化工学报 ›› 2016, Vol. 67 ›› Issue (5): 1892-1899.DOI: 10.11949/j.issn.0438-1157.20151604

• 催化、动力学与反应器 • 上一篇    下一篇

助剂改性FeOOH及其煤直接液化催化活性

谢晶1,2, 卢晗锋1, 陈银飞1, 高山松2, 王洪学2   

  1. 1 浙江工业大学化学工程学院, 浙江 杭州 310014;
    2 中国神华煤制油化工有限公司上海研究院, 煤直接液化国家重点工程实验室, 上海 201108
  • 收稿日期:2015-10-22 修回日期:2016-01-19 出版日期:2016-05-05 发布日期:2016-05-05
  • 通讯作者: 卢晗锋
  • 基金资助:

    神华集团科技创新项目(MZY-13-12)。

Promoters modified FeOOH and their catalytic performances for direct coal liquefaction

XIE Jing1,2, LU Hanfeng1, CHEN Yinfei1, GAO Shansong2, WANG Hongxue2   

  1. 1 College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China;
    2 China Shenhua Coal to Liquid and Chemical Shanghai Research Institute, National Engineering Laboratory for Direct Coal Liquefaction, Shanghai 201108, China
  • Received:2015-10-22 Revised:2016-01-19 Online:2016-05-05 Published:2016-05-05
  • Supported by:

    supported by Science and Technology Development Department of China Shenhua Group (MZY-13-12).

摘要:

采用共沉淀法分别引入Si、Al、La、Ca、Mg、Zr、Cu、Ni和Co 9种助剂元素对FeOOH催化剂改性,借助BET、XRD、SEM手段表征各助剂对催化剂微观结构、晶相和形貌的影响,在0.5 L高压釜内测试各催化剂对神东煤的直接液化催化活性。结果表明,引入Si、Al、Ca、Zr、Ni、Co能改善催化剂比表面积和分散度,分别提高煤液化油收率0.7~2.7个百分点;Ni和Co为最优助剂,Mg没有促进作用,Cu、La降低了油收率。研究表明,Al、Ca、Zr是通过结构支撑改善催化剂的织构性质,促进生成易于转化为活性相的小晶粒g-FeOOH,Ni、Co主要起到电子型助剂作用,通过强化对氢气的活化,促进煤的转化,提高油收率。

关键词: 煤直接液化, FeOOH催化剂, 改性, 助剂, 共沉淀, 油收率

Abstract:

Modified FeOOH catalysts were prepared by a co-precipitation method using Si, Al, La, Ca, Mg, Zr, Cu, Ni and Co as promoters, respectively. The effects on microstructures, crystalline phase and morphology of the catalysts were characterized by BET, XRD and SEM. Their catalytic performances for the direct liquefaction of Shendong coal were evaluated in a 0.5 L stirring autoclave. The results showed that these promoters (Si, Al, Ca, Zr, Ni and Co) could improve the dispersion of the catalysts and surface area, and then improve the catalytic performances for direct coal liquefaction. Increasing by 0.7%—2.7% oil yield over the unmodified the catalyst could be obtained. However, Mg showed no effect on catalytic ability, while Cu and La reduced the Oil yield. The result indicated that Si, Al, Ca and Zr as the structure promoters could significantly improve the texture properties of catalysts, resulting in an increase of γ-FeOOH crystalline phase with small size which was beneficial to form active phase (Fe1-xS). Co and Ni as the electronic promoters could activate H2 preferentially to promote liquefaction, leading to the rising in oil yield.

Key words: direct coal liquefaction, FeOOH catalyst, modify, promoter, co-precipitation, oil yield

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