Improving Copper Active Site Speciation on Cu-Ce/SSZ-13 for Ammonia Oxidation via Si/Al Ratio Modulation
文献类型：期刊论文
| 作者 | Zhao, Yang; Yi XK(衣晓坤); Dou, Baojuan; Kang RN(康润宁) ; Bin F(宾峰)
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| 刊名 | ACS APPLIED MATERIALS & INTERFACES
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| 出版日期 | 2024-05-08 |
| 卷号 | 16期号:20页码:26088-26098 |
| 关键词 | Catalytic oxidation ammonia Cu-Ce/SSZ-13 Si/Al ratio transient behavior |
| ISSN号 | 1944-8244 |
| DOI | 10.1021/acsami.4c01898 |
| 通讯作者 | Dou, Baojuan(bjdou@tust.edu.cn) ; Bin, Feng(binfeng@imech.ac.cn) |
| 英文摘要 | 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. |
| 分类号 | 二类/Q1 |
| WOS关键词 | SELECTIVE CATALYTIC-REDUCTION ; HYDROTHERMAL STABILITY ; NH3-SCR ; CU-SSZ-13 ; NOX ; COMBUSTION ; ZEOLITES ; IONS ; NH3 ; CUO |
| 资助项目 | 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 |
| WOS研究方向 | Science & Technology - Other Topics ; Materials Science |
| 语种 | 英语 |
| WOS记录号 | WOS:001225187200001 |
| 资助机构 | 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 |
| 其他责任者 | Dou, Baojuan ; Bin, Feng |
| 源URL | [http://dspace.imech.ac.cn/handle/311007/95348]  |
| 专题 | 力学研究所_高温气体动力学国家重点实验室 |
| 推荐引用方式 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. |
| 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. |
入库方式： OAI收割
来源：力学研究所
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