The aerobic oxidation of 5-hydroxymethylfurfural (HMF), a key platform compound in cellulose transformation, into 2,5-furandicarboxylic acid (FDCA), a promising renewable alternative to petroleum-derived terephthalic acid, is one of the most attractive reactions for establishing biomass-based sustainable chemical processes. Supported Au catalysts have shown encouraging performance for this reaction, but the need of an excess amount of base additives makes the process less green and less cost-effective. Here, we report a stable and efficient carbon nanotube (CNT)-supported Au−Pd alloy catalyst for the aerobic oxidation of HMF to FDCA in water without any bases. The functionalization of CNT surfaces is crucial for FDCA formation. We have clarified that the CNT containing more carbonyl/ quinone and less carboxyl groups favors FDCA formation by enhancing the adsorption of the reactant and reaction intermediates. Significant synergistic effects exist between Au and Pd in the alloy for the base-free oxidation of HMF to FDCA through three tandem steps. The present work provides understanding of the support-enhanced adsorption effect and the alloying effect for supported Au-based bimetallic catalysts, and this knowledge may help develop efficient catalysts for the aerobic oxidation of relatively complicated organic compounds with different functional groups in water.
The direct transformation of cellulose, which is the main component of lignocellulosic biomass, into building-block chemicals is the key to establishing biomass-based sustainable chemical processes. Only limited successes have been achieved for such transformations under mild conditions. Here we report the simple and efficient chemocatalytic conversion of cellulose in water in the presence of dilute lead(II) ions, into lactic acid, which is a high-value chemical used for the production of fine chemicals and biodegradable plastics. The lactic acid yield from microcrystalline cellulose and several lignocellulose-based raw biomasses is 460% at 463 K. Both theoretical and experimental studies suggest that lead(II) in combination with water catalyses a series of cascading steps for lactic acid formation, including the isomerization of glucose formed via the hydrolysis of cellulose into fructose, the selective cleavage of the C3-C4 bond of fructose to trioses and the selective conversion of trioses into lactic acid.
Metal and metal oxide catalysts for non-oxidative ethane/propane dehydrogenation are outlined with respect to catalyst synthesis, structure–property relationship and catalytic mechanism.
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