A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst
Manganese-cerium catalyst has attracted much attention due to its extraordinarily good low-temperature performance for detrinification technology, but its poor SO2 resistance limits its wide application. A suitable catalyst carrier can enhance the low-temperature activity and anti-poisoning performa...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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Elsevier
2022-12-01
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| Series: | Chemical Physics Impact |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2667022422000561 |
| _version_ | 1811326210085486592 |
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| author | Qiulin Wang Chunyu Gu Zhuping Jiang YiCen Lu FengYun Liu Jing Zhi HuanCong Shi |
| author_facet | Qiulin Wang Chunyu Gu Zhuping Jiang YiCen Lu FengYun Liu Jing Zhi HuanCong Shi |
| author_sort | Qiulin Wang |
| collection | DOAJ |
| description | Manganese-cerium catalyst has attracted much attention due to its extraordinarily good low-temperature performance for detrinification technology, but its poor SO2 resistance limits its wide application. A suitable catalyst carrier can enhance the low-temperature activity and anti-poisoning performance of catalyst. In this paper, density functional theory (DFT) was used to construct MnCe catalyst models that supported by conventional TiO2 and TiO2 nanotubes (TiNTs) (denoted as MnCe/TiO2 and MnCe/TiNTs, respectively) to simulate adsorption behaviors of NH3 and SO2 molecules on catalyst surface. The adsorption energies (Eads) of NH3 and SO2 on catalyst surface, projected density of states (PDOS) of surface metal/nonmetal atoms and Mulliken charge were calculated. The results show that NH3 and SO2 molecules prefer to adsorb on top sites of Mn and Ce atoms respectively, but the competitive adsorption between NH3 and SO2 for top site of Ce atom on MnCe/TiO2 surface exists, for their Eads values (-0.42 eV and -0.44 eV) are similar. TiNTs alleviates their competitive adsorption by increasing the adsorption capacity of NH3 and weakening that of SO2 on catalyst surface. It attributes to the fact that TiNTs increases the coordination unsaturation of Mn and Ce atoms that enhances the electron transformation from NH3 molecule to Mn atom and weakens the electron-donating ability of Ce atom to SO2 molecule. In addition, TiNTs own abundant hydroxyl groups (OH) which can act as surface Brønsted acid sites for NH3 adsorption. These facts deeply reveal the promotion mechanism of TiNTs for low-temperature denitrification activity and sulfur poisoning resistance of MnOx-CeO2 catalyst from a microscopic perspective. |
| first_indexed | 2024-04-13T14:46:08Z |
| format | Article |
| id | doaj.art-85f1eef2bb2f464eaa0bc810d088c383 |
| institution | Directory Open Access Journal |
| issn | 2667-0224 |
| language | English |
| last_indexed | 2024-04-13T14:46:08Z |
| publishDate | 2022-12-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Chemical Physics Impact |
| spelling | doaj.art-85f1eef2bb2f464eaa0bc810d088c3832022-12-22T02:42:45ZengElsevierChemical Physics Impact2667-02242022-12-015100118A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalystQiulin Wang0Chunyu Gu1Zhuping Jiang2YiCen Lu3FengYun Liu4Jing Zhi5HuanCong Shi6School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China; Corresponding authors at: School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, ChinaSchool of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, ChinaSchool of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, ChinaSchool of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, ChinaSchool of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, ChinaSchool of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China; Huzhou Institute of Zhejiang University, Huzhou 313000, China; Corresponding authors at: School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.Manganese-cerium catalyst has attracted much attention due to its extraordinarily good low-temperature performance for detrinification technology, but its poor SO2 resistance limits its wide application. A suitable catalyst carrier can enhance the low-temperature activity and anti-poisoning performance of catalyst. In this paper, density functional theory (DFT) was used to construct MnCe catalyst models that supported by conventional TiO2 and TiO2 nanotubes (TiNTs) (denoted as MnCe/TiO2 and MnCe/TiNTs, respectively) to simulate adsorption behaviors of NH3 and SO2 molecules on catalyst surface. The adsorption energies (Eads) of NH3 and SO2 on catalyst surface, projected density of states (PDOS) of surface metal/nonmetal atoms and Mulliken charge were calculated. The results show that NH3 and SO2 molecules prefer to adsorb on top sites of Mn and Ce atoms respectively, but the competitive adsorption between NH3 and SO2 for top site of Ce atom on MnCe/TiO2 surface exists, for their Eads values (-0.42 eV and -0.44 eV) are similar. TiNTs alleviates their competitive adsorption by increasing the adsorption capacity of NH3 and weakening that of SO2 on catalyst surface. It attributes to the fact that TiNTs increases the coordination unsaturation of Mn and Ce atoms that enhances the electron transformation from NH3 molecule to Mn atom and weakens the electron-donating ability of Ce atom to SO2 molecule. In addition, TiNTs own abundant hydroxyl groups (OH) which can act as surface Brønsted acid sites for NH3 adsorption. These facts deeply reveal the promotion mechanism of TiNTs for low-temperature denitrification activity and sulfur poisoning resistance of MnOx-CeO2 catalyst from a microscopic perspective.http://www.sciencedirect.com/science/article/pii/S2667022422000561NH3-SCRTiNTsDFTSO2 resistance |
| spellingShingle | Qiulin Wang Chunyu Gu Zhuping Jiang YiCen Lu FengYun Liu Jing Zhi HuanCong Shi A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst Chemical Physics Impact NH3-SCR TiNTs DFT SO2 resistance |
| title | A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst |
| title_full | A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst |
| title_fullStr | A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst |
| title_full_unstemmed | A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst |
| title_short | A DFT study on adsorption behaviors of NH3 and SO2 on MnCe/TiNTs catalyst |
| title_sort | dft study on adsorption behaviors of nh3 and so2 on mnce tints catalyst |
| topic | NH3-SCR TiNTs DFT SO2 resistance |
| url | http://www.sciencedirect.com/science/article/pii/S2667022422000561 |
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