Biomass into Chemicals: Aerobic Oxidation of 5-Hydroxymethyl-2-furfural into 2,5-Furandicarboxylic Acid with Gold Nanoparticle Catalysts
Biomass into Chemicals: Aerobic Oxidation of 5-Hydroxymethyl-2-furfural into 2,5-Furandicarboxylic Acid with Gold Nanoparticle Catalysts
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DOI：
10.1002/cssc.200900137
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发表时间：
2009-01-01
期刊：
影响因子：
8.4
通讯作者：
Corma, Avelino
中科院分区：
文献类型：
--
作者：
Casanova, Onofre;Iborra, Sara;Corma, Avelino
在温和条件（65-130 ℃，10巴空气）下，在水中，用负载在纳米颗粒二氧化铈（Au-CeO 2）和二氧化钛（Au-TiO 2）上的金纳米颗粒将5-羟甲基-2-糠醛选择性地转化为2，5-呋喃二甲酸（99摩尔%产率）;前者更具活性和选择性。建立了反应机理，反应的限速步骤是5-羟甲基-2-呋喃甲酸醇氧化成25-呋喃二甲酸。研究了反应压力、反应温度、底物与催化剂的比例、碱用量等因素对反应的影响，找出了最佳反应条件。通过反应溶液的化学分析和通过确认在热水中过滤除去催化剂后不发生反应来证实不存在金属浸出。通过在两个温度步骤中进行反应，大大减少了底物降解，并且增加了催化剂寿命。
5-hydroxymethyl-2-furfural is selectively converted into 2,5-furandicarboxylic acid (99 mol% yield) in water, under mild conditions (65-130 degrees C, 10 bar air) with gold nanoparticles supported on nanoparticulate ceria (Au-CeO2) and on titania (Au-TiO2); the former being more active and selective. A reaction mechanism is established and the rate-limiting step of the reaction is the alcohol oxidation of 5-hydroxymethyl-2-furancarboxylic acid into 25-furandicarboxylic acid. The effects of pressure, temperature, substrate-to-catalyst ratio, and amount of base are studied to find the most suitable reaction conditions. The absence of metal leaching is verified by chemical analysis of the reaction solution and by confirming that the reaction does not occur after catalyst removal by filtration in hot water. Substrate degradation is strongly diminished and the catalyst life increased by performing the reaction in two temperature steps.