Highlights on Key Roles of Y on the Hydrothermal Stability at 900 °C of Cu/SSZ-39 for NH3-SCR

被引:26
作者
Lin, Qingjin [1 ,2 ]
Xu, Shuhao [3 ]
Zhao, Hongyan [4 ]
Liu, Shuang [4 ]
Xu, Haidi [4 ,5 ]
Dan, Yi [1 ]
Chen, Yaoqiang [3 ,5 ]
机构
[1] Sichuan Univ, Polymer Res Inst, State Key Lab Polymer Mat Engn, Chengdu 610064, Peoples R China
[2] CNPC, PetroChina Southwest Oil & Gasfield Co, Res Inst Nat Gas Technol, Key Lab Nat Gas Qual & Energy Measurement, Chengdu 610213, Sichuan, Peoples R China
[3] Sichuan Univ, Coll Chem, Key Lab Green Chem & Technol, Educ Minist, Chengdu 610064, Peoples R China
[4] Sichuan Univ, Inst New Energy & Low Carbon Technol, Chengdu 610064, Peoples R China
[5] Sichuan Prov Ctr Engn Environm Catalyt Mat, Sichuan Prov Ctr Engn Vehicular Exhaust Gases Abat, Chengdu 610064, Peoples R China
来源
ACS CATALYSIS | 2022年 / 12卷 / 22期
基金
中国国家自然科学基金;
关键词
Cu/SSZ-39; yttrium; hydrothermal stability; 900 degrees C; modification mechanism; SELECTIVE CATALYTIC-REDUCTION; RARE-EARTH IONS; CU-SAPO-34; CATALYST; CU-SSZ-13; ZEOLITE; CATION LOCATION; N2O FORMATION; ALKALI-METAL; PERFORMANCE; SSZ-13; CERIUM;
D O I
10.1021/acscatal.2c03757
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The continuously updated after-treatment system of diesel engines drives the selective catalytic reduction of ammonia (NH 3 -SCR) catalysts to withstand hydrothermal stability at higher temperatures (>800 degrees C). To meet the tightened emission of nitrogen oxides (NOx), yttrium ions (Y3+) were employed to improve the hydrothermal stability of the Cu/SSZ-39 catalyst at 900 degrees C. X-ray diffraction, solid nuclear magnetic resonance, H-2 temperature-programmed reduction, NH3 temperature-programmed desorption, and in situ diffuse reflectance infrared Fourier transform spectra verified the key role of Y3+ on the stability of the structure of SSZ-39 zeolite and the isolated copper species. In detail, the optimized structural stability at 900 "C of the Y-modified Cu/SSZ-39 catalyst is achieved as a result of the spatial and electronic effects of Y3+ at ion-exchanged sites. Furthermore, Y3+ ions in the cages of SSZ-39 zeolite induce more isolated copper species in the double six-member rings of SSZ-39 zeolite. The modified catalyst by 1 wt % Y (Cu/Y 1.0 -SSZ-39) shows the best deNO(x) performance after hydrothermal aging at 900 degrees C for 10 h., including higher than 70% NOx conversion at 200-550 degrees C and the maximum NOx conversion of 94% at 300 degrees C, which is remarkably higher than the maximum NOx conversion of 38% over Cu/SSZ39 after same hydrothermal aging. This work provides a vital research strategy for fabricating the extraordinary hydrothermally stabilized Cu-based zeolite catalysts for NH3-SCR reaction, which would meet the "near-zero" emission after hydrothermal aging at 900 degrees C in the future.
引用
收藏
页码:14026 / 14039
页数:14
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