Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective catalytic reduction of NO<sub>x</sub>

doi:10.1007/s11783-020-1337-7

Front. Environ. Sci. Eng.

2021, Vol. 15

Issue (5) : 92 https://doi.org/10.1007/s11783-020-1337-7

RESEARCH ARTICLE

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

Qiuzhun Chen¹, Xiang Zhang¹, Bing Li³, Shengli Niu¹, Gaiju Zhao⁴, Dong Wang²(

), Yue Peng³, Junhua Li³, Chunmei Lu¹, John Crittenden²

¹. National Engineering Laboratory for Coal-Burning Pollutants Emission Reduction, School of Energy and Power Engineering, Shandong University, Jinan 250061, China
². Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, 828 West Peachtree Street, Atlanta, GA 30332, USA
³. State Key Joint Laboratory of Environment Simulation and Pollution Control, National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and Equipment, School of Environment, Tsinghua University, Beijing 100084, China
⁴. Energy Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250013, China

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Abstract

• 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.

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.

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

Corresponding Author(s): Dong Wang

Issue Date: 17 December 2020

Cite this article:

Qiuzhun Chen,Xiang Zhang,Bing Li, et al. Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective catalytic reduction of NO_x[J]. Front. Environ. Sci. Eng., 2021, 15(5): 92.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1337-7
https://academic.hep.com.cn/fese/EN/Y2021/V15/I5/92

Fig.1 SCR performance of the monolithic honeycomb catalysts. (a) The monolithic honeycomb catalysts with different AC contents, (b) Reaction rate calculated at 300°C. SCR reaction conditions: [NH₃] = [NO] = 0.05%, [O₂] = 3.5%, and balanced N₂, total ﬂow rate= 2000 mL/min, and gas hourly space velocity (GHSV) = 3000 h^-¹.

Fig.2 (a) H₂-TPR profiles, (b) H₂ consumption rate vs temperature estimated during H₂-TPR, and (c) NH₃-TPD profiles of the monolithic honeycomb catalysts.

Fig.3 XRD spectra of the monolithic honeycomb catalysts.

Tab.1 Surface physical and chemical properties of the monolithic honeycomb catalysts

Fig.4 (a) Pore volume distributions, (b) Local patterns with pore size range of 1.5?4 nm, (c) Local patterns with pore size range of 4?24 nm, (d) Cumulative pore volume, (e) Cumulative pore area, and (f) N₂ adsorption-desorption isotherms of the monolithic honeycomb catalysts.

Fig.5 SEM images of the monolithic honeycomb catalysts: (a) MHRM, (b) MHRM-AC1, (c) MHRM-AC3, (d) MHRM-AC5. Elements mapping of the monolithic honeycomb catalysts: (e) MHRM, (f) MHRM-AC1, (g) MHRM-AC3, (h) MHRM-AC5.

Fig.6 XPS spectra of the monolithic honeycomb catalysts over the spectral regions of Fe 2p and O 1s.

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