Spotlight on Cu/SAPO-34 with high hydrothermal stability induced by a small amount of SSZ-39

被引:15
|
作者
Lin, Qingjin [1 ]
Liu, Shuang [2 ]
Xu, Shuhao [3 ]
Yao, Pan [2 ]
Pei, Mingming [3 ]
Xu, Haidi [2 ,4 ,5 ]
Dan, Yi [1 ]
Chen, Yaoqiang [3 ,4 ,5 ]
机构
[1] Sichuan Univ, Polymer Res Inst, State Key Lab Polymer Mat Engn, Chengdu 610064, Peoples R China
[2] Sichuan Univ, Inst New Energy & Low Carbon Technol, Chengdu 610064, Peoples R China
[3] Sichuan Univ, Coll Chem, Key Lab Green Chem & Technol Educ Minist, Chengdu 610064, Peoples R China
[4] Sinocat Environm Technol Co Ltd, Ctr Engn Vehicular Exhaust Gases Abatement, Chengdu 611730, Peoples R China
[5] Ctr Engn Environm Catalyt Mat, Chengdu 610064, Peoples R China
基金
中国国家自然科学基金;
关键词
Zeolite; Hybrid microstructure; Crystallization; Hydrothermal stability; SCR; SELECTIVE CATALYTIC-REDUCTION; CU-SAPO-34; CATALYST; NH3; NH3-SCR; ZEOLITES; NOX; SITES; PERFORMANCE; OXIDATION; FRAMEWORK;
D O I
10.1016/j.cej.2022.137283
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The stable structure is key to improving the performance of the selective catalytic reduction of nitrogen oxide (NOx) with ammonia (NH3-SCR) on Cu/zeolite catalysts after the high-temperature hydrothermal aging. In this work, the SSZ-39 seed with a stable texture property was introduced into the precursor of SAPO-34 to fabricate the zeolite with a hybrid microstructure of SAPO-34 + SSZ-39 (simplified as SA + SZ). The Si distributions of the original Al-rich SAPO-34 zeolite (simplified as SA) were optimized by the hybrid microstructure of SA + SZ. The results of solid nuclear magnetic resonance (NMR) and ammonia (NH3) adsorption indicate more Si(1OAl) structures with strong acidity on Cu/(SA + SZ) catalyst rather than on Cu/SA. The NH3-SCR performance within the reaction region of 150-550 degrees C is enhanced on the former. In addition, the Si(nOAl) (n = 2-4) structures of the original SAPO-34 zeolite are retained on Cu/(SA + SZ), which optimizes the low-temperature catalytic performance of Cu/SSZ-39. Furthermore, the SSZ-39 seed induces Cu/(SA + SZ) to form higher content of stable Si (0OAl) structures than Cu/SA. After hydrothermal aging, more isolated copper species can be formed on SA + SZ hybrid zeolite with advanced structural stability compared with Cu/SA, which better activates NOx on the former. And the loss of acid sites is also weakened on Cu/(SA + SZ) than on Cu/SA. These improvements on Cu/ (SA + SZ) compensates for its hydrothermal deactivation to some degree. Hence, SA + SZ hybrid zeolite can be the new-generation candidate for NH3-SCR catalyst by introducing the second zeolite SSZ-39 in the synthesis process of SAPO-34. And the catalytic performance of Cu/(SA + SZ) is superior to Cu/SA.
引用
收藏
页数:13
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