物理化学学报 >> 2015, Vol. 31 >> Issue (3): 527-532.doi: 10.3866/PKU.WHXB201501052

催化和表面科学 上一篇    下一篇

Co-B/γ-Al2O3非晶态催化剂的制备及其催化乳酸乙酯液相加氢性能

赵凤伟, 沈美玉, 王琳, 杜长海   

  1. 长春工业大学化学工程学院, 长春 130012
  • 收稿日期:2014-11-05 修回日期:2015-01-02 发布日期:2015-03-06
  • 通讯作者: 杜长海 E-mail:du661123@163.com
  • 基金资助:

    吉林省科技厅自然科学基金(201215117)资助项目

Preparation of Amorphous Co-B/γ-Al2O3 Catalyst and Its Performance in Catalytic Liquid Phase Hydrogenation of Ethyl Lactate

ZHAO Feng-Wei, SHEN Mei-Yu, WANG Lin, DU Chang-Hai   

  1. School of Chemical Engineering, Changchun University of Technology, Changchun 130012, P. R. China
  • Received:2014-11-05 Revised:2015-01-02 Published:2015-03-06
  • Contact: DU Chang-Hai E-mail:du661123@163.com
  • Supported by:

    The project was supported by the Natural Science Foundation of Jilin Provincial Science &Technology Department, China (201215117).

摘要:

采用浸渍-还原法制备了负载型Co-B/γ-Al2O3非晶态合金催化剂, 并将其应用于乳酸乙酯液相加氢制备1,2-丙二醇(1,2-PDO)反应中, 研究了其催化加氢性能. 采用电感耦合等离子体(ICP)发射光谱仪、X射线衍射(XRD)仪、透射电子显微镜(TEM)、差示扫描量热(DSC)、X射线光电子能谱(XPS)等手段对催化剂的性能进行了表征, 考察了制备条件对催化剂性能的影响. 结果表明, 新鲜的Co-B/γ-Al2O3催化剂具有非晶态结构, Co-B均匀地分散在载体γ-Al2O3上. 随着Co负载量的增加, 催化剂的热稳定性提高, 催化剂表面Co/B原子比增加. 当金属Co理论负载量为30%(质量分数, w)时, Co-B/γ-Al2O3催化剂表现出最高的加氢催化性能, 在160 ℃, 氢气压力为6.0 MPa条件下反应9 h, 乳酸乙酯的转化频率(TOF)为1.41 h-1, 转化率达到93.63%, 1,2-丙二醇的选择性达到96.10%. 催化剂的加氢性能取决于其分散均匀的Co-B纳米粒子、较高的表面Co/B原子比及Co和B之间的电子转移效应.

关键词: 非晶态催化剂, Co-B/γ-Al2O3, 乳酸乙酯, 1,2-丙二醇, 催化加氢

Abstract:

Supported cobalt amorphous catalysts Co-B/γ-Al2O3 were prepared using an impregnation-chemical reduction method for liquid phase hydrogenation of ethyl lactate to 1,2-propanediol (1,2-PDO). The Co-B/γ-Al2O3 catalysts were characterized using inductively coupled plasma (ICP) optical emission spectrometry, X-ray diffraction (XRD), transmission electron microscopy (TEM), differential scanning calorimetry (DSC), and X-ray photoelectron spectroscopy (XPS). The effects of the catalyst preparation conditions on the hydrogenation of ethyl lactate were investigated. All the fresh catalysts showed an amorphous structure and Co-B particles were dispersed uniformly on the γ-Al2O3 support. The thermal stability of the amorphous catalyst and the Co/B atomic ratio of surface composition increased with increasing the Co content. The Co-B/γ-Al2O3 amorphous catalyst showed the highest catalytic activity when the theoretical loading of metal Co was 30% (mass fraction, w). The ethyl lactate turnover frequency (TOF), conversion, and selectivity to 1,2-PDO reached 1.41 h-1, 93.63%, and 96.10%, respectively at a reaction temperature of 160 ℃ and hydrogen pressure of 6.0 MPa for 9 h. The higher catalytic performance of the 30%(w) Co-B/γ-Al2O3 supported amorphous catalyst is attributed to its highly dispersing Co-B particles, higher Co/B atomic ratio of surface composition, and electron transfer effect between Co and B.

Key words: Amorphous catalyst, Co-B/γ-Al2O3, Ethyl lactate, 1,2-Propanediol, Catalytic hydrogenation

MSC2000: 

  • O643