MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance
The ethanol dispersion method was employed to synthesize a series of MnO<sub>x</sub>/SAPO-34 catalysts using SAPO-34 with the hierarchical pore structure as the zeolite carrier, which were prepared by facile acid treatment with citric acid. Physicochemical properties of catalysts were ch...
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MDPI AG
2021-02-01
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| Online Access: | https://www.mdpi.com/2073-4344/11/3/314 |
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| author | Lusha Zhou Jinkun Guan Chenglong Yu Bichun Huang |
| author_facet | Lusha Zhou Jinkun Guan Chenglong Yu Bichun Huang |
| author_sort | Lusha Zhou |
| collection | DOAJ |
| description | The ethanol dispersion method was employed to synthesize a series of MnO<sub>x</sub>/SAPO-34 catalysts using SAPO-34 with the hierarchical pore structure as the zeolite carrier, which were prepared by facile acid treatment with citric acid. Physicochemical properties of catalysts were characterized by XRD, XPS, BET, TEM, NH<sub>3</sub>-TPD, SEM, FT-IR, Py-IR, H<sub>2</sub>-TRP and TG/DTG. NH<sub>3</sub>-SCR performances of the hierarchical MnO<sub>x</sub>/SAPO-34 catalysts were evaluated at low temperatures. Results show that citric acid etching solution at a concentration of 0.1 mol/L yielded a hierarchical MnO<sub>x</sub>/SAPO-34-0.1 catalyst with <i>ca</i>.15 wt.% Mn loading, exhibiting optimal catalytic activity and SO<sub>2</sub> tolerance at low temperatures. Almost 100% NO conversion and over 90% N<sub>2</sub> selectivity at 120 °C under a gas hourly space velocity (GHSV) of 40,000 h<sup>−1</sup> could be obtained over this sample. Furthermore, the NO conversion was still higher than 65% when 100 ppm SO<sub>2</sub> was introduced to the reaction gas for 4 h. These could be primarily attributed to the large specific surface area, high surface acidity concentration and abundant chemisorbed oxygen species provided by the hierarchical pore structure, which could also increase the mass transfer of the reaction gas. This finding suggests that the NH<sub>3</sub>-SCR activity and SO<sub>2</sub> poisoning tolerance of hierarchical MnO<sub>x</sub>/SAPO-34 catalysts at low temperatures can be improved by controlling the morphology of the catalysts, which might supply a rational strategy for the design and synthesis of Mn-based SCR catalysts. |
| first_indexed | 2024-03-09T06:18:47Z |
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| last_indexed | 2024-03-09T06:18:47Z |
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| spelling | doaj.art-6ae7c79c94a240759f85eab2b55159752023-12-03T11:49:34ZengMDPI AGCatalysts2073-43442021-02-0111331410.3390/catal11030314MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> ResistanceLusha Zhou0Jinkun Guan1Chenglong Yu2Bichun Huang3Guangzhou Higher Education Mega Centre, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaGuangzhou Higher Education Mega Centre, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaSchool of Land Resources and Environment, Jiangxi Agricultural University, Nanchang 330045, ChinaGuangzhou Higher Education Mega Centre, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaThe ethanol dispersion method was employed to synthesize a series of MnO<sub>x</sub>/SAPO-34 catalysts using SAPO-34 with the hierarchical pore structure as the zeolite carrier, which were prepared by facile acid treatment with citric acid. Physicochemical properties of catalysts were characterized by XRD, XPS, BET, TEM, NH<sub>3</sub>-TPD, SEM, FT-IR, Py-IR, H<sub>2</sub>-TRP and TG/DTG. NH<sub>3</sub>-SCR performances of the hierarchical MnO<sub>x</sub>/SAPO-34 catalysts were evaluated at low temperatures. Results show that citric acid etching solution at a concentration of 0.1 mol/L yielded a hierarchical MnO<sub>x</sub>/SAPO-34-0.1 catalyst with <i>ca</i>.15 wt.% Mn loading, exhibiting optimal catalytic activity and SO<sub>2</sub> tolerance at low temperatures. Almost 100% NO conversion and over 90% N<sub>2</sub> selectivity at 120 °C under a gas hourly space velocity (GHSV) of 40,000 h<sup>−1</sup> could be obtained over this sample. Furthermore, the NO conversion was still higher than 65% when 100 ppm SO<sub>2</sub> was introduced to the reaction gas for 4 h. These could be primarily attributed to the large specific surface area, high surface acidity concentration and abundant chemisorbed oxygen species provided by the hierarchical pore structure, which could also increase the mass transfer of the reaction gas. This finding suggests that the NH<sub>3</sub>-SCR activity and SO<sub>2</sub> poisoning tolerance of hierarchical MnO<sub>x</sub>/SAPO-34 catalysts at low temperatures can be improved by controlling the morphology of the catalysts, which might supply a rational strategy for the design and synthesis of Mn-based SCR catalysts.https://www.mdpi.com/2073-4344/11/3/314hierarchical SAPO-34manganese oxideslow-temperature NH<sub>3</sub>-SCRmolecular sievesSO<sub>2</sub> resistance |
| spellingShingle | Lusha Zhou Jinkun Guan Chenglong Yu Bichun Huang MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance Catalysts hierarchical SAPO-34 manganese oxides low-temperature NH<sub>3</sub>-SCR molecular sieves SO<sub>2</sub> resistance |
| title | MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance |
| title_full | MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance |
| title_fullStr | MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance |
| title_full_unstemmed | MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance |
| title_short | MnO<sub>x</sub> Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH<sub>3</sub>: Catalytic Activity and SO<sub>2</sub> Resistance |
| title_sort | mno sub x sub supported on hierarchical sapo 34 for the low temperature selective catalytic reduction of no with nh sub 3 sub catalytic activity and so sub 2 sub resistance |
| topic | hierarchical SAPO-34 manganese oxides low-temperature NH<sub>3</sub>-SCR molecular sieves SO<sub>2</sub> resistance |
| url | https://www.mdpi.com/2073-4344/11/3/314 |
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