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Unveiling H2O2-optimized NOx adsorption-selective catalytic reduction (AdSCR) performance of WO3/CeZrO2 catalyst

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Abstract

Recently, NOx emissions in the cold-start period have been a great challenge in eliminating diesel vehicle exhaust. In this study, a type of NOx adsorption-selective catalytic reduction (AdSCR) bifunctional catalyst was developed to remove NOx in the cold-start period by constructing additional NOx adsorption sites on the surface of the selective catalytic reduction of NOx with NH3 catalyst. The AdSCR catalyst exhibited both NOx adsorption–storage performance and NH3-SCR activity. The amount of oxygen vacancies directly affected the adsorption performance of NOx on the catalyst surface. In this study, H2O2 with different pH values was employed to adjust the electronic structure of the CeZrO2 support and construct oxygen vacancies on the surface of CeZrO2, which contributed to improving NOx adsorption and storage on the WO3/CeZrO2 (W/CZ) catalyst below 200 °C. The catalytic performance results show that CZ supports modified by alkaline H2O2 rather than acidic and neutral H2O2 significantly improve the NOx adsorption capacity without decreasing the NH3-SCR activity. The characterization results show that the CZ support modified by alkaline H2O2 possesses more surface oxygen vacancies and chemisorbed oxygen than CZ supports modified by acidic and neutral H2O2. Oxygen vacancies are not only the active sites of NH3-SCR, but also the active sites of NOx adsorption. Therefore, the W/CZ catalyst modified by alkaline H2O2 exhibited an excellent AdSCR performance. This study proposes a novel perspective to address the issue of NOx emissions from diesel vehicles during the cold start period.

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摘要

近年来, 减少冷启动阶段的NOx排放是柴油车尾气面临的一大挑战。本研究开发了一种NOx吸附-选择性催化还原 (AdSCR) 双功能催化剂, 通过在NH3选择性催化还原NOx(NH3-SCR) 催化剂的表面上构建额外的NOx吸附位点, 从而在冷启动阶段去除NOx。AdSCR催化剂同时具有NOx吸附-储存性能和NH3-SCR活性。氧空位的数量直接影响NOx在催化剂表面上的吸附-储存性能。该工作采用不同pH值的H2O2调节CeZrO2 (CZ) 载体的电子结构, 并在CeZrO2表面上构建氧空位, 这有助于改善WO3/CeZrO2催化剂在低于200 °C时的NOx吸附-储存性能。催化性能的结果表明, 与酸性和中性H2O2改性的CZ载体相比, 碱性H2O2改性的CZ载体在不降低NH3-SCR活性的基础上显著提高了NOx吸附能力。表征结果表明, 与酸性和中性H2O2改性的CZ载体相比, 碱性H2O2改性的CZ载体具有更多的表面氧空位和化学吸附氧。氧空位不仅是NH3-SCR的活性位点, 也是NOx吸附的活性位点。因此, 碱性H2O2改性的W/CZ催化剂显示出优异的AdSCR性能。该工作为解决柴油车在冷启动阶段NOx排放问题提出了一个新的思路。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (No. 22072098) and Sichuan Science and Technology Program (No. 2022ZHCG0125).

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Authors and Affiliations

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

    Yan Huang, Shuang Liu, Jia-Yi Li & Hai-Di Xu

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

    Ming-Ming Pei & Yao-Qiang Chen

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

    Hai-Di Xu & Yao-Qiang Chen

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

    Hai-Di Xu & Yao-Qiang Chen

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Huang, Y., Liu, S., Pei, MM. et al. Unveiling H2O2-optimized NOx adsorption-selective catalytic reduction (AdSCR) performance of WO3/CeZrO2 catalyst. Rare Met. 42, 3755–3765 (2023). https://doi.org/10.1007/s12598-023-02369-y

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