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

Qiuzhun Chen, Xiang Zhang, Bing Li, Shengli Niu, Gaiju Zhao, Dong Wang, Yue Peng, Junhua Li, Chunmei Lu, John Crittenden

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Front. Environ. Sci. Eng. ›› 2021, Vol. 15 ›› Issue (5) : 92. DOI: 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 NOx

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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 NOx. 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% NOx 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 NOx reduction in the SCR reaction.

Graphical abstract

Keywords

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

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Qiuzhun Chen, Xiang Zhang, Bing Li, Shengli Niu, Gaiju Zhao, Dong Wang, Yue Peng, Junhua Li, Chunmei Lu, John Crittenden. Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective catalytic reduction of NOx. Front. Environ. Sci. Eng., 2021, 15(5): 92 https://doi.org/10.1007/s11783-020-1337-7

References

[1]
Boningari T, Ettireddy P R, Somogyvari A, Liu Y, Vorontsov A, McDonald C A, Smirniotis P G (2015). Influence of elevated surface texture hydrated titania on Ce-doped Mn/TiO2 catalysts for the low-temperature SCR of NOx under oxygen-rich conditions. Journal of Catalysis, 325: 145–155
CrossRef Google scholar
[2]
Black L, Garbev K, Stemmermann P, Hallam K R, Allen G C (2003). Characterisation of crystalline C-S-H phases by X-ray photoelectron spectroscopy. Cement and Concrete Research, 33(6): 899–911
CrossRef Google scholar
[3]
Cartwright R, Esconjauregui S, Hardeman D, Bhardwaj S, Weatherup R, Guo Y, D’Arsié L, Bayer B, Kidambi P, Hofmann S, Wright E, Clarke J, Oakes D, Cepek C, Robertson J (2015). Low temperature growth of carbon nanotubes on tetrahedral amorphous carbon using Fe-Cu catalyst. Carbon, 81(1): 639–649
CrossRef Google scholar
[4]
Chang H Z, Zhang T, Dang H, Chen X Y, You Y C, Schwank J W, Li J H (2018). Fe2O3@SiTi core-shell catalyst for the selective catalytic reduction of NOx with NH3: Activity improvement and HCl tolerance. Catalysis Science & Technology, 8(13): 3313–3320
CrossRef Google scholar
[5]
Chen K G, Chen R Y, Cang H, Mao A R, Tang Z, Xu Q (2018). Plasma-treated Ce/TiO2-SiO2 catalyst for the NH3-SCR of NOx. Environmental Technology, 39(14): 1753–1764
CrossRef Google scholar
[6]
Chen L, Wang X X, Cong Q L, Ma H Y, Li S J, Li W (2019). Design of a hierarchical Fe-ZSM-5@CeO2 catalyst and the enhanced performances for the selective catalytic reduction of NO with NH3. Chemical Engineering Journal, 369: 957–967
CrossRef Google scholar
[7]
Feng G R, Qi T Y, Guo Y X, Bai J W, Guo J (2020). Physical and chemical characterization of the ash of fallen chinese willow leaves: effects of calcination temperature and aqueous solution. Combustion Science and Technology, 192(5): 871–884
CrossRef Google scholar
[8]
Flink A, Larsson T, Sjölén J, Karlsson L, Hultman L (2005). Influence of Si on the microstructure of arc evaporated (Ti, Si)N thin films; evidence for cubic solid solutions and their thermal stability. Surface and Coatings Technology, 200(5-6): 1535–1542
CrossRef Google scholar
[9]
Gao C, Yang G P, Wang D, Gong Z Q, Zhang X, Wang B, Peng Y, Li J H, Lu C M, Crittenden J (2020). Modified red mud catalyst for the selective catalytic reduction of nitrogen oxides: Impact mechanism of cerium precursors on surface physicochemical properties. Chemosphere, 257: 127215
CrossRef Google scholar
[10]
Gong Z Q, Ma J, Wang D, Niu S L, Yan B H, Shi Q L, Lu C M, Crittenden J (2020). Insights into modified red mud for the selective catalytic reduction of NOx: Activation mechanism of targeted leaching. Journal of Hazardous Materials, 394: 122536
CrossRef Google scholar
[11]
Han F, Xu C N, Wei W, Zhang F, Xu P, Zhong Z X, Xing W H (2018). Corrosion behaviors of porous reaction-bonded silicon carbide ceramics incorporated with CaO. Ceramics International, 44(11): 12225–12232
CrossRef Google scholar
[12]
