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ZrO2晶相对锰铈系SCR催化剂脱硝活性的影响

叶 飞 刘 荣 贡湘君 管 昊

叶 飞, 刘 荣, 贡湘君, 管 昊. ZrO2晶相对锰铈系SCR催化剂脱硝活性的影响[J]. 环境科学研究, 2015, 28(11): 1720-1727.
引用本文: 叶 飞, 刘 荣, 贡湘君, 管 昊. ZrO2晶相对锰铈系SCR催化剂脱硝活性的影响[J]. 环境科学研究, 2015, 28(11): 1720-1727.
YE Fei, LIU Rong, GONG Xiangjun, GUAN Hao. Effects of Zirconia Crystallite Phases on MnOx-CeO2 SCR DeNOx Catalysts[J]. Research of Environmental Sciences, 2015, 28(11): 1720-1727.
Citation: YE Fei, LIU Rong, GONG Xiangjun, GUAN Hao. Effects of Zirconia Crystallite Phases on MnOx-CeO2 SCR DeNOx Catalysts[J]. Research of Environmental Sciences, 2015, 28(11): 1720-1727.

ZrO2晶相对锰铈系SCR催化剂脱硝活性的影响

基金项目: 江苏省环境保护厅基金项目(2013032);江苏高校优势学科建设工程项目

Effects of Zirconia Crystallite Phases on MnOx-CeO2 SCR DeNOx Catalysts

  • 摘要: 采用浸渍法制备了以nm级c-ZrO2(立方相ZrO2)、t-ZrO2(四方相ZrO2)和m-ZrO2(单斜相ZrO2)为载体的负载型MnOx-CeO2/ZrO2催化剂,并在连续流动固定床反应器上考察了催化剂的NH3-SCR低温脱硝性能. 结果表明,催化剂脱硝性能良好,当MnOx负载量(以w计)为15.0%时,以c-ZrO2为载体的催化剂脱硝效率在103 ℃即可达到100%. 在相同活性组分负载量和反应温度条件下,各催化剂的低温脱硝活性体现出MnOx-CeO2/c-ZrO2>MnOx-CeO2/t-ZrO2>MnOx-CeO2/m-ZrO2的规律,因此对MnOx负载量为5.0%的MnOx-CeO2/ZrO2系列催化剂进行进一步表征,以探究该规律的内在影响因素. BET测试结果表明,以c-ZrO2为载体的催化剂的比表面积最大,达到39.67 m2/g,更有利于气体和催化剂表面活性位的接触. XPS测试结果表明,以c-ZrO2为载体的催化剂表面晶格氧含量最丰富,有助于Lewis酸性位的形成. TPR和TPD测试图谱中的峰强及峰面积表明,以c-ZrO2和t-ZrO2为载体的催化剂表面主要存在Lewis酸性位;而在以m-ZrO2为载体的催化剂表面,Lewis酸性位较多,同时还存在少量的Brnsted酸性位. 研究显示,ZrO2晶型结构变化引起MnOx-CeO2/ZrO2催化剂的比表面积、表面活性酸性位的不同是产生晶型效应的原因所在; 采用ZrO2作为负载型低温SCR催化剂载体时,以立方相晶型结构为最佳.

     

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出版历程
  • 收稿日期:  2015-01-21
  • 修回日期:  2015-08-12
  • 刊出日期:  2015-11-25

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