Reaction kinetics and mechanism of CH4-SCR on Ru–In/H-SSZ-13,Catalysis Science & Technology

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Reaction kinetics and mechanism of CH4-SCR on Ru–In/H-SSZ-13
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-07-20 , DOI: 10.1039/d0cy01206h
Jun Yang _{1,

2,

3,

4} , Yupeng Chang _{1,

2,

3,

4} , Guangjun Wu _{1,

2,

3,

4} , Weili Dai _{1,

2,

3,

4} , Naijia Guan _{1,

2,

3,

4,

5} , Landong Li _{1,

2,

3,

4,

5}

Affiliation

The reaction kinetics and mechanism of CH₄-SCR on Ru–In/H-SSZ-13 as a model multifunctional catalyst, together with Ru/H-SSZ-13 and In/H-SSZ-13 for reference, were investigated. In the low-temperature region (<260 °C), quite different apparent activation energy values were obtained for the three catalysts investigated, while similar apparent activation energy values were obtained in the high-temperature region (>260 °C). With increasing reaction temperatures from 250 to 500 °C, the reaction orders of NO in CH₄-SCR on Ru–In/H-SSZ-13 gradually decreased from 1.80 to 0.43 while the reaction orders of CH₄ gradually increased from 0.33 to 0.86 instead. The surface species formed on the catalyst samples and their evolutions at 250 and 400 °C were monitored by in situ DRIFT spectroscopy. The organonitrogen compounds, i.e. methyl nitrite and its isomer nitromethane, were identified as the key intermediates in CH₄-SCR, and their existence was further confirmed by temperature-programmed surface reaction and pulse-response experiments. According to the above-mentioned results, the temperature-dependent CH₄-SCR mechanism on Ru–In/H-SSZ-13 was finally established.

中文翻译：

CH4-SCR在Ru–In / H-SSZ-13上的反应动力学及其机理

研究了CH ₄ -SCR在Ru-In / H-SSZ-13作为多功能催化剂上的反应动力学和机理，并结合Ru / H-SSZ-13和In / H-SSZ-13进行了研究。在低温区域（<260°C），对于所研究的三种催化剂获得了截然不同的表观活化能值，而在高温区域（> 260°C）获得了相似的表观活化能值。随着反应温度从250升至500°C，CH ₄ -SCR中的NO在Ru–In / H-SSZ-13上的反应顺序从1.80逐渐降低到0.43，而CH ₄的反应顺序从0.33逐渐增加到0.86代替。催化剂样品上形成的表面物质及其在250和400°C下的演变通过原位DRIFT光谱。有机氮化合物，即亚硝酸甲酯及其异构体硝基甲烷，被确定为CH ₄ -SCR的关键中间体，并通过程序升温表面反应和脉冲响应实验进一步证实了它们的存在。根据上述结果，最终建立了Ru–In / H-SSZ-13上随温度变化的CH ₄ -SCR机理。

更新日期：2020-09-05

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