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宽工作温度烟气脱硝催化剂制备及反应机理研究

郭凤,  余剑,  牟洋,  初茉,  许光文

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文章导航 > 燃料化学学报（中英文）  > 2014 >  42(01): 101-109
郭凤, 余剑, 牟洋, 初茉, 许光文. 宽工作温度烟气脱硝催化剂制备及反应机理研究[J]. 燃料化学学报（中英文）, 2014, 42(01): 101-109.
引用本文: 郭凤, 余剑, 牟洋, 初茉, 许光文. 宽工作温度烟气脱硝催化剂制备及反应机理研究[J]. 燃料化学学报（中英文）, 2014, 42(01): 101-109.
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GUO Feng, YU Jian, MU Yang, CHU Mo, XU Guang-wen. Preparation of catalyst with wide working-temperature and the reaction mechanism of flue gas denitration[J]. Journal of Fuel Chemistry and Technology, 2014, 42(01): 101-109.
Citation: GUO Feng, YU Jian, MU Yang, CHU Mo, XU Guang-wen. Preparation of catalyst with wide working-temperature and the reaction mechanism of flue gas denitration[J]. Journal of Fuel Chemistry and Technology, 2014, 42(01): 101-109.
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宽工作温度烟气脱硝催化剂制备及反应机理研究

  • 1.

    中国矿业大学(北京) 化学与环境工程学院, 北京 100083;

  • 2.

    中国科学院过程工程研究所 多相复杂系统国家重点实验室, 北京 100190

基金项目: 国家自然科学基金（21106156）；国家高技术研究发展计划（863计划，2010AA065004）；国际合作项目（2013DFA51530）；中国科学院战略性先导科技专项（XDA07030300）。
详细信息
    通讯作者:

    余剑，Tel：010-82544905，E-mail：yujian@home.ipe.ac.cn；许光文，Tel：010-82544886，E-mail：gwxu@home.ipe.ac.cn。

  • 中图分类号: O643

Preparation of catalyst with wide working-temperature and the reaction mechanism of flue gas denitration

  • 1.

    School of Chemical and Environmental Engineering, China University of Mining & Technology, Beijing 100083, China;

  • 2.

    State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China

    摘要
  • 摘要: 以溶胶-凝胶法制备介孔TiO2载体，采用分步浸渍法制备了V2O5-WO3/TiO2催化剂，借助BET、NH3-TPD、H2-TPR、SEM、活性评价、In-situ FT-IR等手段，考察了催化剂的结构、酸性、还原性、脱硝活性及反应机理等。介孔TiO2载体比表面积为158.6 m2/g，制成催化剂后比表面积略有降低，约为136.7 m2/g。针对模拟烟气在φNH3/φNO=0.8的条件下测试催化剂的脱硝活性温度窗口为250~400 ℃，脱硝转化率达到80%。NH3-TPD和H2-TPR表征结果表明，催化剂在活性温度范围内具有典型的表面酸性位，载体TiO2与V2O5之间存在的相互作用使得V2O5还原温度降低。利用In-situ FT-IR研究NH3和NO在V2O5-WO3/TiO2催化剂表面吸附和氧化的反应过程发现，NH3可同时吸附在L酸位和B酸位，NH3在活性位上氧化脱氢形成NH2物种是SCR脱硝反应的控制步骤。研究NO+O2+NH3反应时发现，吸附NH3的催化剂引入NO和O2后，共价吸附的NH3首先消失。选择性催化还原反应发生在吸附态NH3和气态或弱吸附态的NO之间，该反应遵从Eley-Rideal反应机理。
    Abstract: The V2O5-WO3/TiO2 catalyst using the mesoporous support of TiO2 made by sol-gel method was prepared with two-step impregnation method and tested for the selective catalytic reduction (SCR) of NO by NH3. The characterization of the catalyst with BET, NH3-TPD, H2-TPR, SEM, activity evaluation and in-situ FT-IR was made to have a deep understanding of the structure, acidity, redox property, catalytic performance, de-NOx activity and the reaction mechanism. The mesoporous TiO2 has a surface area of 158.6 m2/g, and the prepared de-NOx catalyst has a slightly decreased surface area of 136.7 m2/g. The V2O5-WO3/TiO2 catalyst enables the NO conversions to reach to about 80% at 250~400 ℃ and φNH3/φNO = 0.8, showing the feature of wide working-temperature for the catalyst. The surface adsorption of reactants characterized by in-situ FT-IR shows that NH3 is adsorbed on both the Lewis and Brnsted acidic sites to generate a few different transformation species. The transformation from NH3 to NH2 is the rate-determining step for de-NOx reaction in NH3-SCR. It is found that the NH3-SCR reaction occurs between the adsorbed NH3 and gaseous NO, which follows the Eley-Rideal reaction mechanism.
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  • 收稿日期:  2013-05-03
  • 修回日期:  2013-07-05
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