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作 者:刘琪英[1] 李勇[1] 蔡伟杰[1] 李娟[1] 徐奕德[1] 申文杰[1]
机构地区:[1]中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023
出 处:《分子催化》2007年第4期294-299,共6页Journal of Molecular Catalysis(China)
摘 要:采用浸渍法制备了一系列负载的州催化剂,用于糠醛选择性加氢反应.用XRD、TPR等手段对Ni/γ-Al2O3样品进行了表征.结果表明,Ni负载量在5-115%范围内,高度分散于载体γ-Al2O3表面,Ni负载量进一步提高到20%,则在载体表面聚集成为微晶.在10%Ni/γ-Al2O3样品上提高焙烧温度有利于Ni的前驱体分解且高度分散于载体表面.Ni^2+与γ-Al2O3存在较强的相互作用,但这种相互作用随着州负载量的增加而逐渐减弱,随着焙烧温度的增加而逐渐增强.与其他载体负载的Ni催化剂相比,Ni/γ-Al2O3由于其大的表面和适当的表面结构,在糠醛加氢反应中表现出一定的活性和较高的选择性,且随着Ni负载量的增加,活性逐渐增强,但选择性有所下降.另外催化剂的焙烧温度、还原温度,反应温度和溶剂对该反应均有较大影响,采用极性有机溶剂,适宜的焙烧和还原温度有利于催化剂活性和选择性的提高.Nickel supported hydrogenation of furfural to on various metallic oxides was prepared by impregnation method, and used for selective furfural alcohol in a 100 mL stainless steel autoclave lined with chanical stirrer. The Ni/γ-Al2O3 samples were characterized by X-ray Diffraction (XRD) grammed Reduction (TPR). It was found that nickel could disperse highly on the surface quartz glass with me- and Temperature-Pro- of γ-Al2O3 within the nickel loadings of 5 ~15% and aggregate over 20% Ni/γ-Al2O3. The increase of calcination temperatures promoted the dispersion of nickel through decomposes of nickel hydroxides to nickel oxides. Results of TPR indicated the existence of strong interactions between the metal and support, and the interactions decreased with the increase of nickel loadings. Moreover, the calcination temperatures could promote the interactions due to the highly dispersion of nickel at higher calcined temperature. Some acitivity and high selectivity to furfural alcohol was found in hydrogenation of furfural over 10% Ni/γ-Al2O3 because of the large surface and appropriate surface structures of γ-Al2O3. In addition, hydrogenation of furfural in nonpolar solvent such as cyclohexane exhibited higher selectivity to furfural alcohol comparing to ethanol, due to the elimination of acetals between the reaction of furfural and ethanol.
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