NH3-SCR反应中Fe-ZSM-5的Fe物种分布和酸性位对其水热稳定性及抗硫和抗碳氢性能的影响

doi:10.1016/S1872-2067(14)60268-0

催化学报 ›› 2015, Vol. 36 ›› Issue (4): 649-656.DOI: 10.1016/S1872-2067(14)60268-0

NH₃-SCR反应中Fe-ZSM-5的Fe物种分布和酸性位对其水热稳定性及抗硫和抗碳氢性能的影响

石晓燕, 贺泓, 谢利娟

中国科学院生态环境研究中心, 北京 100085

收稿日期:2014-11-04 修回日期:2014-12-12 出版日期:2015-03-23 发布日期:2015-03-23
通讯作者: Xiaoyan Shi
基金资助:
国家高技术研究发展计划(863计划, 2013AA065301); 国家自然科学基金(51278486, 51221892).

The effect of Fe species distribution and acidity of Fe-ZSM-5 on the hydrothermal stability and SO₂ and hydrocarbons durability in NH₃-SCR reaction

Xiaoyan Shi, Hong He, Lijuan Xie

State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China

Received:2014-11-04 Revised:2014-12-12 Online:2015-03-23 Published:2015-03-23
Supported by:
This work was financially supported by the National High Technology Research and Development Program of China (863 Program, 2013AA065301) and the National Natural Science Foundation of China (51278486, 51221892).

摘要/Abstract

摘要：

以Na⁺型和H⁺型ZSM-5为载体制备了Fe-ZSM-5催化剂并用于氨选择性催化还原(NH₃-SCR)氮氧化物. Fe-H-ZSM-5在新鲜时和750 ^oC含10%水的空气中老化后, 其SCR活性均优于Fe-Na-ZSM-5. 表征结果显示, Fe-H-ZSM-5和Fe-Na-ZSM-5的Fe物种分布和酸性位有所不同. 高温水热老化后Fe-H-ZSM-5分子筛骨架的脱铝较Fe-Na-ZSM-5严重. 水和硫的存在对Fe-H-ZSM-5和Fe-Na-ZSM-5的SCR活性的影响相似, 即降低了低温活性, 略提高了高温活性. Fe-Na-ZSM-5表现出比Fe-H-ZSM-5更好的抗碳氢中毒性能. 这两种催化剂的SO₂和碳氢中毒是可逆的.

关键词: 铁-ZSM-5, 氨选择性催化还原, 氮氧化物净化, 抗硫性能, 水热稳定性

Abstract:

Fe-exchanged ZSM-5 catalysts prepared from Na⁺ and H⁺ forms of ZSM-5 were evaluated for the selective catalytic reduction of NO_x by NH₃ (NH₃-SCR). Fe-H-ZSM-5 showed higher SCR activity than Fe-Na-ZSM-5 both when fresh and after hydrothermal aging at 750 ℃ in 5% H₂O/air. The Fe species distribution and acidity of Fe-H-ZSM-5 and Fe-Na-ZSM-5 were found to be different. The dealumination of the zeolite framework of Fe-H-ZSM-5 during hydrothermal aging was found to be more severe compared with that of Fe-Na-ZSM-5. The durability of Fe-H-ZSM-5 and Fe-Na-ZSM-5 in NH₃-SCR was compared using SO₂ tolerance and hydrocarbon resistance experiments. The effect of water and SO₂ on the activity of the two catalysts was similar, such that their activity decreased at low temperatures and increased at high temperatures. Fe-Na-ZSM-5 showed better propene resistance than Fe-H-ZSM-5. The SO₂ and propene poisoning of the two Fe-ZSM-5 catalysts were found to be reversible.

Key words: Iron-ZSM-5, Ammonia selective catalytic reduction, Removal of nitrogen oxide, SO₂ durability, Hydrothermal stability

石晓燕, 贺泓, 谢利娟. NH₃-SCR反应中Fe-ZSM-5的Fe物种分布和酸性位对其水热稳定性及抗硫和抗碳氢性能的影响[J]. 催化学报, 2015, 36(4): 649-656.

Xiaoyan Shi, Hong He, Lijuan Xie. The effect of Fe species distribution and acidity of Fe-ZSM-5 on the hydrothermal stability and SO₂ and hydrocarbons durability in NH₃-SCR reaction[J]. Chinese Journal of Catalysis, 2015, 36(4): 649-656.

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NH₃-SCR反应中Fe-ZSM-5的Fe物种分布和酸性位对其水热稳定性及抗硫和抗碳氢性能的影响

The effect of Fe species distribution and acidity of Fe-ZSM-5 on the hydrothermal stability and SO₂ and hydrocarbons durability in NH₃-SCR reaction

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