| Improving Copper Active Site Speciation on Cu-Ce/SSZ-13 for Ammonia Oxidation via Si/Al Ratio Modulation | |
Zhao, Yang; Yi XK(衣晓坤); Dou, Baojuan; Kang RN(康润宁) ; Bin F(宾峰)
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| Corresponding Author | Dou, Baojuan([email protected]) ; Bin, Feng([email protected]) |
| Source Publication | ACS APPLIED MATERIALS & INTERFACES
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| 2024-05-08 | |
| Volume | 16Issue:20Pages:26088-26098 |
| ISSN | 1944-8244 |
| Abstract | Catalytic oxidation is a promising purification technique for ammonia (NH3) emission. However, high ignition temperatures and NOx peroxide generation limit its effectiveness due to a lack of active sites. Herein, the effects of Si/Al ratio (SAR) modulation on the speciation of copper active sites and the reaction mechanism at different acidic sites were investigated by loading CuO-CeO2 onto SSZ-13 with different SARs (Cu-Ce/SAR15, 20, and 30). Among them, Cu-Ce/SAR20 exhibits the lowest induction temperature (T-20 = 180 degrees C) and the highest nitrogen selectivity (above 95%), attributing to a higher number of Cu2+ exchange sites. In situ IR spectroscopy and isotopic (O-18(2)) transient response experiments indicate that more active Cu2+ in Cu-Ce/SAR20 provides sufficient Lewis acidic sites for NH3 adsorption and favors the stability of Si-OH-Al structures (Br & oslash;nsted acid sites). NH3 adsorbed at Lewis acidic sites tends to form peroxide byproducts (NOx), while the NH4+ adsorbed at Br & oslash;nsted acidic sites generates the key intermediate NH4NO2, which decomposes to N-2 at high temperatures, thus enhancing nitrogen selectivity. The whole process mainly follows the Mars-van Krevelen (M-K) mechanism, with the Langmuir-Hinshelwood (L-H) mechanism playing a supporting role. Z(2)Cu(2+) coordinates with adjacent Al atoms within the six-membered ring (6MR) and undergoes a slight deformation at high temperatures, facilitating the migration of the lattice oxygen. SAR plays a crucial role in local environmental speciation of reactive Cu2+, where the sufficient isolated Al provided in SAR20 pulls Cu2+ into the eight-membered ring (8MR), allowing it to come into contact with NH3 more readily. |
| Keyword | Catalytic oxidation ammonia Cu-Ce/SSZ-13 Si/Al ratio transient behavior |
| DOI | 10.1021/acsami.4c01898 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:001225187200001 |
| WOS Keyword | SELECTIVE CATALYTIC-REDUCTION ; HYDROTHERMAL STABILITY ; NH3-SCR ; CU-SSZ-13 ; NOX ; COMBUSTION ; ZEOLITES ; IONS ; NH3 ; CUO |
| WOS Research Area | Science & Technology - Other Topics ; Materials Science |
| WOS Subject | Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| Funding Project | National Natural Science Foundation of China[52176142] ; National Natural Science Foundation of China[BX20230380] ; China National Postdoctoral Program for Innovative Talents[2023QN07] ; Youth Fund of the State Key Laboratory of High Temperature Gas Dynamics |
| Funding Organization | National Natural Science Foundation of China ; National Natural Science Foundation of China ; China National Postdoctoral Program for Innovative Talents ; Youth Fund of the State Key Laboratory of High Temperature Gas Dynamics |
| Classification | 二类/Q1 |
| Ranking | 1 |
| Contributor | Dou, Baojuan ; Bin, Feng |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/95349 |
| Collection | 高温气体动力学国家重点实验室 |
| Recommended Citation GB/T 7714 | Zhao, Yang,Yi XK,Dou, Baojuan,et al. Improving Copper Active Site Speciation on Cu-Ce/SSZ-13 for Ammonia Oxidation via Si/Al Ratio Modulation[J]. ACS APPLIED MATERIALS & INTERFACES,2024,16,20,:26088-26098.Rp_Au:Dou, Baojuan, Bin, Feng |
| APA | Zhao, Yang,衣晓坤,Dou, Baojuan,康润宁,&宾峰.(2024).Improving Copper Active Site Speciation on Cu-Ce/SSZ-13 for Ammonia Oxidation via Si/Al Ratio Modulation.ACS APPLIED MATERIALS & INTERFACES,16(20),26088-26098. |
| MLA | Zhao, Yang,et al."Improving Copper Active Site Speciation on Cu-Ce/SSZ-13 for Ammonia Oxidation via Si/Al Ratio Modulation".ACS APPLIED MATERIALS & INTERFACES 16.20(2024):26088-26098. |
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