物理化学学报 >> 2017, Vol. 33 >> Issue (3): 602-610.doi: 10.3866/PKU.WHXB201611251

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锐钛矿型TiO2担载的Pd催化剂用于乙炔选择加氢的催化性能及其表征

高晓平1,2,郭章龙1,2,周亚男1,2,敬方梨1,储伟1,2,*()   

  1. 1 四川大学化学工程学院,成都610065
    2 四川大学新能源与低碳技术研究院,成都610207
  • 收稿日期:2016-08-26 发布日期:2017-03-07
  • 通讯作者: 储伟 E-mail:chuwei1965@scu.edu.cn
  • 基金资助:
    国家自然科学基金(21476145)

Catalytic Performance and Characterization of Anatase TiO2 Supported Pd Catalysts for the Selective Hydrogenation of Acetylene

Xiao-Ping GAO1,2,Zhang-Long GUO1,2,Ya-Nan ZHOU1,2,Fang-Li JING1,Wei CHU1,2,*()   

  1. 1 School of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China
    2 Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610207, P. R. China
  • Received:2016-08-26 Published:2017-03-07
  • Contact: Wei CHU E-mail:chuwei1965@scu.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21476145)

摘要:

采用水热法合成了含有89%{101}晶面的TiO2纳米锭(TiO2-101)和77%{001}晶面的TiO2纳米片(TiO2-001),将其用作载体来制备担载钯催化剂;研究了上述制备的TiO2纳米材料对Pd/TiO2-101和Pd/TiO2-001催化剂用于乙炔选择加氢制聚合级乙烯催化性能的影响.结果表明, Pd/TiO2-101催化剂表现出更好的乙炔转化率和乙烯收率.通过氢气程序升温脱附(H2-TPD)、氢气程序升温还原(H2-TPR)、透射电子显微镜(TEM)、CO化学吸附、X射线光电子能谱(XPS)和热重分析仪(TGA)等对催化剂进行了结构表征和分析.TEM和CO化学吸附结果表明, Pd纳米颗粒(NPs)在TiO2-101载体上有较小的颗粒尺寸(1.53 nm)和较高的分散度(15.95%);而Pd纳米颗粒在TiO2-001载体上的颗粒尺寸是4.36 nm和9.06%的分散度.Pd/TiO2-101催化剂上较小的Pd颗粒尺寸及其较高的分散度使催化剂具有更多的反应活性位点,这促进了其反应的催化活性.

关键词: Pd/TiO2催化剂, 乙炔选择加氢, 锐钛矿型TiO2, {101}晶面, 结构表征

Abstract:

Anatase TiO2 nanospindles containing 89% exposed {101} facets (TiO2-101) and nanosheets with 77% exposed {001} facets (TiO2-001) were hydrothermally synthesized and used as supports for Pd catalysts. The effects of the TiO2 materials on the catalytic performance of Pd/TiO2-101 and Pd/TiO2-001 catalysts were investigated in the selective hydrogenation of acetylene to polymer-grade ethylene. The Pd/TiO2-101 catalyst exhibited enhanced performance in terms of acetylene conversion and ethylene yield. To understand these effects, the catalysts were characterized by H2 temperature-programmed desorption (H2-TPD), H2 temperatureprogrammed reduction (H2-TPR), transmission electron microscopy (TEM), pulse CO chemisorption, X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The TEM and CO chemisorption results confirmed that Pd nanoparticles (NPs) on the TiO2-101 support had a smaller average particle size (1.53 nm) and a higher dispersion (15.95%) than those on the TiO2-001 support (average particle size of 4.36 nm and dispersion of 9.06%). The smaller particle size and higher dispersion of Pd on the Pd/TiO2-101 catalyst provided more reaction active sites, which contributed to the improved catalytic activity of this supported catalyst.

Key words: Pd/TiO2 catalyst, Acetylene selective hydrogenation, Anatase TiO2, {101}plane, Structure characterization

MSC2000: 

  • O643