Han J, Zhang D S, Maitarad P, Shi L Y, Cai S X, Li H R, Huang L, Zhang J P (2015). Fe2O3 nanoparticles anchored in situ on carbon nanotubes via an ethanol-thermal strategy for the selective catalytic reduction of NO with NH3. Catalysis Science & Technology, 5(1): 438–446
CrossRef Google scholar
[13]
Husnain N, Wang E L, Fareed S, Tuoqeer Anwar M (2019). Comparision on the low-temperature NH3-SCR performance of g-Fe2O3 catalysts prepared by two different methods. Catalysts, 9(12): 1018
CrossRef Google scholar
[14]
Jo M R, Heo Y U, Lee Y C, Kang Y M (2014). A nano-Si/FeSi2Ti hetero-structure with structural stability for highly reversible lithium storage. Nanoscale, 6(2): 1005–1010
CrossRef Google scholar
[15]
Li Z H, Geng Y, Ma L, Chen X Y, Li J H, Chang H Z, Schwank J W (2020). Catalytic oxidation of CO over Pt/Fe3O4 catalysts: Tuning O2 activation and CO adsorption. Frontiers of Environmental Science & Engineering, 14(4): 65
CrossRef Google scholar
[16]
Liu J X, Zhao Z, Xu C M, Liu J (2019a). Structure, synthesis, and catalytic properties of nanosize cerium-zirconium-based solid solutions in environmental catalysis. Chinese Journal of Catalysis, 40(10): 1438–1487
CrossRef Google scholar
[17]
Liu J X, Liu J, Zhao Z, Wei Y C, Song W Y (2017a). Fe-Beta@CeO2 core-shell catalyst with tunable shell thickness for selective catalytic reduction of NOx with NH3. AIChE Journal. American Institute of Chemical Engineers, 63(10): 4430–4441
CrossRef Google scholar
[18]
Liu J X, Liu J, Zhao Z, Tan J B, Wei Y C, Song W Y (2018). Fe/Beta@SBA-15 core-shell catalyst: Interface stable effect and propene poisoning resistance for NO abatement. AIChE Journal. American Institute of Chemical Engineers, 64(11): 3967–3978
CrossRef Google scholar
[19]
Liu J X, Liu J, Zhao Z, Wei Y C, Song W Y, Li J M, Zhang X (2017b). A unique Fe/Beta@TiO2 core-shell catalyst by small-grain molecular sieve as the core and TiO2 nano-size thin film as the shell for the removal of NOx. Industrial & Engineering Chemistry Research, 56(20): 5833–5842
CrossRef Google scholar
[20]
Liu J X, Cheng H F, Tan J B, Liu B, Zhang Z H, Xu H D, Zhao M J, Zhu W S, Liu J, Zhao Z (2020). Solvent-free rapid synthesis of porous CeWOx by mechanochemical self-assembly strategy for the abatement of NOx. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 8(14): 6717–6731
CrossRef Google scholar
[21]
Liu X S, Chen H F, Wu X D, Cao L, Jiang P, Yu Q F, Ma Y (2019b). Effects of SiO2 modification on the hydrothermal stability of the V2O5/WO3-TiO2 NH3-SCR catalyst: TiO2 structure and vanadia species. Catalysis Science & Technology, 9(14): 3711–3720
CrossRef Google scholar
[22]
Liu Z M, Su H, Chen B H, Li J H, Woo S I (2016). Activity enhancement of WO3 modified Fe2O3 catalyst for the selective catalytic reduction of NOx by NH3. Chemical Engineering Journal, 299: 255–262
CrossRef Google scholar
[23]
Lyu Z K, Niu S L, Lu C M, Zhao G J, Gong Z Q, Zhu Y (2020). A density functional theory study on the selective catalytic reduction of NO by NH3 reactivity of a-Fe2O3 (0 0 1) catalyst doped by Mn, Ti, Cr and Ni. Fuel, 267: 117147
CrossRef Google scholar
[24]
Matsui Y, Nakao S, Sakamoto A, Taniguchi T, Pan L, Matsushita T, Shirasaki N (2015). Adsorption capacities of activated carbons for geosmin and 2-methylisoborneol vary with activated carbon particle size: Effects of adsorbent and adsorbate characteristics. Water Research, 85: 95–102
CrossRef Google scholar
[25]
Mukherjee D, Rao B G, Reddy B M (2016). CO and soot oxidation activity of doped ceria: Influence of dopants. Applied Catalysis B: Environmental, 197: 105–115
CrossRef Google scholar
[26]
Mu W T, Zhu J, Zhang S, Guo Y Y, Su L Q, Li X Y, Li Z (2016). Novel proposition on mechanism aspects over Fe-Mn/ZSM-5 catalyst for NH3-SCR of NOx at low temperature: Rate and direction of multifunctional electron-transfer-bridge and in-situ DRIFTs analysis. Catalysis Science & Technology, 6(20): 7532–7548
CrossRef Google scholar
[27]
Ni Z J, Qin H F, Kang S F, Bai J R, Wang Z L, Li Y G, Zheng Z, Li X (2018). Effect of graphitic carbon modification on the catalytic performance of Fe@SiO2-GC catalysts for forming lower olefins via Fischer-Tropsch synthesis. Journal of Colloid and Interface Science, 516: 16–22
