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Aluminium-induced component engineering of mesoporous composite materials for low-temperature NH₃-SCR.

ABSTRACT: Supported Mn₂O₃ is useful in achieving high dinitrogen selectivity at low temperature during ammonia-selective catalytic reduction (SCR). However, its controlled synthesis is challenging when the supporting material is the conventional pure silicon SBA-15 mesoporous molecular sieve. Here we show that silicon and aluminium in fly ash, the solid waste produced by coal-fired power plants, can be used to synthesize an Al-SBA-15 mesoporous molecular sieve support, which can guide the growth of Mn₂O₃ in the as-synthesized Fe-Mn/Al-SBA-15 NH₃-SCR catalyst. Its superior catalytic performance is demonstrated by the high NO_x conversion (≥90%) and selectivity (≥86%) at low temperatures (150-300 °C). The combined theoretical and experimental results reveal that the introduction of Al induces the growth of Mn₂O₃ catalysts. Our findings, therefore, provide a strategy for the rational design of low-temperature NH₃-SCR catalysts through dopant-induced component engineering of composite materials.

SUBMITTER: Li G

PROVIDER: S-EPMC9814655 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Aluminium-induced component engineering of mesoporous composite materials for low-temperature NH3-SCR.

Li Ge G Wang Baodong B Ma Ziran Z Wang Hongyan H Ma Jing J Zhao Chunlin C Zhou Jiali J Lin Dehai D He Faquan F Han Zhihua Z Sun Qi Q Wang Yun Y

Communications chemistry 20200527 1

Supported Mn2O3 is useful in achieving high dinitrogen selectivity at low temperature during ammonia-selective catalytic reduction (SCR). However, its controlled synthesis is challenging when the supporting material is the conventional pure silicon SBA-15 mesoporous molecular sieve. Here we show that silicon and aluminium in fly ash, the solid waste produced by coal-fired power plants, can be used to synthesize an Al-SBA-15 mesoporous molecular sieve support, which can guid ...[more]

PMID: 36703450

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Project description:The group has shown that Baiyun Ebo rare earth concentrate has excellent performance in NH3-SCR denitrification when used as a carrier, where rare earth elements are mainly present in cerium fluorocarbon ore (CeCO3F) and monazite (CePO4) mineral phases. In this paper, a new low-temperature NH3-SCR catalyst of Mn-Fe/CeCO3F-monazite was prepared by an impregnation method, using synthetic CeCO3F and purified monazite as carriers. By exploring its denitrification performance and mechanistic analysis, it provides theoretical guidance for the use of rare earth concentrates as low-temperature NH3-SCR catalysts. Our previous studies have determined the optimum loading of Fe, so this paper needs to be investigated for the optimum doping ratio of the active substance Mn. The results of the activity tests, XRD and BET have determined that the best denitrification rate and catalytic performance was achieved at a ratio of Mn : Ce of 1 : 5. The denitrification activity of the different catalysts was investigated by loading Fe, Mn and Fe and Mn together. The results obtained by means of experimental analyses such as XRD, SEM, BET and activity tests showed that the composite catalyst loaded with Fe and Mn at the same time, had the highest activity and its denitrification rate could reach 94.8% at 250 °C. This is mainly attributed to the fact that the interaction of Fe, Mn can promote the dispersion of each other on the carrier surface, which greatly improves the specific surface area of the catalyst. The introduction of Fe and Mn increases the acidic sites and the amount of acid on the catalyst surface, which results in the formation of a large number of oxygen vacancies and the presence of more oxygen species on the catalyst surface, which facilitate the migration of oxygen. The new catalyst was investigated by Fourier transform infrared (FTIR) spectroscopy to characterise the adsorption and transformation behaviour of the reactive species on the surface of the catalyst, and to investigate the reaction mechanism. The results showed that the entire reaction process followed the L-H mechanism, with the gaseous NO adsorption and activation on the catalyst surface generating bidentate nitrate, bridging nitrate species and NH3/NH4 + species as the main intermediate species involved in the reaction, both of which underwent redox reactions on the catalyst surface to produce N2 and H2O. The above results indicated that the CeCO3F-monazite carrier has excellent performance, and provided a theoretical basis for the high-value utilization of rare earth concentrates.

Dataset Information

Aluminium-induced component engineering of mesoporous composite materials for low-temperature NH₃-SCR.

Publications

Aluminium-induced component engineering of mesoporous composite materials for low-temperature NH<sub>3</sub>-SCR.

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