镍锆纳米氧化物,高效催化生物质合成γ戊内酯GVL
γ戊内酯(GVL)已被确定为一种绿色的和可再生的溶剂,用以提高生物质转化和各种有机反应。它可作为液体燃料,香料和食物的添加剂。更重要的是,GVL可以用来合成汽油和柴油燃料(例如,C8-C18烷烃和2-甲基四氢呋喃)和高价值的化学物质(如1,4-戊二醇,甲基戊酸,离子液体和聚合物)。

生物能源组与贵州大学联合培养的博士生李虎在导师杨松教授和方真研究员的指导下,用共沉淀方法合成了一系列的混合氧化物纳米颗粒。研究发现,在不使用外部氢源的情况下,还原后的磁性镍 – 氧化锆纳米颗粒可直接高效转化生物质衍生物(如乙酰丙酸乙酯,果糖,葡萄糖,纤维二糖和羧甲基纤维素)为GVL。用磁性纳米颗粒Zr5Ni5(< 20纳米)作为催化剂,在200℃下反应3小时,最大GVL产率为95.2%。这些纳米催化剂具备酸碱二重性,对GVL的合成具有协同作用。 此外,磁性Zr5Ni5纳米颗粒可很方便地由磁铁回收,可进行至少五次的重复利用。

近日,文章“H Li, Zhen Fang*, S Yang, Direct Catalytic Transformation of Biomass Derivatives into Biofuel Component γ-Valerolactone with Magnetic NiZr Nanoparticles, 81, 135-142, (2016).” 在国际期刊《ChemPlusChem》发表:  http://onlinelibrary.wiley.com/doi/10.1002/cplu.201500492/abstract
Converting biomass derivatives into biofuel component γ-valerolactone (GVL) with magnetic NiZr nanoparticles

γ-valerolactone (GVL) has been identified as a green and renewable solvent to improve the performance of biomass conversion and various organic reactions, and as an additive suitable for liquid fuels, perfumes and food. More importantly, GVL is able to be employed as a precursor to produce gasoline and diesel fuels (e.g., C8−C18 alkanes and 2-methyltetrahydrofurane) and valuable chemicals such as 1,4-pentanediol and methyl pentenoate, as well as ionic liquids and polymers.

Mr. Hu Li, a PhD student, co-supervised by Prof. Song Yang (Guizhou University) and Prof. Zhen FANG (Biomass Group, Xishuangbanna Tropical Botanical Garden, CAS) successfully synthesized g-valerolactone.

In their work, a series of mixed oxide nanoparticles were prepared by coprecipitation method and characterized by many techniques. NiZr oxide catalysts and their partially reduced magnetic counterparts were highly efficient in direct transformation of biomass derivatives including ethyl levulinate, fructose, glucose, cellobiose and carboxymethyl cellulose into GVL without using external hydrogen source, producing a maximum GVL yield of 95.2% at 200 ºC for 3 h with H2 reduced magnetic Zr5Ni5 nanoparticles (< 20 nm). Acid-base bifunctionality of these nanocatalysts is found to play a synergic role in synthesis of GVL in alcohols, while appropriate control of Ni/Zr molar ratio is able to improve the selectivity towards GVL (~98%), along with high formation rates (up to 54.9 mmol g−1 h−1). Moreover, the magnetic Zr5Ni5 nanoparticles were conveniently recovered by a magnet for five recycles with almost constant activity.

The study entitled “H Li, Zhen Fang*, S Yang, Direct Catalytic Transformation of Biomass Derivatives into Biofuel Component γ-Valerolactone with Magnetic NiZr Nanoparticles, 81, 135-142, (2016).” has been published in ChemPlusChem:  http://onlinelibrary.wiley.com/doi/10.1002/cplu.201500492/abstract

 Presentation1

 Magnetic nanoparticles: Acid-base bifunctional NiZr nanocatalysts with strong magnetism show high activity and reusability in transformation of biomass derivatives including EL, fructose, glucose, cellobiose and carboxymethyl cellulose into γ-valerolactone (GVL) with 95.2% yield and 98% selectivity.

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