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[二氧化硫对CoH-ZSM-5催化甲烷选择性还原NO催化性能的影响]

[Effect of SO2 on the catalytic performance of CoH-ZSM-5 for selective catalytic reduction of NO by CH4].

作者信息

Zhang Jin-qiao, Liu Yu-ying, He Yong, Fan Wei-bin, Li Rui-feng

机构信息

Institute of Special Chemicals, Taiyuan University of Technology, Taiyuan 030024, China.

出版信息

Huan Jing Ke Xue. 2006 Sep;27(9):1717-21.

Abstract

Selective catalytic reduction of NO by methane over CoH-ZSM-5 in the presence of SO2 was studied. SO2-TPSR and NO+ (O2)-TPD techniques were applied to quantify the active sites and probe the poison effect. At 773 K, addition of 78 x 10(-6) SQ2, the NO to N2 conversion ratio decreases from 72% and reaches stable level 58%. Increasing the reaction temperature to 823 K, the NO to N2 conversion ratio increases to 62%. Co-existence of 2.55% H2O and 78 x 10(-6) SO2 at 773 K, the NO to N2 conversion ratio decreases further to 51% , but almost no effect is observed at 873 K. Three SO2 desorption centers at around 690 K, 810 K and 910 K are formed over the SO2-TPSR spectrum of the poisoned catalyst. Even at 970 K, the species contained sulfur is not desorbed completely. The amount of adsorbed NO and active intermediate--NO, species decreases over the poisoned catalyst, indicating that partial active sites are covered by the compound contained sulfur. As a result, the NO conversion ratio decreases. On the other hand, the presence of SO2 inhibits the conversion of CH4 and the compounds contained sulfur is desorbed further at higher temperature, which causes the temperature where the optimum NO conversion shifts to 823 K.

摘要

研究了在SO₂存在下,甲烷在CoH-ZSM-5上对NO的选择性催化还原。采用SO₂程序升温表面反应(SO₂-TPSR)和NO+(O₂)程序升温脱附(NO+(O₂)-TPD)技术来定量活性位点并探究中毒效应。在773 K时,添加78×10⁻⁶的SO₂,NO到N₂的转化率从72%下降并达到稳定水平58%。将反应温度提高到823 K,NO到N₂的转化率增加到62%。在773 K时,2.55%的H₂O和78×10⁻⁶的SO₂共存,NO到N₂的转化率进一步降至51%,但在873 K时几乎没有观察到影响。在中毒催化剂的SO₂-TPSR谱图上形成了三个约690 K、810 K和910 K的SO₂脱附中心。即使在970 K时,含硫物种也没有完全脱附。中毒催化剂上吸附的NO和活性中间体——NO物种的量减少,表明部分活性位点被含硫化合物覆盖。结果,NO转化率降低。另一方面,SO₂的存在抑制了CH₄的转化,并且含硫化合物在较高温度下进一步脱附,这导致最佳NO转化温度移至823 K。

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