甲醇热制备四方相ZrO2及其负载镍催化剂的顺酐加氢性能

doi:10.11949/j.issn.0438-1157.20170005

摘要/Abstract

摘要：

通过改变甲醇热时间制备了一系列不同晶粒尺寸的四方相 ZrO₂，采用过体积浸渍法制备了Ni 含量（质量分数）为10%的Ni/ZrO₂催化剂，并考察了其催化顺酐液相加氢性能。采用氮气吸附-脱附（BET）、X射线衍射（XRD）、氢气程序升温还原（H₂-TPR）、X射线光电子能谱（XPS）、原位红外光谱（in situ FTIR）等手段对催化剂进行了表征。研究结果表明，分散性好、晶粒尺寸小的Ni物种有利于C=C键加氢生成丁二酸酐；而金属-载体强相互作用的形成则有利于C=O加氢生成 γ-丁内酯。当甲醇热时间为2 h时，制备的Ni/ZrO₂催化剂的C=O加氢活性最高，在反应温度为210℃，反应压力为5 MPa，反应时间为3 h时，其顺酐转化率达100%，γ-丁内酯选择性为44.7%。

关键词: 顺酐加氢, γ-丁内酯, 催化剂, 金属-载体强相互作用

Abstract:

A series of tetragonal ZrO₂ which support different crystalline size were prepared by methanol thermal method. Ni/ZrO₂catalysts with Ni content of 10%(mass) were prepared by impregnation method and applied in the liquid phase hydrogenation of maleic anhydride. All catalysts were characterized by N₂ physical adsorption-desorption, H₂-temperature programmed reduction(H₂-TPR), X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS) and in situ Fourier transform infrared spectroscopy(in situ FTIR). Higher dispersion and smaller crystallite size of metallic Ni favored the hydrogenation of C=C to produce succinic anhydride. While the formation of strong metal-support interaction contributed the hydrogenation of C=O to produce γ-butyrolactone. When methanol thermal time was 2 h, the Ni/ZrO₂-2 catalyst showed the highest catalytic activity for C=O hydrogenation.

Key words: liquid phase hydrogenation of maleic anhydride, γ-butyrolactone, catalyst, strong metal-support interaction

中图分类号:

O643.36

梁二艳, 张因, 赵丽丽, 徐亚琳, 赵永祥. 甲醇热制备四方相ZrO₂及其负载镍催化剂的顺酐加氢性能[J]. 化工学报, 2017, 68(6): 2352-2358.

LIANG Eryan, ZHANG Yin, ZHAO Lili, XU Yalin, ZHAO Yongxiang. Selective hydrogenation of maleic anhydride over Ni/ZrO₂catalysts with ZrO₂ prepared by methanol thermal method[J]. CIESC Journal, 2017, 68(6): 2352-2358.

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甲醇热制备四方相ZrO₂及其负载镍催化剂的顺酐加氢性能

Selective hydrogenation of maleic anhydride over Ni/ZrO₂catalysts with ZrO₂ prepared by methanol thermal method

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