Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective catalytic reduction of NO_x

Highlights

• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst.

• The surface acidity and reducibility were highly improved, as well as the pore structure.

• The enrichment of the surface Fe²⁺ and the adsorbed oxygen account for the improvement.

Abstract

Our previous study proved that the acid-pretreatment process could efficiently activate red mud (RM) for the selective catalytic reduction (SCR) of NO_x. However, in terms of the molding process, which is the key step determining whether it can be applied in large-scale industrial, the surface acidity and reducibility of catalyst always decreased dramatically, and part of surface area and pore structure were lost. In this study, we prepared monolithic honeycomb red mud (MHRM) catalysts with activated carbon (AC) as an accelerant and investigated the effect of AC on the MHRM. The results showed that the MHRM with 3 wt.% of AC (MHRM-AC3) exhibited the best SCR performance, and kept more than 80% NO_x conversion in the range of 325°C–400°C. Compared with the MHRM, MHRM-AC1, and HMRM-AC5, the MHRM-AC3 has more mesoporous and macroporous structures, which can provide more adsorption active sites. The AC significantly improved NH₃ adsorption and surface reducibility, which was mainly due to the increase of the surface acid sites (especially the Brönsted acid sites), the concentration of Fe(II), and the surface adsorbed oxygen. The presence of more Fe(II) enriched the surface oxygen vacancies, as well as the surface adsorbed oxygen, due to the charge imbalance and unsaturated chemical bond. And surface adsorbed oxygen exhibited more active than lattice oxygen owing to its higher mobility, which was conducive to NO_x reduction in the SCR reaction.

Graphical abstract

Keywords

NO_x / Selective catalytic reduction / Iron-based catalyst / Red mud / Monolithic catalyst / Activated carbon

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Grant No. 21906090), the National Key Research and Development Program (Nos. 2017YFC0210200 and 2017YFC0212800), and Primary Research & Development Project of Shandong Province (Nos. 2018GSF117034 and 2019JZZY020305).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-020-1337-7 and is accessible for authorized users.

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