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Evolution mechanism of active sites for selective catalytic reduction of NOx with NH3 over Fe-ZSM-5 catalysts doped by Ce/Cu

Ce/Cu掺杂Fe-ZSM-5 催化剂NH3选择性催化还原NOx的活性位点演化机理

  • The 2nd World Congress on Internal Combustion Engines
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Abstract

Fe-ZSM-5 catalysts modified by Cu and Ce by aqueous solution ion-exchange and incipient wetness impregnation methods were tested in the selective catalytic reduction of NOx with NH3. A variety of characterization techniques (NH3-SCO, BET, XRD, XPS, UV-Vis, NH3-TPD, H2-TPR) were used to explore the changes of the active sites, acid sites and pore structure of the catalyst. It was found that the dispersion of active Cu species and Fe species had great influences on the catalytic activity in the whole catalytic process. The Cu doping into the Fe-ZSM-5 catalyst produced new active species, isolated Cu ions and CuO particles, resulting in the improved low-temperature catalytic activity. However, the NH3 oxidation was enhanced, and part of the Fe3+ active sites and more Brønsted acidic sites in the catalyst were occupied by Cu species, which causes the decrease of the high-temperature activity. The recovery of high-temperature activity could be attributed to the recovery of active Cu species and Fe species promoted by Ce and the promotion of active species dispersion. The results provide theoretical support for adjusting the active window of Fe-based SCR catalyst by multi-metal doping.

摘要

通过水溶液离子交换法和初湿浸渍法制备Cu和Ce改性的Fe-ZSM-5催化剂,研究其在NH3选择 性催化还原NOx中的作用。通过表征技术(NH3-SCO,BET,XRD,XPS,UV-Vis,NH3-TPD,H2-TPR) 探讨了催化剂活性位、酸性位和孔结构的变化,发现活性Cu物种和Fe 物种的分散情况是影响整个催 化过程中催化活性的重要因素。Fe-ZSM-5 催化剂中Cu 的掺杂带来了新的活性物种,孤立Cu 离子和 CuO颗粒,从而改善了低温催化活性。然而,催化剂的氨氧化作用也随之加强,催化剂中的部分Fe3+ 活性位和Brønsted 酸性位被Cu物种取代,这导致了高温活性的降低。进一步掺杂Ce 后,高温活性得 到恢复,可以归因于Ce 促进了活性Cu 物种和Fe 物种的高度分散。这些发现为多金属掺杂调节铁基 SCR催化剂的活性窗口提供了理论支持。

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Authors and Affiliations

  1. School of Automotive and Traffic Engineering, Jiangsu University, Zhenjiang, 212013, China

    Yu-bo Zhang  (张宇博), Pan Wang  (王攀), Dan Yu  (于丹), Hong-yu Zhao  (赵虹钰), Xing-lei Lyu  (吕星磊) & Li-li Lei  (雷利利)

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  1. Yu-bo Zhang  (张宇博)
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Contributions

The overarching research goals were developed by ZHANG Yu-bo, WANG Pan, and YU Dan. ZHANG Yu-bo and YU Dan analyzed the measured data. ZHAO Hong-yu and LYU Xing-lei analyzed the results. The initial draft of the manuscript was written by ZHANG Yu-bo and WANG Pan. All authors replied to reviewers’ comments and revised the final version.

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Correspondence to Pan Wang  (王攀).

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Conflict of interest

ZHANG Yu-bo, WANG Pan, YU Dan, ZHAO Hong-yu, LYU Xing-lei, LEI Li-li declare that they have no conflict of interest.

Foundation item: Project(51906089) supported by the National Natural Science Foundation of China; Project(NELMS2018A18) supported by the National Engineering Laboratory for Mobile Source Emission Control Technology, China: Project(XNYQ2021-002) supported by the Provincial Engineering Research Center for New Energy Vehicle Intelligent Control and Simulation Test Technology of Sichuan, China; Project(GY2020016) supported by the Zhenjiang City Key R&D Program, China

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Zhang, Yb., Wang, P., Yu, D. et al. Evolution mechanism of active sites for selective catalytic reduction of NOx with NH3 over Fe-ZSM-5 catalysts doped by Ce/Cu. J. Cent. South Univ. 29, 2239–2252 (2022). https://doi.org/10.1007/s11771-022-5077-7

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