Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study
The main active sites and the catalytic process in selective catalytic reduction of NO<sub>x</sub> by CH<sub>4</sub> (CH<sub>4</sub>-SCR) on In/BEA catalyst were investigated by density functional theory (DFT) using a periodic model. The [InO]<sup>+</sup&...
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MDPI AG
2020-05-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/10/5/572 |
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| author | Erhao Gao Hua Pan Li Wang Yao Shi Jun Chen |
| author_facet | Erhao Gao Hua Pan Li Wang Yao Shi Jun Chen |
| author_sort | Erhao Gao |
| collection | DOAJ |
| description | The main active sites and the catalytic process in selective catalytic reduction of NO<sub>x</sub> by CH<sub>4</sub> (CH<sub>4</sub>-SCR) on In/BEA catalyst were investigated by density functional theory (DFT) using a periodic model. The [InO]<sup>+</sup> and [InOH]<sup>2+</sup> moieties were constructed in the channel of periodic BEA zeolite representing the Lewis and Brønsted acid sites. The electronic structures [InO]<sup>+</sup> and [InOH]<sup>2+</sup> were analyzed, and it was found that the [InO]<sup>+</sup> group were the main active sites for CH<sub>4</sub> activation and NO/NO<sub>2</sub> adsorption in the CH<sub>4</sub>-SCR process. CH<sub>4</sub> molecules could be activated on the O site of the [InO]<sup>+</sup> group in In/BEA, which was resulted from the strong interactions between the C-p orbital of the CH<sub>4</sub> molecule and the O-p orbital of the [InO]<sup>+</sup> group. CH<sub>4</sub> activation was the initial step in CH<sub>4</sub>-SCR on In/BEA catalyst. NO<sub>2</sub> molecules were essential in the SCR process, and they could be produced by NO reacting with gaseous O<sub>2</sub> or the O atom of the [InO]<sup>+</sup> group. The presence of NO<sub>2</sub> could facilitate the key intermediate nitromethane (CH<sub>3</sub>NO<sub>2</sub>) formation and lower the reaction barrier in the SCR process. |
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| language | English |
| last_indexed | 2024-03-10T19:43:24Z |
| publishDate | 2020-05-01 |
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| spelling | doaj.art-0695907a7c6c48cfad27415e4dced1222023-11-20T01:00:04ZengMDPI AGCatalysts2073-43442020-05-0110557210.3390/catal10050572Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational StudyErhao Gao0Hua Pan1Li Wang2Yao Shi3Jun Chen4College of Biology and Environment Engineering, Zhejiang Shuren University, Hangzhou 310015, ChinaCollege of Biology and Environment Engineering, Zhejiang Shuren University, Hangzhou 310015, ChinaCollege of Biology and Environment Engineering, Zhejiang Shuren University, Hangzhou 310015, ChinaCollege of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, ChinaCollege of Biology and Environment Engineering, Zhejiang Shuren University, Hangzhou 310015, ChinaThe main active sites and the catalytic process in selective catalytic reduction of NO<sub>x</sub> by CH<sub>4</sub> (CH<sub>4</sub>-SCR) on In/BEA catalyst were investigated by density functional theory (DFT) using a periodic model. The [InO]<sup>+</sup> and [InOH]<sup>2+</sup> moieties were constructed in the channel of periodic BEA zeolite representing the Lewis and Brønsted acid sites. The electronic structures [InO]<sup>+</sup> and [InOH]<sup>2+</sup> were analyzed, and it was found that the [InO]<sup>+</sup> group were the main active sites for CH<sub>4</sub> activation and NO/NO<sub>2</sub> adsorption in the CH<sub>4</sub>-SCR process. CH<sub>4</sub> molecules could be activated on the O site of the [InO]<sup>+</sup> group in In/BEA, which was resulted from the strong interactions between the C-p orbital of the CH<sub>4</sub> molecule and the O-p orbital of the [InO]<sup>+</sup> group. CH<sub>4</sub> activation was the initial step in CH<sub>4</sub>-SCR on In/BEA catalyst. NO<sub>2</sub> molecules were essential in the SCR process, and they could be produced by NO reacting with gaseous O<sub>2</sub> or the O atom of the [InO]<sup>+</sup> group. The presence of NO<sub>2</sub> could facilitate the key intermediate nitromethane (CH<sub>3</sub>NO<sub>2</sub>) formation and lower the reaction barrier in the SCR process.https://www.mdpi.com/2073-4344/10/5/572In/BEAactive sitesCH<sub>4</sub> activationSCR |
| spellingShingle | Erhao Gao Hua Pan Li Wang Yao Shi Jun Chen Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study Catalysts In/BEA active sites CH<sub>4</sub> activation SCR |
| title | Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study |
| title_full | Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study |
| title_fullStr | Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study |
| title_full_unstemmed | Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study |
| title_short | Identification of Main Active Sites and the Role of NO<sub>2</sub> on NO<sub>x</sub> Reduction with CH<sub>4</sub> over In/BEA Catalyst: A Computational Study |
| title_sort | identification of main active sites and the role of no sub 2 sub on no sub x sub reduction with ch sub 4 sub over in bea catalyst a computational study |
| topic | In/BEA active sites CH<sub>4</sub> activation SCR |
| url | https://www.mdpi.com/2073-4344/10/5/572 |
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