铝负载铜镍催化剂对糠醛和5-羟甲基糠醛加氢的协同作用研究

Sanjay Srivastava, G.C. Jadeja, Jigisha Parikh
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引用次数: 109

摘要

采用XRD、n2 -吸附、TEM、H2-TPR、NH3-TPD、XANES/EXAFS和CHNS等多种表征技术,对浸渍法制备的铝负载铜镍催化剂的结构进行了研究。一系列表征表明,由于镍和氧化铜颗粒之间的强相互作用,随着α -Al2O3上镍负载的增加,铜的分散性增加。这也导致在镍和铜的最高负载(即Cu/Ni = 1)下,煅烧催化剂中形成混合铜镍氧化物。在催化活性方面,单金属Cu/ α -Al2O3和Ni/ α -Al2O3分别对糠醛和5-羟甲基糠醛加氢成2-甲基呋喃(2- mf)和2,5 -二甲基呋喃(DMF)的活性和选择性较低。然而,随着镍负载的增加,Cu/Ni -Al2O3的活性和选择性都急剧增加,Cu-Ni/ Ni -Al2O3 (Cu/Ni = 1)的催化活性最高。此外,Cu/Ni比和温度的组合对产物分布有重要影响,如在糠醛加氢的情况下,在较低的温度下,糠醇(FOL)是主要产物,而在较高的温度下,2-甲基呋喃(2-MF)是Cu-Ni/ α -Al2O3 (Cu/Ni = 1)催化剂的主要产物。同样,2,5-双羟基甲基呋喃(BHF)在较低温度下是主要产物,而2,5-二甲基呋喃(DMF)在较高温度下选择性地在HMF加氢过程中产生。此外,还讨论了两种反应的反应途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Synergism studies on alumina-supported copper-nickel catalysts towards furfural and 5-hydroxymethylfurfural hydrogenation

The structure of alumina-supported copper-nickel catalysts prepared by impregnation method was studied by using a combination of various characterization techniques including XRD, N2-sorption, TEM, H2-TPR, NH3-TPD, XANES/EXAFS and CHNS methods. A series of characterizations revealed that dispersion of copper increases with an increase in nickel loading on ɣ-Al2O3 due to strong interaction between nickel and copper oxide particles. This also led to the formation of mixed copper-nickel oxides in calcined catalysts at the highest loading of nickel and copper (i.e. Cu/Ni = 1). In catalytic activity, both the monometallic Cu/ɣ-Al2O3 and Ni/ɣ-Al2O3 showed lower activity and selectivity towards hydrogenation of both Furfural and 5-Hydroxymethylfurfural to 2-methylfuran (2-MF) and 2, 5-dimethylfuran (DMF), respectively. However, with increase in nickel loading, the activity and the selectivity of Cu/ɣ-Al2O3 drastically increased for both the cases and Cu-Ni/ɣ-Al2O3 (Cu/Ni = 1) showed the highest catalytic activity. Furthermore, combination of Cu/Ni ratios and temperature plays a significant role in the product distribution, as in the case of furfural hydrogenation, at a lower temperature, furfuryl alcohol (FOL) appears as the main product while at a higher temperature, 2-methylfuran (2-MF) is found to be the dominant product over Cu-Ni/ɣ-Al2O3 (Cu/Ni = 1) catalysts. Similarly, 2,5-bishydroxymethylfuran (BHF) is found to be the major product at a lower temperature and 2,5-dimethylfuran (DMF) is selectively produced at a higher temperature in the HMF hydrogenation. Furthermore, reaction pathways are discussed for both the reactions.

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期刊介绍: The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.
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