- Royal Society
- Diamond Light Source [SP8688]
- Engineering and Physical Sciences Research Council [EP/G007594/4, EP/K014676/1] Funding Source: researchfish
- EPSRC [EP/K014676/1, EP/G007594/4] Funding Source: UKRI
Nanoparticulate gold has emerged as a promising catalyst for diverse mild and efficient selective aerobic oxidations. However, the mechanism of such atom-economical transformations, and synergy with functional supports, remains poorly understood. Alkali-free Mg-Al hydrotalcites are excellent solid base catalysts for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furan dicarboxylic acid (FDCA), but only in concert with high concentrations of metallic gold nanoparticles. In the absence of soluble base, competitive adsorption between strongly-bound HMF and reactively-formed oxidation intermediates site-blocks gold. Aqueous NaOH dramatically promotes solution phase HMF activation, liberating free gold sites able to activate the alcohol function within the metastable 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) reactive intermediate. Synergistic effects between moderate strength base sites within alkali-free hydrotalcites and high gold surface concentrations can afford highly selective and entirely heterogeneous catalysts for aqueous phase aldehyde and alcohol cascade oxidations pertinent to biomass transformation.
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