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| Remarkable N-2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies | |
| Chen, Sining1; Vasiliades, Michalis A.2; Yan, Qinghua3; Yang, Guangpeng4; Du, Xuesen4; Zhang, Cheng1; Li, Yuran5; Zhu, Tingyu5; Wang, Qiang1; Efstathiou, Angelos M.2 | |
| 2020-11-15 | |
| Source Publication | APPLIED CATALYSIS B-ENVIRONMENTAL
 |
| ISSN | 0926-3373 |
| Volume | 277Pages:19 |
| Abstract | A Co0.5Mn1Fe0.25Al0.75Ox-LDO catalyst was developed which showed excellent performance for the low-temperature NH3-SCR. NOx conversions 100% were achieved in the whole 100-250 degrees C range, while after 10-h operation at 150 degrees C with 100 ppm SO2/5 vol% H2O in the feed, the NOx conversion was maintained at 80%. This catalyst provided a much better N-2-selectivity than the Mn1Fe0.25Al0.75Ox-LDO and Mn1Al1Ox-LDO, especially at 150-300 degrees C. It was found that Co0.5Mn1Fe0.25Al0.75Ox possessed higher surface acidity and reducibility, while XPS analyses indicated an electron transfer between Co3+/Co2+ and Mn4+/Mn3+ redox cycles, leading to a much lower N2O formation, supported by Density Functional Theory (DFT) calculations. Detailed analysis of gas responses obtained upon various step-gas switches was performed, which allowed to measure the surface concentration and reactivity of preadsorbed NOx-s and NHx-s leading to N-2 and N2O. Transient kinetic and DFT studies strongly suggested likely mechanisms of NH3-SCR and the critical role of Co for N-2-selectivity enhancement. |
| Keyword | LDHs NH3-SCR MnOx-based catalyst Co-based NH3-SCR Transient kinetics |
| DOI | 10.1016/j.apcatb.2020.119186 |
| Language | 英语 |
| WOS Keyword | SELECTIVE CATALYTIC-REDUCTION ; LOW-TEMPERATURE NH3-SCR ; INITIO MOLECULAR-DYNAMICS ; LAYERED DOUBLE HYDROXIDE ; OXIDE-BASED CATALYSTS ; MIXED-OXIDE ; NITRIC-OXIDE ; SULFUR RESISTANCE ; REACTION PATHWAYS ; N-2 SELECTIVITY |
| Funding Project | Fundamental Research Funds for the Central Universities[2019JQ03015] ; National Natural Science Foundation of China[U1810209] ; Beijing Municipal Education Commission through the Innovative Transdisciplinary Program "Ecological Restoration Engineering" ; Research Committee of the University of Cyprus |
| WOS Research Area | Chemistry ; Engineering |
| WOS Subject | Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical |
| Funding Organization | Fundamental Research Funds for the Central Universities ; National Natural Science Foundation of China ; Beijing Municipal Education Commission through the Innovative Transdisciplinary Program "Ecological Restoration Engineering" ; Research Committee of the University of Cyprus |
| WOS ID | WOS:000552015900023 |
| Publisher | ELSEVIER |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.ipe.ac.cn/handle/122111/41503 |
| Collection | 中国科学院过程工程研究所 |
| Corresponding Author | Wang, Qiang; Efstathiou, Angelos M. |
| Affiliation | 1.Beijing Forestry Univ, Coll Environm Sci & Engn, 35 Qinghua East Rd, Beijing 100083, Peoples R China 2.Univ Cyprus, Heterogeneous Catalysis Lab, Chem Dept, 1 Univ Ave,Univ Campus, CY-2109 Nicosia, Cyprus 3.Qingdao Agr Univ, Coll Resource & Environm, Qingdao 266109, Peoples R China 4.Chongqing Univ, Sch Energy & Power Engn, Minist Educ, Key Lab Low Grade Energy Utilizat Technol & Syst, Chongqing 400044, Peoples R China 5.Chinese Acad Sci, Res Ctr Proc Pollut Control, Natl Engn Lab Hydromet Cleaner Prod Technol, Inst Proc Engn, Beijing 100190, Peoples R China |
| Recommended Citation GB/T 7714 | Chen, Sining,Vasiliades, Michalis A.,Yan, Qinghua,et al. Remarkable N-2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2020,277:19. |
| APA | Chen, Sining.,Vasiliades, Michalis A..,Yan, Qinghua.,Yang, Guangpeng.,Du, Xuesen.,...&Efstathiou, Angelos M..(2020).Remarkable N-2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies.APPLIED CATALYSIS B-ENVIRONMENTAL,277,19. |
| MLA | Chen, Sining,et al."Remarkable N-2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies".APPLIED CATALYSIS B-ENVIRONMENTAL 277(2020):19. |
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