镍基催化剂:制备及水相催化糠醛加氢脱氧反应性能
Ni-Based Catalysts: Preparation and Catalytic Performance for Aqueous-Phase Hydrodeoxygenation of Furfural
作者单位
张兴华 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640
中国科学院研究生院北京 100049 
王铁军 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640 
马隆龙 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640 
江 婷 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640
中国科学院研究生院北京 100049 
刘琪英 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640 
章 青 中国科学院可再生能源与天然气水合物重点实验室中国科学院广州能源研究所广州 510640 
摘要: 以SiO2-Al2O3、γ-Al2O3为载体采用浸渍法制备了不同负载量的镍基催化剂,以XRD、H2-TPR、NH3-TPD与低温N2吸附等技术对催化剂特性进行了表征,并进行了水相催化糠醛加氢脱氧实验研究以制备以C5为主要成分的生物汽油。重点考察了催化剂的镍负载量、载体种类及反应温度对糠醛转化率、目标产物C5选择性的影响,并对催化剂的重复利用性能和糠醛水相加氢脱氧反应机理进行了探讨。结果表明,Ni/SiO2-Al2O3催化性能明显优于Ni/γ-Al2O3。在140 ℃、氢冷压3.0 MPa的优化反应条件下,14wt% Ni/SiO2-Al2O3催化糠醛反应的转化率为63%,C5选择性高达93%。升高反应温度可以提高糠醛的转化率,但反应产物的选择性降低。催化剂在第3次重复使用时糠醛的转化率明显降低,催化剂表面有明显的残留有机聚合物和积碳,达到25wt%左右。
关键词: 镍催化剂  加氢脱氧  糠醛  生物汽油
基金项目: 
Abstract: The nickel-based catalysts for aqueous-phase hydrodeoxygenation of furfural were prepared by impregnation method using different supports and characterized by XRD, H2-TPR, NH3-TPD and low temperature N2 adsorption The effects of support, nickel loading and reaction temperature on conversion of furfural and selectivity of desired C5 products were studied. The reaction mechanism of furfural aqueous-phase hydrodeoxygenation and the recyclability of catalysts were also discussed. The results showed that the activities of Ni/SiO2-Al2O3 were obviously better than that of the Ni/γ-Al2O3 under the same reaction conditions. The conversion of furfural over 14wt% Ni/SiO2-Al2O3 catalyst was 63% and the selectivity for C5 was as high as 93% under the optimization condition of 140 ℃ and the cold H2 pressure of 3.0 MPa. Conversion of furfural increased with increasing temperature, but the selectivity for desired C5 product decreased with increasing temperature. The conversion of furfural decreased swiftly when the catalyst was re-used for the third time. About 25wt% residual cokes and polymers deposited on the used catalyst surface.
Keywords: Ni catalyst  hydrodeoxygenation  furfural  bio-gasoline
 
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张兴华,王铁军,马隆龙,江 婷,刘琪英,章 青.镍基催化剂:制备及水相催化糠醛加氢脱氧反应性能[J].无机化学学报,2010,26(12):2182-2188.
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