CrossRef Google scholar
[28]
Ren B, Liu J J, Wang Y L, Chen Y G, Gan K, Rong Y D, Yang J L (2019). Hierarchical cellular scaffolds fabricated via direct foam writing using gelled colloidal particle-stabilized foams as the ink. Journal of the American Ceramic Society, 102(11): 6498–6506
CrossRef Google scholar
[29]
Subramanian V, Ordomsky V V, Legras B, Cheng K, Cordier C, Chernavskii P A, Khodakov A Y (2016). Design of iron catalysts supported on carbon-silica composites with enhanced catalytic performance in high-temperature Fischer-Tropsch synthesis. Catalysis Science & Technology, 6(13): 4953–4961
CrossRef Google scholar
[30]
Schill L, Putluru S S R, Fehrmann R, Jensen A D (2014). Low-temperature NH3–SCR of NO on mesoporous Mn0.6Fe0.4/TiO2 prepared by a hydrothermal method. Catalysis Letters, 144(3): 395–402
CrossRef Google scholar
[31]
Sun F W, Liu H B, Shu D B, Chen T H, Chen D (2019). The characterization and SCR performance of Mn-containing a-Fe2O3 derived from the decomposition of siderite. Minerals (Basel), 9(7): 393
CrossRef Google scholar
[32]
Wang B, Ma J, Wang D, Gong Z Q, Shi Q L, Gao C, Lu C M, Crittenden J (2020). Acid-pretreated red mud for selective catalytic reduction of NOx with NH3: Insights into inhibition mechanism of binders. Catalysis Today,
CrossRef Google scholar
[33]
Wang C, Wang J, Wang J Q, Shen M Q (2021). Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe/Beta catalysts. Frontiers of Environmental Science & Engineering, 15(2): 30
CrossRef Google scholar
[34]
Wu J K, Gong Z Q, Lu C M, Niu S L, Ding K, Xu L T, Zhang K (2018). Preparation and performance of modified red mud-based catalysts for selective catalytic reduction of NOx with NH3. Catalysts, 8(1): 35
CrossRef Google scholar
[35]
Xie A J, Tang Y R, Huang X Y, Jin X, Gu P F, Luo S P, Yao C, Li X Z (2019). Three-dimensional nanoflower MnCrOx/Sepiolite catalyst with increased SO2 resistance for NH3-SCR at low temperature. Chemical Engineering Journal, 370: 897–905
CrossRef Google scholar
[36]
Xiong Z B, Liu J, Zhou F, Liu D Y, Lu W, Jin J, Ding S F (2017). Selective catalytic reduction of NOx with NH3 over iron-ceriumtungsten mixed oxide catalyst prepared by different methods. Applied Surface Science, 406: 218–225
CrossRef Google scholar
[37]
Xu L T, Niu S L, Lu C M, Wang D, Zhang K, Li J (2017). NH3-SCR performance and characterization over magnetic iron-magnesium mixed oxide catalysts. Korean Journal of Chemical Engineering, 34(5): 1576–1583
CrossRef Google scholar
[38]
Yao X J, Chen L, Kong T T, Ding S M, Luo Q, Yang F M (2017). Support effect of the supported ceria-based catalysts during NH3-SCR reaction. Chinese Journal of Catalysis, 38(8): 1423–1430
CrossRef Google scholar
[39]
Yang J, Ren S, Zhang T S, Su Z H, Long H M, Kong M, Yao L (2020). Iron doped effects on active sites formation over activated carbon supported Mn-Ce oxide catalysts for low-temperature SCR of NO. Chemical Engineering Journal, 379: 122398
CrossRef Google scholar
[40]
Yang Q L, Wang D, Wang C Z, Li K Z, Peng Y, Li J H (2018). Promotion effect of Ga-Co spinel derived from layered double hydroxides for toluene oxidation. ChemCatChem, 10(21): 4838–4843
CrossRef Google scholar
[41]
Yang S J, Wang C Z, Ma L, Peng Y, Qu Z, Yan N Q, Chen J H, Chang H Z, Li J H (2013). Substitution of WO3 in V2O5/WO3-TiO2 by Fe2O3 for selective catalytic reduction of NO with NH3. Catalysis Science & Technology, 3(1): 161–168
CrossRef Google scholar
[42]
Zhan S H, Qiu M Y, Yang S S, Zhu D D, Yu H B, Li Y (2014). Facile preparation of MnO2 doped Fe2O3 hollow nanofibers for low temperature SCR of NO with NH3. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2(48): 20486–20493
CrossRef Google scholar
[43]
Zhao K, Han W L, Tang Z C, Lu J Y, Hu X (2018). High-efficiency environmental-friendly Fe-W-Ti catalyst for selective catalytic reduction of NO with NH3: The structure-activity relationship. Catalysis Surveys from Asia, 22(1): 20–30
CrossRef Google scholar

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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