Effect of surface coating CeO2 on the SO2 resistance of Cu-ZSM-5 with highly selective catalytic reduction activity

IF 1.7 4区化学 Q4 CHEMISTRY, PHYSICAL Reaction Kinetics, Mechanisms and Catalysis Pub Date : 2024-05-27 DOI:10.1007/s11144-024-02667-1

De Fang, Fenghe Sheng, Sensheng Hou, Qinglei Li, Feng He, Junlin Xie

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Abstract

Cu-ZSM-5 (Cu-Zeolite Socony Mobil-five) catalysts with different Cu loadings were prepared by ion exchange method. Different Ce loadings were coated on the surface of 0.1Cu-ZSM-5 to form CeO₂-Cu-ZSM-5 catalysts. Cu could improve the NH₃-SCR activity and broaden SCR temperature window. 0.1Cu-ZSM-5 showed the best catalytic performance (above 90%) in 200–400 ℃. 30% CeO₂-Cu-ZSM-5 catalyst was able to increase the NO conversion in the low-temperature region and keep the activity unchanged in the high-temperature region. CeO₂ that was coated on the catalysts preferentially reacted with SO₂, enhancing the excellent anti-sulfur poisoning performance. TPD, TPR, and XPS results showed that the synergistic effect of Ce and Cu increased the acidic sites and improved the redox capacity of catalysts. According to in situ DRIFTS spectra, Cu-ZSM-5 catalyst followed the Langmuir–Hinshelwood mechanism, and 30% CeO₂–0.1Cu-ZSM-5 catalyst followed not only the Langmuir–Hinshelwood mechanism but also the Eley–Rideal mechanism.

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表面镀层 CeO2 对具有高选择性催化还原活性的 Cu-ZSM-5 抗二氧化硫能力的影响

采用离子交换法制备了不同 Cu 负载的 Cu-ZSM-5（Cu-沸石 Socony Mobil-five）催化剂。在 0.1Cu-ZSM-5 表面包覆不同的 Ce，形成 CeO2-Cu-ZSM-5 催化剂。Cu 可以提高 NH3-SCR 活性并拓宽 SCR 温度窗口。0.1Cu-ZSM-5 在 200-400 ℃ 时的催化性能最好（90% 以上）。30% CeO2-Cu-ZSM-5 催化剂能够提高低温区的氮氧化物转化率，并在高温区保持活性不变。涂覆在催化剂上的 CeO2 优先与 SO2 反应，增强了催化剂优异的抗硫中毒性能。TPD、TPR 和 XPS 结果表明，Ce 和 Cu 的协同作用增加了催化剂的酸性位点，提高了催化剂的氧化还原能力。根据原位 DRIFTS 图谱，Cu-ZSM-5 催化剂遵循 Langmuir-Hinshelwood 机制，而 30% CeO2-0.1Cu-ZSM-5 催化剂不仅遵循 Langmuir-Hinshelwood 机制，还遵循 Eley-Rideal 机制。

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来源期刊

Reaction Kinetics, Mechanisms and Catalysis CHEMISTRY, PHYSICAL-

CiteScore

3.30

自引率

5.60%

发文量

201

审稿时长

2.8 months

期刊介绍： Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.