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化学学报
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化学学报 ›› 2011, Vol. 69 ›› Issue (13): 1517-1523. 上一篇    下一篇

研究论文

高分散Mn-KIT-6催化剂的制备及催化性能研究

徐玉然1, 王灵灵1, 原恩临1, 金军江1, 李永生*,1, 赵文茹1, 李华1, 施剑林1,2   

  1. (1华东理工大学材料科学与工程学院 超细材料制备与应用教育部重点实验室 上海 200237)
    (2中国科学院上海硅酸盐研究所 上海 200052)
  • 投稿日期:2010-11-24 修回日期:2011-01-26 发布日期:2011-03-07
  • 通讯作者: 李永生 E-mail:ysli@ecust.edu.cn

Preparation of Highly Dispersed Mn-KIT-6 Catalysts and Their Catalysis Performance

Xu Yuran1; Wang Lingling1; Yuan Enlin1; Jin Junjiang1; Li Yongsheng*,1; Zhao Wenru1; Li Hua1; Shi Jianlin1,2   

  1. (1 Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237)
    (2 Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200052)
  • Received:2010-11-24 Revised:2011-01-26 Published:2011-03-07

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1253

被引次数

12

以介孔分子筛KIT-6为载体, 采用溶液浸渍法将乙酰丙酮锰(III)的糠醇溶液灌注到KIT-6的孔道内, 一定条件下将糠醇碳化后再焙烧脱除碳, 制得Mn-KIT-6催化剂. 通过X射线衍射(XRD)|氮气物理吸附-脱附|紫外-可见吸收光谱(UV-Vis)|傅里叶变换红外光谱(FT-IR)|电感耦合等离子发射光谱(ICP-AES)|透射电镜(TEM)|氨气-程序升温脱附(NH3-TPD)及X射线光电子能谱(XPS)等方法对样品进行了表征. 结果表明锰在KIT-6孔道内部高度分散, 同时催化剂保持高度有序的孔道结构、较大的比表面积和孔容. 正丁醇和乙酸的催化酯化反应结果表明, 该催化剂具有很高的催化活性, 反应4 h后乙酸正丁酯的产率高达97.3%, 使用5次后催化剂依然具有较高的活性.

关键词: 氧化锰, KIT-6, 液相等体积共浸渍, 高分散, 酯化反应

In this paper, highly dispersed Mn-KIT-6 catalysts were prepared via a simple incipient wetness co-impregnation route by casting furfurylalcohol (FA) solution of manganese(III) acetylacetonate, which were used as carbon and Mn sources, respectively, into the channels of KIT-6, followed by the subsequent removal of the carbon resulted from carbonized FA. The catalysts were characterized by X-ray diffraction (XRD), N2 adsorption-desorption, UV-visible absorption spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR)|inductively coupled plasma emission spectroscopy (ICP-AES), transmission electron microscope (TEM), temperature programmed desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS). The results showed that Mn species were highly dispersed onto the pore surface of KIT-6 with the well maintenance of the highly ordered meso-structure of KIT-6. The catalysts exhibited high catalytic activity in the etherification of N-butanol and acetic acid, with the yield of butyl acetate as high as 97% after 4 h reaction. The reusability and stability were demonstrated with the high activity after 5 runs.

Key words: manganese oxide, KIT-6, incipient wetness co-impregnation, high dispersion, etherification