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Application of silica-alumina as hydrothermally stable supports for Pt catalysts for acid-assisted soot oxidation

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Abstract

In this work, silica-alumina mixed oxides with different SiO2 contents (5% and 30%) were adopted as acidic supports for platinum catalysts for soot oxidation. The obtained catalysts were hydrothermally aged in 10% H2O/air at 750 °C for 20 h. The catalysts were characterized by X-ray diffraction (XRD), N2 adsorption, inductively coupled plasma (ICP), CO chemisorption, NH3 temperature-programmed desorption (TPD), infrared (IR) spectroscopy of CO adsorption, temperature-programmed oxidation (TPO) of NO, and TPD of NOx. The surface acidity of catalyst was positive correlated with the content of SiO2, which kept platinum in metallic and partially oxidized states in an oxidizing atmosphere. Compared with sulfation treatment on the alumina support, the application of SiO2–Al2O3 mixed oxides does not result in the coverage of Pt active sites and the prepared catalysts exhibit excellent activity for NO oxidation. They promote NOx preferential adsorption on soot and decomposition of surface oxygenated compounds (SOCs) as the sulfated Pt/Al2O3 catalyst does.

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摘要

采用不同二氧化硅质量含量（5% 和 30%）的硅铝复合氧化物作为铂基碳烟氧化催化剂的酸性载体，并将制得的催化剂在 750 °C含 10% 水蒸气的空气中水热老化 20 h。对催化剂进行了 X 射线衍射 (XRD)、氮气吸附、电感耦合等离子体 (ICP)、一氧化碳化学吸附、氨气程序升温脱附 (TPD)、一氧化碳吸附红外 (IR) 光谱、一氧化氮程序升温氧化 (TPO) 和 氮氧化物程序升温脱附 (TPD) 表征。结果发现催化剂的表面酸性与SiO2含量正相关，其促使铂在氧化气氛中保持金属态和部分氧化态。与磺化处理的氧化铝负载铂催化剂相比，采用硅铝复合氧化物载体不会导致铂活性位点被覆盖，所制备的催化剂表现出优异的一氧化氮氧化活性，并促进氮氧化物在碳烟表面的选择性吸附和碳烟表面含氧化合物 (SOCs) 的分解。

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Acknowledgements

This study was financially supported by the National Key R&D Program of China (No. 2017YFC0211102), the National Natural Science Foundation of China (No. 21906091) and the Mobile Source Emission Control Technology (No. NELMS2020A08).

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Author notes

  1. Shu-Ran Liu and Shu-Ting Luo have contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Advanced Materials of Ministry of Education of China, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China

    Shu-Ran Liu, Shu-Ting Luo, Xiao-Dong Wu, Tao-Jin Wang, Rui Ran & Duan Weng

  2. International Graduate School at Shenzhen, Tsinghua University, Shenzhen, 518055, China

    Zhi-Chun Si

  3. School of Materials Science and Engineering, Ocean University of China, Qingdao, 266100, China

    Shuang Liu

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Liu, SR., Luo, ST., Wu, XD. et al. Application of silica-alumina as hydrothermally stable supports for Pt catalysts for acid-assisted soot oxidation. Rare Met. 42, 1614–1623 (2023). https://doi.org/10.1007/s12598-022-02199-4

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