催化学报

催化学报 ›› 2013, Vol. 34 ›› Issue (1): 263-271.DOI: 10.3724/SP.J.1088.2013.20846

• 研究论文 • 上一篇    下一篇

Ni/SiO2 和 SO3H-C/SBA-15 复合催化剂上硝基苯加氢制对氨基苯酚

白玉婷, 朱学成, 张利雄*, 徐南平   

  1. 南京工业大学化学化工学院, 材料化学工程国家重点实验室, 江苏南京 210009
  • 收稿日期:2012-08-20 修回日期:2012-10-22 出版日期:2013-01-23 发布日期:2013-01-23

Catalytic hydrogenation of nitrobenzene to p-aminophenol over Ni/SiO2 and SO3H-C/SBA-15 solid acid mixed catalyst

BAI Yuting, ZHU Xuecheng, ZHANG Lixiong*, XU Nanping   

  1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, Jiangsu, China
  • Received:2012-08-20 Revised:2012-10-22 Online:2013-01-23 Published:2013-01-23

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摘要： 将 Ni/SiO2 催化剂与磺酸功能化的 C/SBA-15 固体酸 (SO3H-C/SBA-15) 混合用于催化硝基苯制对氨基苯酚的反应, 考察了二者的质量比、反应压力和温度、搅拌速度和反应时间等对反应性能的影响, 采用 X 射线衍射、H2 程序升温脱附、透射电镜、N2 吸附-脱附、红外光谱和热重分析对催化剂进行了表征. 结果表明, Ni/SiO2 上活性中心分布均匀, 碳含量为 40% 的 SO3H-C/SBA-15 上固体酸酸值最大. 当 Ni/SiO2 和 SO3H-C/SBA-15 质量比为 1:6 时, 反应活性较好; 在 120 ºC, 0.6 MPa 和搅拌速度 1200 r/min 的条件下反应 3 h, 硝基苯转化率为 85.1%, 对氨基苯酚选择性为 23.8%. 与文献中大多数采用 Pt 和固体酸混合用作催化剂时相当.

关键词: 镍催化剂, 固体酸, 磺酸功能基, SBA-15 分子筛, 硝基苯加氢, 对氨基苯酚

Abstract: Mechanical mixed catalysts comprised of 20% Ni/SiO2 and carbon-silica mesoporous composite functionalized with sulfonic acid groups (SO3H-C/SBA-15) were used for hydrogenation of nitrobenzene to p-aminophenol. The effects of the mass ratio of Ni/SiO2 to SO3H-C/SBA-15, reaction pressure, temperature, stirring speed, and reaction time were examined. The catalysts were characterized by X-ray diffraction, H2 temperature-programmed desorption, transmission electron microscopy, infrared spectroscopy, and thermal gravity analysis. The results indicated that Ni is uniformly dispersed on the support, forming a single active center. The SO3H-C/SBA-15 solid acid with 40% carbon content exhibits the highest acid density. The mixed catalyst with a Ni/SiO2 to SO3H-C/SBA-15 mass ratio of 1:6 shows the highest activity. Under optimized reaction conditions of a reaction temperature of 120 ºC, reaction pressure of 0.6 MPa, stirring speed of 1200 r/min, and reaction time of 3 h, the nitrobenzene conversion of 85.1% and p-aminophenol selectivity of 23.8% were obtained. The reaction result is comparable with those on most mixed catalysts containing Pt and solid acid reported in the literature.

Key words: nickel catalyst, solid acid, sulfonic acid group, SBA-15 zeolite, nitrobenzene hydrogenation, p-aminophenol