Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature
Manganese alumina composited oxides (MnAlO<i><sub>x</sub></i>) catalysts with ordered mesoporous structure prepared by evaporation-induced self-assembly (EISA) method was designed for the selective catalytic reduction (SCR) of NO<i><sub>x</sub></i> wit...
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2022-06-01
|
| Series: | Catalysts |
| Subjects: | |
| Online Access: | https://www.mdpi.com/2073-4344/12/6/637 |
| _version_ | 1797489043382992896 |
|---|---|
| author | Qixiong Hou Yongjin Liu Yaqin Hou Xiaojin Han Zhanggen Huang |
| author_facet | Qixiong Hou Yongjin Liu Yaqin Hou Xiaojin Han Zhanggen Huang |
| author_sort | Qixiong Hou |
| collection | DOAJ |
| description | Manganese alumina composited oxides (MnAlO<i><sub>x</sub></i>) catalysts with ordered mesoporous structure prepared by evaporation-induced self-assembly (EISA) method was designed for the selective catalytic reduction (SCR) of NO<i><sub>x</sub></i> with NH<sub>3</sub> at low temperature. The effect of calcination temperature of MnAlO<i><sub>x</sub></i> catalysts was investigated systematically, and it was correlated with SCR activity. Results showed that with an increase in calcination temperature, the SCR activity of MnAlO<i><sub>x</sub></i> catalysts increased. When the calcination temperature was raised up to 800 °C, the NO<i><sub>x</sub></i> conversion was more than 90% in the operation temperature range of 150~240 °C. Through various characterization analysis, it was found that MnAlO<i><sub>x</sub></i>-800 °C catalysts possessed enhanced redox capacities as the higher content of Mn<sup>4+</sup>/(Mn<sup>3+</sup> + Mn<sup>4+</sup>). Moreover, the improved redox properties could contribute to a higher NO<i><sub>x</sub></i> adsorption and activation ability, which lead to higher SCR performance of MnAlO<i><sub>x</sub></i>-800 °C catalysts. In situ DRIFTs revealed that the adsorbed NO<sub>2</sub> and bidentate nitrate are the reactive intermediate species, and NH<sub>3</sub> species bonded to Lewis acid sites taken part in SCR progress. The SCR progress predominantly followed E–R mechanism, while L–H mechanism also takes effect to a certain degree. |
| first_indexed | 2024-03-10T00:10:54Z |
| format | Article |
| id | doaj.art-3390e49508bf4ecca6a8e168cc3576d5 |
| institution | Directory Open Access Journal |
| issn | 2073-4344 |
| language | English |
| last_indexed | 2024-03-10T00:10:54Z |
| publishDate | 2022-06-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Catalysts |
| spelling | doaj.art-3390e49508bf4ecca6a8e168cc3576d52023-11-23T15:59:46ZengMDPI AGCatalysts2073-43442022-06-0112663710.3390/catal12060637Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low TemperatureQixiong Hou0Yongjin Liu1Yaqin Hou2Xiaojin Han3Zhanggen Huang4State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, ChinaManganese alumina composited oxides (MnAlO<i><sub>x</sub></i>) catalysts with ordered mesoporous structure prepared by evaporation-induced self-assembly (EISA) method was designed for the selective catalytic reduction (SCR) of NO<i><sub>x</sub></i> with NH<sub>3</sub> at low temperature. The effect of calcination temperature of MnAlO<i><sub>x</sub></i> catalysts was investigated systematically, and it was correlated with SCR activity. Results showed that with an increase in calcination temperature, the SCR activity of MnAlO<i><sub>x</sub></i> catalysts increased. When the calcination temperature was raised up to 800 °C, the NO<i><sub>x</sub></i> conversion was more than 90% in the operation temperature range of 150~240 °C. Through various characterization analysis, it was found that MnAlO<i><sub>x</sub></i>-800 °C catalysts possessed enhanced redox capacities as the higher content of Mn<sup>4+</sup>/(Mn<sup>3+</sup> + Mn<sup>4+</sup>). Moreover, the improved redox properties could contribute to a higher NO<i><sub>x</sub></i> adsorption and activation ability, which lead to higher SCR performance of MnAlO<i><sub>x</sub></i>-800 °C catalysts. In situ DRIFTs revealed that the adsorbed NO<sub>2</sub> and bidentate nitrate are the reactive intermediate species, and NH<sub>3</sub> species bonded to Lewis acid sites taken part in SCR progress. The SCR progress predominantly followed E–R mechanism, while L–H mechanism also takes effect to a certain degree.https://www.mdpi.com/2073-4344/12/6/637ordered mesoporous MnAlO<i><sub>x</sub></i>calcination temperatureSCRlow temperature |
| spellingShingle | Qixiong Hou Yongjin Liu Yaqin Hou Xiaojin Han Zhanggen Huang Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature Catalysts ordered mesoporous MnAlO<i><sub>x</sub></i> calcination temperature SCR low temperature |
| title | Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature |
| title_full | Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature |
| title_fullStr | Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature |
| title_full_unstemmed | Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature |
| title_short | Ordered Mesoporous MnAlO<i><sub>x</sub></i> Oxides Dominated by Calcination Temperature for the Selective Catalytic Reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> at Low Temperature |
| title_sort | ordered mesoporous mnalo i sub x sub i oxides dominated by calcination temperature for the selective catalytic reduction of no i sub x sub i with nh sub 3 sub at low temperature |
| topic | ordered mesoporous MnAlO<i><sub>x</sub></i> calcination temperature SCR low temperature |
| url | https://www.mdpi.com/2073-4344/12/6/637 |
| work_keys_str_mv | AT qixionghou orderedmesoporousmnaloisubxsubioxidesdominatedbycalcinationtemperaturefortheselectivecatalyticreductionofnoisubxsubiwithnhsub3subatlowtemperature AT yongjinliu orderedmesoporousmnaloisubxsubioxidesdominatedbycalcinationtemperaturefortheselectivecatalyticreductionofnoisubxsubiwithnhsub3subatlowtemperature AT yaqinhou orderedmesoporousmnaloisubxsubioxidesdominatedbycalcinationtemperaturefortheselectivecatalyticreductionofnoisubxsubiwithnhsub3subatlowtemperature AT xiaojinhan orderedmesoporousmnaloisubxsubioxidesdominatedbycalcinationtemperaturefortheselectivecatalyticreductionofnoisubxsubiwithnhsub3subatlowtemperature AT zhanggenhuang orderedmesoporousmnaloisubxsubioxidesdominatedbycalcinationtemperaturefortheselectivecatalyticreductionofnoisubxsubiwithnhsub3subatlowtemperature |