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Determining hydrothermal deactivation mechanisms on Cu/SAPO-34 NH3-SCR catalysts at low- and high-reaction regions: establishing roles of different reaction sites

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Abstract

Hydrothermal deactivation is a constant challenge in commercial catalytic process aimed at NOx emission control, which may be observed in the low (150–400 °C) or high (400–550 °C)-reaction regions. To the best of our knowledge, there is a lack of systematic research regarding the correlation between the reaction sites and the mechanism of hydrothermal degradation at various reaction regions. For a targeted investigation of this, Cu/zeolite catalysts have been prepared using different amounts of polyvinyl alcohol for adjusting their redox and acid properties. These catalysts exhibit hydrothermal deactivation in different reaction regions. No change is observed in the reaction mechanism even with hydrothermal deactivation, but various reaction sites determine the performance deterioration in the low- and high-reaction regions. The redox properties and weak acid sites affect the hydrothermal deactivation in the low-reaction region, whereas the moderate/strong acid sites related to the structure mainly influence the hydrothermal deactivation in the high-reaction region. This work provides several theoretical insights for optimizing the hydrothermal stabilities of Cu/zeolite catalysts.

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摘要

高温水热老化后, 脱硝催化剂在不同反应区间(低温150–400 °C和高温 400–550 °C)表现出不同程度的性能劣化, 但目前仍缺乏对反应中心与不同反应区间高温水热失活机制关系的系统性研究. 因此, 本项工作通过不同含量的聚乙烯醇 (PVA) 来调节Cu/分子筛催化剂上氧化还原中心和酸中心的性质, 使催化剂分别在不同反应区间表现出高温水热失活. 研究结果表明, 高温水热失活未改变催化剂的反应机理, 但反应中心的性质差异造成了低温和高温反应区间不同的性能劣化情况. 氧化还原中心与弱酸中心共同导致低温反应区间的水热失活, 而与结构相关的中/强酸中心则是高温反应区间水热失活的主要原因. 本工作为优化Cu/分子筛脱硝催化剂在不同反应区间的高温水热稳定性提供了一定的理论依据.

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 22072098 and 21802099), Sichuan Science and Technology Program (No. 2021YJ0333) and the National Engineering Laboratory for Mobile Source Emission Control Technology (No. NELMS2017A06).

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Authors and Affiliations

  1. State Key Laboratory of Polymer Materials Engineering, Polymer Research Institute, Sichuan University, Chengdu, 610064, China

    Qing-Jin Lin & Yi Dan

  2. Key Laboratory of Green Chemistry and Technology, College of Chemistry, Sichuan University, Ministry of Education, Chengdu, 610064, China

    Ming-Ming Pei, Shu-Hao Xu & Yao-Qiang Chen

  3. Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu, 610064, China

    Pan Yao, Shuang Liu & Hai-Di Xu

  4. Weichai Power Co., Ltd, Weifang, 261061, China

    Shi Xu

  5. Sichuan Provincial Automobile Exhaust Purification Engineering Technology Research Center, Chengdu, 610064, China

    Hai-Di Xu & Yao-Qiang Chen

  6. Sichuan Provincial Environmental Protection Environmental Catalytic Materials Engineering Technology Center, Chengdu, 610064, China

    Hai-Di Xu & Yao-Qiang Chen

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  1. Qing-Jin Lin
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  2. Ming-Ming Pei
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  4. Shi Xu
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Lin, QJ., Pei, MM., Yao, P. et al. Determining hydrothermal deactivation mechanisms on Cu/SAPO-34 NH3-SCR catalysts at low- and high-reaction regions: establishing roles of different reaction sites. Rare Met. 41, 1899–1910 (2022). https://doi.org/10.1007/s12598-021-01933-8

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