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Study on the denitrification performance of FexLayOz/activated coke for NH3-SCR and the effect of CO escaped from activated coke at mid-high temperature on catalytic activity

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Abstract

Currently, activated coke is widely used in the removal of multiple pollutants from industrial flue gas. In this paper, a series of novel FexLayOz/AC catalysts was prepared by the incipient wetness impregnation for NH3-SCR denitrification reaction. The introduction of Fe-La bimetal oxides significantly improved the denitrification performance of activated coke at mid-high temperature, and 4% Fe0.3La0.7O1.5/AC exhibited a superior NOx conversion efficiency of 90.1% at 400 °C. The catalysts were further characterized by BET, SEM, XRD, Raman, EPR, XPS, FTIR, NH3-TPD, H2-TPR, et al., whose results showed that the perovskite-type oxide of LaFeO3 and oxygen vacancies were produced on the catalysts’ surfaces during roasting. Fe-La doping enhanced the amount of acid sites (mainly Lewis and other stronger acid sites) and the content of multifarious oxygen species, which were beneficial for NOx removal at mid-high temperature. Moreover, it was investigated that the effect of released CO from activated coke at mid-high temperature on the NOx removal through the lifetime test, in which it was found that a large amount of CO produced by pyrolysis of activated coke could promote the NOx removal, and long-term escaping of CO on the activated coke carrier did not have a significant negative impact on catalytic performance. The results of the TG-IR test showed that volatile matter is released from the activated coke while TG results showed that the weight loss rate of 4% Fe0.3La0.7O1.5/AC only was 0.0015~0.007%/min at 300–400 °C. Hence, 4% Fe0.3La0.7O1.5/AC had excellent thermal stability and denitrification performance to be continuously used at mid-high temperature. Finally, the mechanisms were proposed on the basis of experiments and characterization results.

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Funding

This work was financially supported by the National Key R&D Program of China (No. 2017YFC0210303), Joint Fund of the National Natural Science Foundation of China (No. U1560110), Beijing Science and Technology Project (No. D161100004516001), Beijing Nova Program (Z171100001117084), and the Open Fund of National Engineering Laboratory for Mobile Source Emission Control Technology (NELMS2017A14).

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Correspondence to Wei Su or Yi Xing.

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Responsible editor: Philippe Garrigues

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We would like to dedicate this paper to Pei Lu, who unfortunately passed away just before the paper was submitted for publication. Pei Lu played an essential role in the research described here, and he is greatly missed.

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Wang, J., Lu, P., Su, W. et al. Study on the denitrification performance of FexLayOz/activated coke for NH3-SCR and the effect of CO escaped from activated coke at mid-high temperature on catalytic activity. Environ Sci Pollut Res 26, 20248–20263 (2019). https://doi.org/10.1007/s11356-019-05090-5

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  • DOI: https://doi.org/10.1007/s11356-019-05090-5

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