催化学报

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2009-2017.DOI: 10.1016/S1872-2067(12)60715-3

• 研究论文 • 上一篇    下一篇

选择氧化物载体调变乙醇重整和1,3-丁二烯加氢反应双金属催化剂

王铁峰a, Willim Lonergnb, 陈经广c   

  1. a 清华大学化工系, 绿色反应工程与工艺北京市重点实验室, 北京100084, 中国;
    b 特拉华大学化学与生物分子工程系, 催化科技中心, 纽瓦克DE 19716, 美国;
    c 哥伦比亚大学化工系, 纽约NY 10027, 美国
  • 收稿日期:2013-09-12 修回日期:2013-09-16 出版日期:2013-10-18 发布日期:2013-10-18
  • 通讯作者: Tiefeng Wang,Jingguang G. Chen
  • 基金资助:

    美国能源部基金(DE-SC0001004);新世纪优秀人才支持计划(NCET-12-0297).

Selection of oxide supports to anchor desirable bimetallic structures for ethanol reforming and 1, 3-butadiene hydrogenation

Tiefeng Wanga, William Lonerganb, Jingguang G. Chenc   

  1. a Beijing Key Lab of Green Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China;
    b Center for Catalytic Science and Technology (CCST), Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA;
    c Department of Chemical Engineering, Columbia University, New York, NY 10027, USA
  • Received:2013-09-12 Revised:2013-09-16 Online:2013-10-18 Published:2013-10-18
  • Contact: Tiefeng Wang,Jingguang G. Chen
  • Supported by:

    This work was supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences under Award Number DE-SC0001004, and Program for New Century Excellent Talents in University of China (NCET-12-0297).

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被引次数

2

摘要：

研究了不同载体负载的Pt-Ni双金属和单金属催化剂上乙醇重整和1,3-丁二烯加氢反应性能, 以考察氧化物载体对双金属结构和催化活性的影响. 所用的氧化物载体包括γ-Al2O3, SiO2, TiO2, CeO2以及高比表面积(HSA)和低比表面积(LSA)ZrO2. 采用共浸渍法制备催化剂, 用CO化学吸附、透射电镜和扩展X射线吸收精细结构光谱进行催化剂表征, 采用傅里叶变换红外间歇反应器进行化学反应评价. 对于乙醇重整反应, Pt-Ni双金属催化剂优于单金属催化剂, Pt-Ni双金属催化剂活性顺序为TiO2 > SiO2 > γ-Al2O3 ≈ LSA-ZrO2 > CeO2 > HSA-ZrO2. 对于1,3-丁二烯加氢反应, 在SiO2, TiO2和HSA-ZrO2载体上双金属催化剂优于单金属催化剂, Pt-Ni双金属催化剂活性顺序为SiO2 > CeO2 > γ-Al2O3 > LSA-ZrO2 > HSA-ZrO2 ≈ TiO2.

关键词: 铂镍双金属催化剂, 载体影响, 乙醇重整, 1,3-丁二烯加氢, 扩展X射线吸收精细结构光谱

Abstract:

Ethanol reforming and 1,3-butadiene hydrogenation reactions were studied on Pt-Ni bimetallic and monometallic catalysts supported on several supports, including γ-Al2O3, SiO2, TiO2, CeO2, and high surface area (HSA) and low surface area (LSA) ZrO2, to elucidate the effect of oxide supports on the bimetallic structures and catalytic activity. The catalysts were prepared by co-impregnation and were characterized by pulse CO chemisorption, transmission electron microscopy, and extended X-ray absorption fine structure. Reactions were carried out in a Fourier transform infrared batch reactor. The supports strongly affected the catalytic activity. For ethanol reforming, the activities of the Pt-Ni bimetallic catalysts were in the order TiO2 > SiO2 > γ-Al2O3 ≈ LSA-ZrO2 > CeO2 > HSA-ZrO2; while for 1,3-butadiene hydrogenation, the order was SiO2 > CeO2 > γ-Al2O3 > LSA-ZrO2 > HSA-ZrO2 ≈ TiO2. For the hydrogenation reaction, the Pt-Ni bimetallic catalysts outperformed the Pt and Ni monometallic catalysts; in contrast, for the reforming reaction, synergetic bimetallic effects were only found on SiO2, TiO2, and HSA-ZrO2.

Key words: Platium-nickel bimetallic catalyst, Support effect, Ethanol reforming, 1,3-Butadiene hydrogenation, Extended X-ray absorption fine structure